Patent Description:
wherein the amino acid polymer(s) A1 has(have) a total weight average molecular weight Mw,total of at least <NUM>/mol and at most <NUM>/mol and wherein the binder composition comprises at least <NUM> wt. -% amino acid polymer(s) A1 based on the total weight of the amino acid polymer(s) A1 and component B1.

Further, the present invention relates to the use of a composition kit for the preparation of lignocellulose-based composite articles comprising the binder composition, wherein component A and component B are stored separately, and to lignocellulose-based composite articles comprising a plurality of lignocellulosic pieces and the reacted binder composition. Moreover, the present invention relates to processes of forming lignocellulose-based composite articles comprising the reacted binder composition as well as to the reacted binder composition.

Lignocellulose-based composite articles, such as oriented strand board (OSB), oriented strand lumber, chipboard, also called particleboard, scrimber, agrifiber board, flakeboard, and fiberboard, e.g. medium density fiberboard (MDF), are generally produced by blending or spraying lignocellulosic pieces with a binder composition, e.g. a resin, while the lignocellulosic pieces are tumbled or agitated in a blender or similar apparatus. After blending sufficiently to form a binder composition-lignocellulose mixture, the lignocellulosic pieces, which are now coated with the binder composition, are formed into a product, in particular a loose mat, which is subsequently compressed between heated platens or plates to set the binder composition and to bond these lignocellulosic pieces together in densified form, such as in a board, panel, or other shape. Conventional processes for compressing the loose mat are generally carried out by hot pressing along with heat transfer from hot surfaces (usually between <NUM> and <NUM>) to the mat, in the presence of varying amounts of steam, either purposefully injected into the loose mat or generated by liberation of entrained moisture from the lignocellulosic pieces or the binder composition in the loose mat.

Binder compositions that have been used for making such lignocellulose-based composite articles include phenol formaldehyde (PF) resins, urea formaldehyde (UF) resins, melamine urea formaldehyde (MUF) resins and isocyanates (<NPL>). From an environmental perspective there is the need to provide binder compositions which are formaldehyde-free and isocyanate-free or have at least low formaldehyde-emissions and still have excellent properties.

Carbohydrate-based binder compositions are mainly derived from renewable resources. They require press conditions which are quite different from the traditional phenol-formaldehyde binder composition, urea formaldehyde or isocyanate resins. Carbohydrate polyamine binder compositions can substitute said traditional binder compositions. However, carbohydrate polyamine binder composition solutions are associated with a variety of disadvantages such as large binder composition amounts, long press times and poor structural properties of the resulting boards. <CIT> describes a binder composition for wood boards comprising a reaction product of lysine and a carbohydrate component, but the obtained wood boards have low internal bond strengths even at long press times. <CIT> describes a binder composition comprising a carbohydrate and a polyamine and a matrix polymer. However, such binder compositions for chipboards require long press times and result in chipboards with a low internal bond strength and an insufficient swelling value in water. <CIT> describes a binder composition in the surface layer comprising a nitrogen source and reducing sugars, wherein the weight amount of reducing sugars is equal or higher than the weight amount of the nitrogen source to improve surface properties. However, the internal bond strength and surface properties are insufficient. <CIT>, <CIT>, <CIT>, <CIT>, <CIT>, <CIT> disclose binders comprising amino acid polymers and pentoses, hexoses, or disaccharides.

It is an object of the invention to provide the use of a binder composition, in particular for lignocellulose-based composite articles, with good mechanical properties and swelling values.

It is further an object of the present invention to provide a single-layer or multilayer board comprising reduced amounts of formaldehyde and/or isocyanate or which is formaldehyde-free and/or isocyanate-free, and which provides good mechanical properties to the composite articles as well as reduced or no formaldehyde emission.

This object is achieved by the use of a binder composition, preferably a wood binder composition, comprising.

Component B1 selected from the group consisting of pentoses, hexoses, disaccharides of pentoses and/or hexoses and mixtures thereof may comprise one, two or more different pentoses, one, two or more different hexoses and/or one, two or more different disaccharides thereof.

The binder composition according to the present invention may comprise at least <NUM> wt. -%, more preferably at least <NUM> wt. -%, most preferably at least <NUM> wt. -%, amino acid polymer(s) A1 based on the total weight of the amino acid polymer(s) A1 and component B1 selected from the group consisting of pentoses, hexoses, disaccharides of pentoses and/or hexoses and mixtures thereof. The binder composition may comprise <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% amino acid polymer(s) A1 based on the total weight of the amino acid polymer(s) A1 and the component B1 selected from the group consisting of pentoses, hexoses, disaccharides of pentoses and/or hexoses and mixtures thereof. The pentoses and/or hexoses and/or disaccharides of pentoses and/or hexoses may be glucose, fructose, xylose, sucrose and/or mixtures thereof, preferably glucose and/or fructose.

Preferably, component B1 is a mixture comprising.

Preferably, component B1 is a mixture consisting of.

Binder composition means component A and component B and optionally any further component prior to reacting. The binder composition may be cured by heating, which may be carried out by contact heating and/or heat transfer from hot air and/or steam and/or dielectric heating (e. g microwave heating, or high frequency heating) to obtain the reacted binder composition. The binder composition may be cured by applying heat and optionally pressure at the same time or subsequently to obtain the reacted binder composition. The reacted binder composition means the cured binder composition. The reacted binder composition is obtainable or may be obtained by reacting the binder components A and B.

Reacting or reacted means that amino acid polymer(s) A1 react(s) with the component B1 selected from the group consisting of pentoses, hexoses, disaccharides of pentoses and/or hexoses and mixtures thereof. Besides, further components may also react with amino acid polymer(s) A1 and/or the component B1 selected from the group consisting of pentoses, hexoses, disaccharides of pentoses and/or hexoses and mixtures thereof. The reaction may lead to crosslinked polymers.

Optionally reacting or reacted means that amino acid polymer(s) A1 react(s) with component B1 selected from the group consisting of pentoses, hexoses, disaccharides of pentoses and/or hexoses and mixtures thereof and.

Component B2 is further explained below.

Component A may comprise <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% of the amino acid polymer(s) A1 based on the total weight of component A.

Advantageously, the components A and B are not provided as a mixture, and this allows easy transportation and long storage for several months. Therefore, according to one aspect of the present invention, the binder composition is provided as a kit, wherein Component A and Component B are stored separately.

Components A and B may be brought into contact either directly on the lignocellulosic pieces, preferably made from wood, or by mixing them before the application to the lignocellulosic pieces, preferably made from wood.

Component A and/or B may be provided in the form of an aqueous solution or dispersion.

Amino acid polymer(s) A1 comprise(s) at least one or consists of at least one poly(amino acid) which is a polymerization product of amino acids and optionally other monomers selected from the group consisting of.

and mixtures thereof,
wherein preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, more preferably at least <NUM> wt. -%, most preferably <NUM> wt. -% amino acids, are used as monomers for the polymerization reaction based on the total amount of monomers.

The term amine and/or amino group as used according to the present invention does not include amide-groups such as e.g. R-CO-NH<NUM> and/or R-CO-NH-R.

Amino acid polymer(s) A1 may comprise a polymerization product of one or two or more different amino acids. The term "polymer" is used for such polymerization product, even if the polymerization reaction is not run to completion. Amino acid polymer A1 may consist of dimers (n=<NUM>), trimers (n=<NUM>), oligomers (n = <NUM> - <NUM>) and macromolecules (n > <NUM>) - wherein n is the number of monomers which have been reacted to form the dimers, trimers, oligomers and macromolecules - and may also include monomers. These monomers may be present due to incomplete conversion of the monomers during the polymerization reaction and/or due to an addition of additional monomers after finishing the polymerization reaction, wherein the additional monomers are selected from the group of the monomers, which have been used for the polymerization reaction. Preferably, no monomers are added after finishing the polymerization reaction. Amino acid polymer A1 may also include other monomers than amino acids, like e.g. di- and/or tricarboxylic acids and/or amines comprising at least two amino groups, wherein the amines and/or the di- and tricarboxylic acids are no amino acids.

The amino acid polymer may be a polymerization product of amino acids and optionally other monomers, wherein at least <NUM> wt. -%, preferably <NUM> wt. -%, more preferably <NUM> wt. -%, more preferably <NUM> wt. -%, more preferably <NUM> wt. -%, more preferably <NUM> wt. -%, more preferably <NUM> wt. -%, most preferably <NUM> wt. -% amino acids are used as monomers for the polymerization reaction based on total amount of monomers.

The amino acid polymer(s) A1 may be or comprise polymerization product(s) of.

wherein preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably <NUM> wt. -% amino acids are used as monomers for the polymerization reaction based on the on total weight of amino acid polymer(s) A1.

According to this invention the term amino acid polymer also includes amino acid polymer derivatives, which may be obtained by modification of the amino acid polymer after polymer synthesis.

The modification of the amino acid polymer may be performed by reaction with.

The polymerization of the amino acid polymer(s) A1 may not be proceeded until full conversion. Therefore, monomers, e.g. amines comprising at least <NUM> amino groups and/or amino acids and/or dicarboxylic acids and/or tricarboxylic acids, may be present in the amino acid polymer(s) A1 after synthesis of the amino acid polymer(s) A1 by polymerization.

Each amino acid polymer A1 may contain less than <NUM> wt. -% monomers, more preferably less than <NUM> wt. -% monomers, more preferably less than <NUM> wt. -% monomers based on the total weight of amino acid polymer(s) A1. The weight amount of monomers is calculated based on total weight of each polymer A1 including its monomers. The monomers may be present as a result of incomplete conversion of the monomers in the polymerization or may be added after polymerization. Preferably, no monomers are added after finishing the polymerization reaction.

Amino acid polymer(s) A1 according to the present invention may comprise poly(amino acid)s, e.g. synthetic poly(amino acid)s, natural poly(amino acid)s, polypeptides, proteins or mixtures thereof. Poly(amino acid)s are produced by polymerization of one or different amino acids. Poly(amino acid)s can be obtained by chemical synthesis or by biosynthesis in living organisms. In particular proteins may be obtained by biosynthesis in living organisms. Polypeptides may be obtained by hydrolysis of proteins.

According to this invention the term poly(amino acid)s may also include poly(amino acid) derivatives, which may be obtained by modification of the poly(amino acid) after polymer synthesis.

The modification of poly(amino acid)s may be performed by reaction with.

Amino acid(s) mean organic compounds comprising at least one primary amine (-NH<NUM>) and at least one carboxyl (-COOH) functional groups. The amino acid(s) may be lysine, histidine, isoleucine, leucine, methionine, phenylalanine, threonine, tryptophan, valine, arginine, aspartic acid, glutamic acid, serine, asparagine, glutamine, cysteine, selenocysteine, glycine, alpha-alanine, beta-alanine, tyrosine, gamma-aminobutyric acid, epsilon-aminocaproic acid, ornithine, diaminopimelic acid, <NUM>,<NUM>-diaminopropionic acid, <NUM>,<NUM>-diaminobutyric acid or mixtures thereof. The amino acids can be used in their L- or D- or racemic form. The amino acids may also be used in their cyclic lactam form, e.g. epsilon-caprolactam.

Preferred amino acids which are used for the polymerization reaction are diamino acids comprising two amine groups (-NH<NUM>) and at least one carboxyl (-COOH) functional group. Such diamino acids may be ornithine, diaminopimelic acid, <NUM>,<NUM>-diaminopropionic acid, <NUM>,<NUM>-diaminobutyric acid, and/or lysine, preferably lysine, more preferably L-lysine. Although they are sometimes named as diamino acids, according to this invention asparagine and glutamine are not included in the group of diamino acids, since the second functional group is an amide (CO-NH<NUM>) and not an amine (-NH<NUM>).

Poly(amino acid)s may contain less than <NUM> wt. -% amino acid monomers, more preferably less than <NUM> wt. -% amino acid monomers, more preferably less than <NUM> wt. -% amino acid monomers based on the total weight of poly(amino acid)s. The weight amount of monomers is calculated based on total weight of poly(amino acid)s including its monomers.

Optionally the amino acid polymer(s) A1 contain at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, most preferably <NUM> wt. -% poly(amino acid)s based on the total weight of the amino acid polymer(s) A1.

Optionally the poly(amino acid)(s) of amino acid polymer(s) A1 has (have) a weight-average molecular weight in the range from <NUM>/mol to <NUM>,<NUM>/mol, preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, preferably, <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, more preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol.

Component A may comprise one amino acid polymer A1 having primary and/or secondary amino groups or different amino acid polymers A1 having primary and/or secondary amino groups, wherein amino acid polymer(s) A1 may have a primary and secondary amine nitrogen content (NCps) of at least <NUM> wt.

The term primary and/or secondary amino groups as used according to the present invention does not include amide-groups such as e.g. R-CO-NH<NUM> and/or R-CO-NH-R.

The primary amine nitrogen content (NCp) is the content of nitrogen in wt. -% nitrogen which corresponds to the primary amine groups in amino acid polymer(s) A1. The secondary amine nitrogen content (NCs) is the content of nitrogen in wt. -% nitrogen which corresponds to the secondary amine groups in amino acid polymer(s) A1. The primary and secondary amine group nitrogen content of the amino acid polymer(s) A1 (NCps) is calculated using the following equation: <MAT>.

The primary amino group nitrogen content (NCp) and the secondary amino group nitrogen content (NCs) can be measured based on EN ISO <NUM>:<NUM> (determination of primary, secondary and tertiary amino group nitrogen content).

The wording "amino acid polymer(s) A1 has(have) a primary and secondary amine group nitrogen content (NCps) of at least <NUM> wt. -%" means the following:
If amino acid polymer(s) A1 consist(s) of one polymer having primary and/or secondary amino groups, the amino acid polymer A1 has a NCps of at least <NUM> wt. -%, or if amino acid polymer(s) A1 consist of different polymers having primary and/or secondary amino groups, these amino acid polymers A1 in total have a NCps of at least <NUM> wt.

Optionally amino acid polymer(s) A1 has(have) a NCps of at least <NUM> wt. -%, preferably <NUM> wt. -%, preferably at least <NUM> wt. -%, more preferably at least <NUM> wt. -% and optionally at least one amino acid polymer of amino acid polymers A1, preferably each amino acid polymer A1, has a NCps of at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, more preferably at least <NUM> wt.

Optionally amino acid polymer(s) A1 has(have) a NCps from <NUM> to <NUM> wt. -%, preferably from <NUM> to <NUM> wt. -%, preferably from <NUM> to <NUM> wt. -%, preferably from <NUM> to <NUM> wt. -% and
optionally at least one amino acid polymer of amino acid polymer(s) A1, preferably each amino acid polymer A1, has a NCps from <NUM> to <NUM> wt. -%, preferably from <NUM> to <NUM> wt. -%, preferably from <NUM> to <NUM> wt. -%, preferably from <NUM> to <NUM> wt.

In case component A comprises one amino acid polymer A1, this amino acid polymer A1 has a weight-average molecular weight Mw of at least <NUM>/mol, preferably at least <NUM>,<NUM>/mol, preferably at least <NUM>,<NUM>/mol more, preferably at least <NUM>,<NUM>/mol, more preferably at least <NUM>,<NUM>/mol and at most <NUM>,<NUM>/mol, preferably at most <NUM>,<NUM>/mol.

In case component A comprises different amino acid polymers A1, amino acid polymers A1 have a total weight-average molecular weight Mw,total of at least <NUM>/mol, preferably at least <NUM>,<NUM>/mol, preferably at least <NUM>,<NUM>/mol more, preferably at least <NUM>,<NUM>/mol, more preferably at least <NUM>,<NUM>/mol and amino acid polymers A1 have a total weight average molecular weight Mw,total of at most <NUM>,<NUM>/mol, preferably at most <NUM>,<NUM>/mol.

Weight-average molecular weights are determined by size exclusion chromatography (SEC) as described in the example section ("Measured values and measuring methods"). The weight-average molecular weight Mw refers to the weight-average molecular weight of one single amino acid polymer A1 and is determined by size exclusion chromatography (SEC) for each amino acid polymer A1 separately.

The total weight-average molecular weight Mw,total of the amino acid polymer(s) A1 in total may be calculated via equation (<NUM>) from the individual weight-average molecular weights Mw,j of each polymer A1j(j = <NUM> to k with k being the number of individual amino acid polymers A1 in the totality of polymers A1).

The number portion pj is calculated from the mass portion mj and the weight-average molecular weight Mw,j of each single amino acid polymer via equations (<NUM>) and (<NUM>). <MAT> <MAT>.

If for example amino acid polymers A1 consist of <NUM> wt. -% amino acid polymer A1<NUM> (Mw,<NUM> = <NUM>/mol), <NUM> wt. -% amino acid polymer A1<NUM> (Mw,<NUM> = <NUM>,<NUM>/mol) and <NUM> wt. -% amino acid polymer A1<NUM> (Mw,<NUM> = <NUM>,<NUM>/mol), the total weight-average molecular weight Mw,total is <NUM>,<NUM>/mol. If amino acid polymer A1 consists of one single amino acid polymer A1, e.g. amino acid polymer A1<NUM> (Mw,<NUM> = <NUM>,<NUM>/mol), then Mw,total is identical to the Mw of this single amino acid polymer A1.

Amino acid polymer(s) A1 may contain less than <NUM> wt. -% monomers, more preferably less than <NUM> wt. -% monomers, more preferably less than <NUM> wt. -% monomers based on the total weight of amino acid polymer(s) A1 including its monomers.

Each amino acid polymer A1 may contain less than <NUM> wt. -% monomers, more preferably less than <NUM> wt. -% monomers, more preferably less than <NUM> wt. -% monomers based on the weight of said amino acid polymer A1 including its monomers.

Optionally amino acid polymer(s) A1 have a total weight-average molecular weight Mw,total of at least <NUM>/mol, preferably at least <NUM>,<NUM>/mol, preferably at least <NUM>,<NUM>/mol more, preferably at least <NUM>,<NUM>/mol, more preferably at least <NUM>,<NUM>/mol and amino acid polymers A1 have a total weight average molecular weight Mw,total of at most <NUM>,<NUM>/mol, preferably at most <NUM>,<NUM>/mol,
and
optionally at least one amino acid polymer A1, preferably each amino acid polymer A1, has a weight-average molecular weight Mw of at least <NUM>/mol, preferably at least <NUM>,<NUM>/mol, preferably at least <NUM>,<NUM>/mol more, preferably at least <NUM>,<NUM>/mol, more preferably at least <NUM>,<NUM>/mol and at least one amino acid polymer A1, preferably each amino acid polymer A1, has a weight average molecular weight Mw of at most <NUM>,<NUM>/mol, preferably at most <NUM>,<NUM>/mol. Amino acid polymer(s) A1 may comprise or consist of branched polymer(s).

In case component A comprises one amino acid polymer A1, this amino acid polymer A1 is preferably a branched polymer. In case component A comprises different amino acid polymers A1, preferably at least one of the amino acid polymers A1, more preferably each amino acid polymer A1, is a branched polymer.

Optionally at least one amino acid polymer A1, more preferably each amino acid polymer A1, has a degree of branching (DB) of at least <NUM>, preferably from <NUM> to <NUM>, preferably from <NUM> to <NUM>, and more preferably from <NUM> to <NUM>.

The DB is determined by <NUM>H-NMR-spectroscopy. The DB is obtained by comparison of the intensity of the signals. The degree of branching is calculated according to the following equation: <MAT> wherein D, T and L are the fractions of dendritic, terminal or
linearly incorporated monomers in the resulting branched polymers obtained from integration of the respective signals in NMR-spectra. For further information reference is further made to <NPL>.

Optionally, amino acid polymer(s) A1 has (have) a total weight-average molecular weight Mw,total of at least <NUM>/mol, preferably at least <NUM>,<NUM>/mol, preferably at least <NUM>,<NUM>/mol more, preferably at least <NUM>,<NUM>/mol, more preferably at least <NUM>,<NUM>/mol and amino acid polymer(s) A1 has (have) a total weight-average molecular weight Mw,total of at most <NUM>,<NUM>/mol, preferably at most <NUM>,<NUM>/mol,.

Preferably, amino acid polymer(s) A1 comprise(s) at least one polylysine or consist(s) of one or more polylysine(s), which is (are) a polymerization product of monomer lysine, preferably L-lysine, and optionally other monomers selected from the group consisting of.

and mixtures thereof,
wherein at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably <NUM> wt. -% lysine is used as monomer for the polymerization reaction based on total amount of monomers.

Polylysine consist of dimers (n=<NUM>), trimers (n=<NUM>), oligomers (n = <NUM> - <NUM>) and macromolecules (n > <NUM>) - wherein n is the number of monomers which have been reacted to form the dimers, trimers, oligomers and macromolecules - and monomers. These monomers can be present either due to incomplete conversion of the monomers during the polymerization reaction or due to an addition of additional monomers after finishing the polymerization reaction, wherein the additional monomers are selected from the group of the monomers, which have been used for the polymerization reaction. Preferably, no monomers are added after finishing the polymerization reaction.

Optionally amino acid polymer(s) A1 comprise(s) or consists of one or more polylysine(s), more preferably poly-L-lysine(s). Preferably, the amino acid polymer(s) A1 comprise at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, preferably at least <NUM> wt. -%, most preferably <NUM> wt. -% polylysine(s) based on the total weight of the amino acid polymer(s) A1. For the sake of clarity polylysines means different polylysines, e.g. with different weight-average molecular weight and/or different degree of branching.

Optionally amino acid polymer(s) A1 comprise(s) polylysine(s) or consist(s) of polylysine(s), wherein polylysine(s) has (have) a total weight-average molecular weight Mw,total in the range from <NUM>/mol to <NUM>,<NUM>/mol, preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, preferably, <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, more preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, more preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol.

Preferably, amino acid polymer(s) A1 comprise(s) polylysine(s) or consist(s) of polylysine(s), wherein polylysines(s) has (have) a total weight-average molecular weight Mw,total in the range from <NUM>/mol to <NUM>,<NUM>/mol, preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, preferably, <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, more preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, more preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol and optionally at least one polylysine of amino acid polymer(s) A1 , preferably each polylysine of amino acid polymer(s) A1, has (have) a weight-average molecular weight in the range from <NUM>/mol to <NUM>,<NUM>/mol, preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, more preferably <NUM>,<NUM>/molto <NUM>,<NUM>/mol, more preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol.

Lysine has two possibilities to react during polymerization. Either the α-NH<NUM> or the ε-NHz can react with the carboxylic acid. Therefore, two linear polylysine types exist, i.e. α-polylysine or the ε-polylysine. Polymerisation can also be performed in a manner, that both α-NH<NUM> and the ε-NHz react with the carboxylic acid group to form both α-linkages and ε-linkages. Preferably, the polylysine is a branched polylysine. Preferred polylysine(s) as used according to the present invention have more ε-linkages than α-linkages. Preferably, the ratio of ε-linkages to α-linkages is between <NUM> : <NUM> and <NUM> : <NUM>, preferably between <NUM> : <NUM> and <NUM> : <NUM>, preferably between <NUM> : <NUM> and <NUM> : <NUM>. This ratio can be determined by integration of the corresponding signals in the <NUM>H-NMR spectra of the polylysines.

Polylysine(s) may contain less than <NUM> wt. -% lysine monomers, more preferably less than <NUM> wt. -% lysine monomers, more preferably less than <NUM> wt. -% lysine monomers based on the total weight of Polylysine(s).

Each polylysine may contain less than <NUM> wt. -% lysine monomers, more preferably less than <NUM> wt. -% lysine monomers, more preferably less than <NUM> wt. -% lysine monomers based on the total weight of said polylysine.

The branched polylysine may, for example, have a degree of branching (DB) from <NUM> to <NUM>, preferably from <NUM> to <NUM>, preferably from <NUM> to <NUM>.

In case component A comprises one polylysine, the NCps of the polylysine may be from <NUM> to <NUM> wt. -%, more preferably from <NUM> to <NUM> wt. %, more preferably from <NUM> to <NUM> wt. -%, most preferably from <NUM> to <NUM> wt.

In case component A comprise two or more polylysines, the NCps of polylysines in total may be from <NUM> to <NUM> wt. -%, more preferably from <NUM> to <NUM> wt. %, more preferably from <NUM> to <NUM> wt. -%, most preferably from <NUM> to <NUM> wt. -%, and preferably the NCps of at least one polylysine, preferably of each polylysine, may be from <NUM> to <NUM> wt. -%, more preferably from <NUM> to <NUM> wt. %, more preferably from <NUM> to <NUM> wt. -%, most preferably from <NUM> to <NUM> wt.

Optionally amino acid polymer(s) A1 comprise(s) or consist(s) of polylysine(s), wherein polylysine(s) has (have) a total weight-average molecular weight Mw,total in the range from <NUM>/mol to <NUM>,<NUM>/mol, preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, more preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, more preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol and optionally at least one polylysine, preferably each poylysine, has a weight-average molecular weight in the range from <NUM>/mol to <NUM>,<NUM>/mol, preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, more preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol, more preferably <NUM>,<NUM>/mol to <NUM>,<NUM>/mol and optionally at least one polylysine, preferably each polylysine, has a degree of branching (DB) of between <NUM> and <NUM>, preferably <NUM> and <NUM>, preferably between <NUM> and <NUM> and optionally the polylysine(s) has (have) NCps from <NUM> to <NUM> wt. -%, more preferably <NUM> to <NUM> wt. %, more preferably from <NUM> to <NUM> wt. -% , most preferably from <NUM> to <NUM> wt. -% and optionally at least one polylysine, preferably each polylysine, has a NCps from <NUM> to <NUM> wt. -%, more preferably <NUM> to <NUM> wt. %, more preferably from <NUM> to <NUM> wt. -% , most preferably from <NUM> to <NUM> wt.

The production of polylysine is generally known and may be performed as e.g. described in <CIT>, preferably in claim <NUM>, most preferably in any Examples <NUM> to <NUM>. Another method for producing polylysine from lysine salts is described in <CIT>.

According to this invention the term polylysine(s) also include polylysine derivatives, which may be obtained by modification of the polylysine after polymer synthesis.

The modification of polylysine may be performed by reaction with.

Optionally amines comprising two amino groups, which are suitable for use as monomers in the polymerization to amino acid polymer A1, are selected from the group consisting of <NUM>,<NUM>-ethylenediamine, <NUM>,<NUM>-propylenediamine, <NUM>,<NUM>-proplylenediamine, butylenediamine (for example <NUM>,<NUM>- or <NUM>,<NUM>-butylenediamine), diaminopentane (for example <NUM>,<NUM>- and/or or <NUM>,<NUM> diaminopentane), diaminohexane (for example <NUM>,<NUM>- and/or <NUM>,<NUM>-diaminohexane), diaminoheptane (for example <NUM>,<NUM>- and/or <NUM>,<NUM>-diaminoheptane), diaminooctane (for example <NUM>,<NUM>- and/or <NUM>,<NUM>-diaminooctane), diaminononane (for example <NUM>,<NUM>- and/or <NUM>,<NUM>-diaminononane), diaminodecane (for example <NUM>,<NUM>- and/or <NUM>,<NUM>-diaminodecane), diaminoundecane (for example <NUM>,<NUM>- and/or <NUM>,<NUM>-diaminoundecane), diaminododecane (for example <NUM>,<NUM>- and/or <NUM>,<NUM>-diaminododecane, cyclo-hexylenediamine, bis-(<NUM>-aminopropyl)amine, bis-(<NUM>-aminoethyl)amine, N-(<NUM>-aminoethyl)-<NUM>,<NUM>-propylenediamine, bis-N-(<NUM>-aminoethyl)-<NUM>,<NUM>-propylenediamine, N,N'-bis-(<NUM>-aminopropyl)-<NUM>,<NUM>-ethylenediamine, N,N'-bis-(<NUM>-aminopropyl)-<NUM>,<NUM>-butylenediamine N,N-bis-(<NUM>-aminopropyl)-<NUM>,<NUM>-ethylenediamine, tris-(aminopropyl)amine, tris-(aminoethyl)amine, amine-terminated polyoxyalkylene polyols (so-called jeffamines), amine-terminated polytetramethylene glycols and mixtures thereof.

Preferred amines comprising two amino groups are selected from the group consisting of: <NUM>,<NUM>-ethylenediamine, <NUM>,<NUM>-propylenediamine, bis-(<NUM>-aminopropyl)amine, N-(<NUM>-aminoethyl)-<NUM>,<NUM>-propylenediamine, bis-(<NUM>-aminoethyl)amine, bis-N-(<NUM>-aminoethyl)-<NUM>,<NUM>-propylenediamine, N,N'-bis-(<NUM>-aminopropyl)-<NUM>,<NUM>-ethylenediamine, N,N-bis-(<NUM>-aminopropyl)-<NUM>,<NUM>-ethylenediamine and mixtures thereof. Most preferred are <NUM>,<NUM>-ethylenediamine, <NUM>,<NUM>-propylenediamine, N-(<NUM>-aminoethyl)-<NUM>,<NUM>-propylenediamine, N,N'-Bis-(<NUM>-aminopropyl)-<NUM>,<NUM>-ethylenediamine and mixtures thereof.

Suitable dicarboxylic acids for use as monomers in the polymerization to amino acid polymer A1 are oxalic acid, malonic acid, succinic acid, glutaric acid, adipic acid, pimelic acid, suberic acid, azelaic acid, sebacic acid, undecane-<NUM>,<NUM>-dicarboxylic acid, dodecane- <NUM>,<NUM>-dicarboxylic acid, maleic acid, fumaric acid, malic acid, cis- and trans-cyclohexane-<NUM>,<NUM>-dicarboxylic acid, cis- and trans-cyclohexane-<NUM>-dicarboxylic acid, cis- and trans-cyclohexane-<NUM>,<NUM>-dicarboxylic acid, cis- and trans-cyclopentane-<NUM>,<NUM>-dicarboxylic acid as well as cis- and trans-cyclopentane-<NUM>,<NUM>-dicarboxylic acid or mixtures thereof, preferably malonic acid, succinic acid, glutaric acid and/or adipic acid.

Suitable tricarboxylic acids or tetracarboxylic acids for use as monomers in the polymerization to amino acid polymer A1 are trimesic acid, trimellitic acid, pyromellitic acid, butanetricarboxylic acid, naphthalene tricarboxylic acid and cyclohexane-<NUM>,<NUM>,<NUM>-tricarboxylic acid, citric acid or mixtures thereof, preferably citric acid. Preferred are dicarboxylic acids.

Component A comprises amino acid polymer(s) A1 and optionally comprises component A2 and comprises optionally component A3 which is water. Preferably, Component A comprises amino acid polymer(s) A1 and comprises component A3 which is water and optionally comprises further component A2. Amino acid polymer(s) A1 and component A2 do not comprise water. Component A3 which is water may be used to dissolve or disperse amino acid polymer(s) A1 and/or component A2.

Component A2 may comprise or consist of one or more substances selected from the group consisting of polyols, urea, urea derivatives like ethylene urea, <NUM>,<NUM>-dimethylurea, co-solvents, rheology modifiers, and other auxiliaries like biocides, dyes, pigments, flame retardants, and mixtures thereof.

Polyols may be selected from the group consisting of ethylene glycol, diethylene glycol, propylene glycol, dipropylene glycol, butanediol, glycerine, trimethylolpropane, triethanolamine, pentaerythritol, sorbitol, and mixtures thereof. Other suitable polyols are biopolyols, such as polyols derived from soya oil, rapeseed oil, castor oil, sunflower oil or mixtures thereof. Other suitable polyols are polyether polyols which can be obtained via polymerization of cyclic oxides, for example ethylene oxide, propylene oxide, butylene oxide, or tetrahydrofuran in the presence of polyfunctional initiators or mixtures thereof.

Co-solvents may be selected from alcohols, like ethanol, and/or carbonates, like diethyl carbonate.

Rheology modifiers may be selected from the group of polymeric thickeners, e.g. carboxy-methylcellulose and/or polyvinylalcohol.

<NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% amino acid polymer(s) A1, and optionally <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% component A2, and <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% preferably <NUM> to <NUM> wt. -% component A3 which is water, based on the weight amount of Component A, wherein the weight amount of all amino acid polymer(s) A1, components A2 and A3 is selected such that the total weight of the sum of the polymers (s) A1, components A2 and A3 does not exceed <NUM> wt. -% or is preferably <NUM> wt. -%, wherein preferably <NUM> to <NUM> wt. -% of component A2, preferably <NUM> to <NUM> wt. -% of component A2, preferably <NUM> to <NUM> wt. -% of component A2 is urea and/or urea derivative(s), preferably urea.

Component B comprises component B1 selected from the group consisting of pentoses, hexoses, disaccharides of pentoses and/or hexoses and mixtures thereof, which are preferably selected from the group consisting of glucose, fructose, xylose, sucrose and mixtures thereof, more preferably selected from fructose and/or glucose, and
optionally comprises component B2 and optionally component B3 which is water. Preferably, Component B comprises component B1 and comprises component B3 which is water and optionally comprises component B2. Component B1 and component B2 do not comprise water. Component B3 which is water may be used to dissolve or disperse component B1 and/or component B2.

Component B may comprise <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% of component B1 based on the total weight of component B.

Component B2 may comprise less than <NUM> wt. -%, preferably less than <NUM> wt. -%, preferably less than <NUM> wt. -%, carbohydrates which are different from component B1, based on the total weight of component B1. Component B2 does preferably not comprise any carbohydrate. Carbohydrate means monosaccharides having the formula CnH2nOn (polyhydroxyaldehydes (aldoses) and/or polyhydroxyketones (ketoses)) and/or higher molecular compounds, which can be transformed to these monosaccharides by hydrolysis, like disaccharides having the formula CnH2n-<NUM>On-<NUM>, oligosaccharides and polysaccharides (e.g. starches). Preferably, such carbohydrates are selected from the group consisting of monosaccharides, disaccharides, oligosaccharides, polysaccharides and mixtures thereof, more preferably from the group consisting of monosaccharides, disaccharides and mixtures thereof.

Component B2 may comprise less than <NUM> wt. -%, preferably less than <NUM> wt. -%, preferably less than <NUM> wt. -% glycolaldehyde and/or hydroxyacetone based on the total weight of component B1 or may also comprise no glycolaldehyde and/or hydroxyacetone.

The carbohydrate component may be or comprise a monosaccharide in its aldose or ketose form or a mixture of different types, including a triose, tetrose, or a heptose; or a disaccharide, a polysaccharide; or combinations thereof, excluding
pentoses, hexoses, disaccharides of pentoses and/or hexoses and/or mixtures thereof.

For example, when a triose serves as carbohydrate component, glyceralaldehyd and/or dihydroxyacetone may be utilized. When a tetrose serves as the carbohydrate component aldotetrose sugars, such as erythrose and/or threose may be utilized; and/or ketotetrose sugars, such as erythrulose, may be utilized. When a heptose serves as the carbohydrate component, a ketoheptose sugar such as sedoheptulose may be utilized. Other stereoisomers of such carbohydrate components not known to occur naturally are also contemplated to be useful as component B1 of component B.

As mentioned above, the component B1 may be or comprise a disaccharide of hexoses and/or pentoses. For example, the carbohydrate component may be or comprise sucrose, maltose, lactose and/or cellobiose, preferably sucrose, maltose and/or lactose, more preferably sucrose.

As mentioned above, the carbohydrate component in component B2 may be or comprise a polysaccharide. For example, the carbohydrate component may be or comprise a polysaccharide with a low degree of polymerization, including, for example, molasses, starch hydrolysates, cellulose hydrolysates, or mixtures thereof.

According to a specific example, a starch hydrolysate, e.g. maltodextrin, or a mixture thereof, forms (optionally with other components) components B1 and B2.

Component B comprises component B1 selected from the group consisting of pentoses, hexoses, disaccharides of pentoses and/or hexoses and mixtures thereof, which are preferably selected from the group consisting of glucose, fructose, xylose, sucrose and mixtures thereof, more preferably selected from glucose and/or fructose, and optionally comprises component B2 and optionally component B3 which is water. Preferably, Component B comprises component B1 and comprises component B3 which is water and optionally comprises component B2. Component B1 and component B2 do not comprise water. Component B3 which is water may be used to dissolve or disperse component B1 and/or component B2.

Component B2 may comprise or consist of one or more substances selected from the group consisting of polyols, urea, urea derivatives like ethylene urea, <NUM>,<NUM>-dimethylurea, organic acids, co-solvents, rheology modifiers, and/or other auxiliaries like biocides, dyes, pigments, flame retardants, and mixtures thereof. The organic acids may be e.g. lactic acid and/or formic acid.

Polyols may be selected from the group consisting of ethylene glycol, diethylene glycol, propylene glycol, dipropylene glycol, butanediol, glycerine, trimethylolpropane, triethanolamine, pentaerythritol, sorbitol, and mixtures thereof. Other suitable polyols may be biopolyols, such as polyols derived from soya oil, rapeseed oil, castor oil, sunflower oil or mixtures thereof. Other suitable polyols may be polyether polyols which can be obtained via polymerization of cyclic oxides, for example ethylene oxide, propylene oxide, butylene oxide, or tetrahydrofuran in the presence of polyfunctional initiators or mixtures thereof.

Rheology modifiers may be selected from the group of polymeric thickeners, e.g. carboxymethyl-cellulose.

The binder composition according to the present invention may comprise urea as component A2 and/or B2, wherein preferably the binder composition comprises <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, more preferably <NUM> to <NUM> wt. -%, most preferably <NUM> to <NUM> wt. -% urea in total based on the total weight of the sum of amino acid polymer(s) A1 and component B1.

The binder composition according to the present invention may comprise
<NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% preferably <NUM> to <NUM> wt. -% amino acid polymer(s) A1, based on the total weight of the sum of amino acid polymer(s) A1 and component B1.

Optionally the binder composition according to the present invention comprises <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% preferably <NUM> to <NUM> wt. -% amino acid polymer(s) A1, and <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% component B1, based on the total weight of the sum of amino acid polymer(s) A1 and component B1, wherein the weight amounts of the amino acid polymer(s) A1 and component B1 are selected such that the total weight of the sum of amino acid polymer(s) A1 and component B1 is <NUM> wt.

In the binder composition Component A may comprise.

and component B may comprise
<NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% component B1,.

Optionally <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -% component B2, and.

Optionally the binder composition according to the present invention comprises.

Functional additives are additives for the improvement of certain properties of the lignocellulose-based composite article, e.g. the water resistance and/or the resistance against microorganisms.

The functional additive C1 may be selected from the group of hydrophobizing agents, such as paraffin, rheology modifiers, fillers, fungicides, biocides, flame retardants, pigments, dyes, or mixtures thereof.

One preferred component C is paraffin emulsion, in which paraffin (component C1) is emulsified in water (component C2).

Optionally the binder composition comprises <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, component C1 based on the total weight of the sum of amino acid polymer(s) A1 and component B1 and component C1.

The present invention also relates to a composition kit comprising the above defined binder composition, wherein component A and component B and optionally component C are stored separately. The binder kit comprises two separate components A and B, which are mixed either before or during or after application to a plurality of lignocellulosic particles.

The present invention also relates to a reacted binder composition obtainable or obtained by reacting the components A and B, in particular the binder composition, according to the present invention.

The present invention also relates to a reacted binder composition obtainable or obtained by reacting the binder composition according to the present invention.

The binder composition according to the present invention may be used as binder or adhesive for different materials in different shapes, such as mineral fibers (including slag wool fibers, stone wool fibers, glass fibers), aramid fibers, ceramic fibers, ceramic powder, metal fibers, metal powder, carbon fibers, polyimide fibers, polyester fibers, reyon fibers, cellulosic fibers, cellulosic sheets, cellulosic chips, cellulosic strands, cellulosic layers or lignocellulosic pieces.

Optionally the binder composition according to the present invention is used for lignocellulosic pieces, more preferably lignocellulosic particles, in particular wood particles.

A further aspect of the present invention relates to a lignocellulose-based composite article comprising:.

The reacted binder composition preferably means a binder composition cured at <NUM> to <NUM>° C, preferably <NUM> to <NUM>, preferably <NUM> to <NUM>° C, more preferably <NUM> to <NUM>° C and optionally at a pressure of <NUM> to <NUM> bar, preferably <NUM> to <NUM> bar, preferably <NUM> to <NUM> bar, preferably <NUM> to <NUM> bar.

A high-frequency electrical field may be applied during pressing until <NUM> to <NUM>, preferably <NUM> to <NUM>° C, more preferably <NUM> to <NUM>° C and most preferably <NUM> to <NUM> is reached in the center of the mat, optionally at a pressure of <NUM> to <NUM> bar, preferably <NUM> to <NUM> bar, preferably <NUM> to <NUM> bar, preferably <NUM> to <NUM> bar.

The term "high-frequency electrical field" used herein designates and includes any kind of high-frequency electrical or electromagnetic field such as microwave irradiation or a high-frequency electrical field, which results after applying a high-frequency alternating voltage at a plate capacitor between two capacitor plates. Suitable frequencies for the high-frequency electrical field are in the range of from <NUM> to <NUM>, preferably <NUM> to <NUM>, more preferably <NUM> to <NUM>. Especially suitable and preferred are the respective
nationally and internationally approved frequencies such as <NUM>,<NUM>, <NUM>,<NUM>, <NUM>,<NUM>, <NUM>,<NUM>, <NUM>,<NUM>, <NUM>,<NUM>, more preferably <NUM>,<NUM> und <NUM>,<NUM>. The electrical power used to create such a high-frequency electrical field in the processes of the present invention preferably is in the range of from <NUM> to <NUM> kWh, more preferably of from <NUM> to <NUM> kWh, most preferably of from <NUM> to <NUM> kWh.

Preferably the curing reaction is a crosslinking reaction, preferably crosslinking of the amino acid polymer(s) A1 by reaction with component B1, in particular pentoses, hexoses, and /or disaccharides thereof, wherein the temperature is the maximum temperature reached in the binder composition during the curing step.

Said reacted binder composition may still comprise unreacted amino acid polymer(s) A1, optionally unreacted component A2, optionally unreacted component B1, in particular pentoses, hexoses, and/or disaccharides thereof, optionally unreacted component B2 and/or optionally unreacted components C1.

Optionally said reacted binder composition comprises less than <NUM> wt. -%, preferably less than <NUM> wt. -%, more preferably less than <NUM> wt. -% unreacted amino acid polymer(s) A1, unreacted component B1, unreacted component A2 and unreacted component B2 in total based on the total weight of the sum of amino acid polymer(s) A1, component A2, component B1 and component B2 before reacting the binder composition.

Lignocellulosic pieces as used according to the present invention may be produced by cutting, sawing, crushing and/or grinding lignocellulose-containing materials. Cutting, sawing, crushing and/or grinding of the lignocellulosic materials into lignocellulosic pieces can be carried out by methods known in the art (cf. for example M. Niemz, Holzwerkstoffe and Leime [Wood Materials and Glues], pp. <NUM> to <NUM>, Springer Verlag Heidelberg, <NUM>). Suitable lignocellulosic materials may be ordinarily lignocellulose-containing plants and/or plant parts, in particular wood. Examples of suitable plants include trees, grasses, flax, hemp or mixtures thereof, preferably trees. Preferably lignocellulosic pieces are made from wood. Any desired type of coniferous wood and/or hardwood may be suitable for the production of the wood particles, such as industrial wood residues, forest timber and/or plantation timber, preferably eucalyptus, spruce, beech, pine, larch, linden, poplar, ash, oak, fir or mixtures thereof, more preferably eucalyptus, spruce, pine, beech or mixtures thereof.

However, other plants comprising lignin, agricultural and/or forestry raw materials and/or residues comprising lignin, such as e.g. straw, flax straw, and/or cotton stalks, can also be used for preparation of lignocellulosic pieces. Palms and/or grasses with lignified stems, such as bamboo, are also suitable for preparation of lignocellulosic pieces. A further source of lignocellulose-containing material for the preparation of lignocellulosic pieces may be waste wood, such as old furniture. One or a plurality of lignocellulosic materials can be used for the production of lignocellulosic pieces.

There are no restrictions on the average density of the lignocellulosic materials from which the lignocellulosic pieces are produced, and this density may be <NUM> to <NUM>/cm<NUM>, preferably <NUM> to <NUM>/cm<NUM>, particularly preferably <NUM> to <NUM>/cm<NUM>, in particular <NUM> to <NUM>/cm<NUM>. Here, density refers to the bulk density in a standard atmosphere (<NUM>/<NUM>% humidity) as defined in DIN <NUM>, i.e. taking into consideration the hollow space contained in the lignocellulose-containing starting material, e.g. the tree trunk.

Lignocellulosic pieces may comprise beams, lamellas, planks, veneers, strips, particles (like strands, chips or fibers), and/or dust. Preferably, the lignocellulose-containing pieces are used in the form of fibers, strands, chips, dust or mixtures thereof, preferably chips, fibers, dust or mixtures thereof, particularly preferably chips, fibers or mixtures thereof, most preferably chips. The lignocellulosic pieces used can comprise foreign matter that does not originate from lignocellulose-containing plants. The content of foreign matter can vary over a broad range, and is ordinarily <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, particularly preferably <NUM> to <NUM> wt. -%, in particular <NUM> to <NUM> wt. -%, based on the oven dry weight of the lignocellulosic pieces. Foreign matter can be plastics, adhesives, coatings and/or dyes, etc. contained for example in waste wood.

The oven-dry weight of the lignocellulosic pieces is the weight of the lignocellulosic pieces minus the water present therein and can be determined according to EN <NUM>:<NUM> by placing the pieces in a drying oven at a temperature of (<NUM> ± <NUM>) °C until constant mass has been reached.

The lignocellulosic pieces may be totally or partially delignified before using them for the production of the composite articles. Preferably at least <NUM> wt. -%, more preferably at least <NUM> wt. -%, more preferably at least <NUM> wt. -% of the lignin of the lignocellulosic pieces is removed by the delignification step. Delignification may be performed by treatment with an aqueous solution of H<NUM>O<NUM>and acetic acid as described in <NPL>, or by treatment with an aqueous solution of NaOH and Na<NUM>SO<NUM> as described in <NPL>. Preferably, the lignocellulosic pieces are used without a previous delignification step.

According the present invention the lignocellulose-based composite articles may belong to one of the categories solid wood composite (e.g. glulam), veneer composite (e.g. plywood), chip/strand composites (e.g. chipboard, oriented strand board) or fiber composites (e.g. medium density fiber board) as listed in M. Niemz, Holzwerkstoffe and Leime [Wood Materials and Glues], page <NUM>, Springer Verlag Heidelberg, <NUM>.

Chip/strands composites and fiber composites are collectively referred to as composites made from particles.

According to this invention the term lignocellulosic particles is used as a generic term for fibers, strands and chips.

The lignocellulosic particles can be dried according to common drying methods known to the person skilled in the art, resulting in the common low residual water content (within a common range of variability; so-called "residual moisture content"). Common drying methods are listed in <NPL>. The moisture content of the particles can be measured according to EN <NUM>:<NUM> by placing the particles in a drying oven at a temperature of (<NUM> ± <NUM>) °C until constant mass has been reached. Chips may be dried to a moisture content of <NUM> to <NUM> %, preferably <NUM> to <NUM> %, before adding the binder composition.

According to this invention the lignocellulose-based composite articles made from lignocellulosic particles, preferably from wood particles, may be chipboard (also called particle board), oriented strand board (OSB), medium density fiber board (MDF), high density fiberboard (HDF) and/or wood fiber insulation board (WFI). The production methods for these composites and the use of these composites are known to the person skilled in the art and are described for example in <NPL>. Preferably the lignocellulose-based composite article is chipboard, MDF, HDF or WFI, more preferably chipboard.

Strands may be used for example for the production of oriented strand board (OSB) boards. The average size of the strands is ordinarily <NUM> to <NUM>, preferably <NUM> to <NUM>, particularly preferably <NUM> to <NUM>.

Chips may be used for the production of chipboards. Chips needed for this purpose can be classified according to size by means of sieve analysis as described in <NPL>. Appropriate sieves are defined in DIN ISO <NUM>-<NUM>:<NUM>-<NUM>. The average size of the chips, as defined in <NPL>, may be <NUM> to <NUM>, preferably <NUM> to <NUM>, particularly preferably <NUM> to <NUM>.

Fibers may be wood fibers, hemp fibers, bamboo fibers, miscanthus fibers, bagasse fibers (sugar cane) or mixtures thereof, preferably wood fibers. The length of the fibers may be <NUM> to <NUM>, preferably <NUM> to <NUM>, particularly preferably <NUM> to <NUM>.

Strands may be wood strands, hemp strands, bamboo strands, bagasse strands or mixtures thereof, preferably wood strands. The length of the strands may be <NUM> to <NUM>, preferably <NUM> to <NUM>, particularly preferably <NUM> to <NUM>. The width of the strands may be <NUM> to <NUM>, preferably <NUM> to <NUM>, particularly preferably <NUM> to <NUM>. The thickness of the strands may be <NUM> to <NUM>, preferably <NUM> to <NUM>, particularly preferably <NUM> to <NUM>. Strands may also be called flakes. Wood wool belongs to the group of wood strands.

The total thickness of the lignocellulose-based composite articles made from lignocellulosic particles according to the present invention varies with the field of use. Lignocellulose-based composite articles made from particles are preferably in the range from <NUM> to <NUM>, preferably in the range from <NUM> to <NUM>, especially <NUM> to <NUM>.

The lignocellulose-based composite articles made from lignocellulosic particles according to the present invention may comprise one or several layers. Single-layered or multi-layered composite articles such as for example single-layered or three-layered chipboard are commonly known (<NPL>).

The lignocellulose-based composite article may be a multi-layer, preferably a three-layered chipboard. Optionally the lignocellulose-based composite article consists of a core layer and two surface layers. The lignocellulose-based composite article comprises the reacted binder composition according to the present invention in at least one layer. The lignocellulose-based composite article may comprise the reacted binder composition according to the present invention in more than one layer, wherein binder compositions according to the present invention, which are used in the different layers may be the same or different for the different layers. Preferably, the surface layers comprise the reacted binder composition according to the present invention. The core layer may comprise a reacted binder composition according to the present invention or a reacted binder composition selected from the group consisting of phenol-formaldehyde resins, amino resins, a binder based on organic isocyanate or mixtures thereof, preferably a reacted binder composition according to the present invention.

The multi -layer particle board, preferably a three-layered chipboard, preferably has a formaldehyde emission measured according to EN717-<NUM> lower than <NUM>/m<NUM>h, preferably lower than <NUM>/m<NUM>h.

Suitable phenol-formaldehyde resins (also termed PF resins) are known to the person skilled in the art, see by way of example <NPL>. Skilled in the art, see by way of example <NPL>.

Suitable amino resin can be any of the amino resins known to the person skilled in the art, preferably those for the production of wood-based composites. These resins, and also production thereof, are described by way of example in<NPL> "<NPL>and also in <NPL> (MUF and UF with small quantity of melamine). These are generally polycondensates of compounds having at least one carbamide group or amino group, optionally to some extent substituted with organic moieties (another term for the carbamide group being carboxamide group), preferably carbamide group, preferably urea or melamine, and of an aldehyde, preferably formaldehyde. Preferred polycondensates are urea-formaldehyde resins (UF resins), urea-formaldehyde resins (MF resins) and melamine-containing urea-formaldehyde resins (MUF resins), with particular preference urea-formaldehyde resins, for example Kaurit® glue products from BASF SE.

Suitable organic isocyanates are organic isocyanates having at least two isocyanate groups and mixtures of these, in particular any of the organic isocyanates known to the person skilled in the art and mixtures of these, preferably those for the production of wood-based materials or of polyurethanes. These organic isocyanates, and also the production thereof, are described for example in<NPL>.

Preferred organic isocyanates are oligomeric isocyanates having from <NUM> to <NUM>, preferably from <NUM> to <NUM>, monomer units and on average at least one isocyanate group per monomer unit, and mixtures of these. The isocyanates can be either aliphatic, cycloaliphatic or aromatic. Particular preference is given to the organic isocyanate MDI (methylenediphenyl diisocyanate) and/or the oligomeric organic isocyanate PMDI (polymeric methylenediphenyl diisocyanate), these being obtainable via condensation of formaldehyde with aniline and phosgenation of the isomers and oligomers produced during the condensation (see by way of example <NPL>, final paragraph to p. <NUM>, second paragraph and p. <NUM>, fifth paragraph), and mixtures of MDI and/or PMDI. Very particular preference is given to products in the LUPRANATE® range from BASF SE, in particular LUPRANATE® M <NUM> FB from BASF SE.

The organic isocyanate may be also an isocyanate-terminated prepolymer which is the reaction product of an isocyanate, e.g. PMDI, with one or more polyols and/or polyamines.

The composite articles of the invention made from particles may have a mean overall density of <NUM> to <NUM>/m<NUM>, preferably <NUM> to <NUM>/m<NUM>. The chipboards of the invention may have a mean overall density of <NUM> to <NUM>/m<NUM>, more preferably <NUM> to <NUM>/m<NUM>, especially <NUM> to <NUM>/m<NUM>. The density is determined <NUM> hours after production according to EN <NUM>:<NUM>.

Optionally <NUM> to <NUM> wt. -%, more preferably <NUM> to <NUM> wt. -%, more preferably <NUM> to <NUM> wt. -%, most preferably <NUM> to <NUM> wt. -%, most preferably <NUM> to <NUM> wt. -% amino acid polymer(s) A1 and component B1 in total based on the total oven-dry weight of the lignocellulosic pieces, preferably particles, are used for the preparation of the lignocellulose-based composite article.

Optionally the minimum amount of A1 based on the total oven-dry weight of the lignocellulosic pieces, preferably particles, is <NUM> wt. -%, preferably <NUM> wt. -%, preferably <NUM> wt. %, preferably <NUM> wt.

Preferably the lignocellulosic pieces are fibers or chips, more preferably chips.

Optionally <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, more preferably <NUM> to <NUM> wt. -%, most preferably <NUM> to <NUM> wt. -%, amino acid polymer(s) A1 and component B1 in total based on the total oven-dry weight of the lignocellulosic chips, preferably wood chips, are used for the preparation of composite articles, preferably chip boards.

Optionally <NUM> to <NUM> wt. -%, preferably <NUM> to <NUM> wt. -%, more preferably <NUM> to <NUM> wt. -%, amino acid polymer(s) A1 and component B1 in total based on the total oven-dry weight of the lignocellulosic fibers, preferably wood fibers, are used for the preparation of composite articles, preferably fiber boards like medium density fiber board (MDF), high density fiberboard (HDF) or wood fiber insulation board (WFI), preferably MDF.

A further aspect of the present invention relates to a process for the batchwise or continuous production of lignocellulose-based composite articles, in particular single-layered lignocellulose-based boards or multi-layered lignocellulose-based boards, with a core and with at least one upper and one lower surface layer, comprising the following steps.

The temperature given for step c) refers to the surface temperature of the heated surface used for pressing, in particular the surface temperature of the press-plates.

At the end of the pressing in step c) the temperature in the center of the pressed mat may be at least <NUM>, preferably between <NUM> and <NUM>° C, preferably between <NUM> and <NUM>° C, more preferably <NUM> to <NUM>° C. The boards can be cooled down in a star cooler or more slowly by hot stacking.

The process according to the present invention for the batchwise or continuous production of multi-layered lignocellulose-based boards, with a core and with at least one upper and one lower surface layer, may comprise the following steps.

The process according to the present invention also relates to a method for the batchwise or continuous production of lignocellulose-based composite articles, in particular single-layered lignocellulose-based boards or multi-layered lignocellulose-based boards with a core and with at least one upper and one lower surface layer, comprising the following steps:.

The temperature given for step c') refers to the temperature in the center of the pressed mat at the end of step c'). The boards can be cooled down in a star cooler or more slowly by hot stacking.

In particular, the process according to the present invention relates to a method for the batchwise or continuous production of multi-layered lignocellulose-based boards with a core and with at least one upper and one lower surface layer, comprising the following steps:.

The measurement of the temperature in the center of the pressed mat may be carried out according to known methods, in particular according to <NPL> or <NPL>. For the wireless measurement of the temperature sensors such as the CONTI LOG - or EASYlog-sensors of the Fagus-Grecon Greten GmbH& Co. KG can be used, which can be inserted in the mat during the scattering of the mat.

The time from the start to the end of pressing in step c) or c') is the press time. The press time factor is the press time devided by the target thickness of the board as described in the example section ("Measured values and measuring methods"). Optionally in the process according to the present invention the press time factor is at most <NUM>/mm, preferably at most <NUM>/mm, preferably at most <NUM>/mm, preferably at most <NUM>/mm, preferably at most <NUM>/mm and optionally in the process according to the present invention the press time factor is at least <NUM>/mm, preferably at least <NUM>/mm, preferably at least <NUM>/mm, preferably at least <NUM>/mm.

Components A and B of the binder composition may be added separately or as a mixture as defined below. Optionally component C may be added as a mixture with components A and/or B or separately.

The corresponding methods for producing lignocellulose-based composites, in particular single-layered lignocellulose-based boards or multi-layered lignocellulose-based boards with at least a core and two surface layers, comprising the steps a), b) and c) are generally known to the person skilled in the art, and are described for example in <NPL>or in <NPL>or <NPL>and. The method according to the invention can be carried out discontinuously or continuously, and preferably continuously.

The mixture(s) obtained by step a) comprise(s) water. The water can derive from the residual moisture comprised in the lignocellulosic particles and from the components A and B and optional C. The water content of these mixture(s) may be adapted using lignocellulosic particles with an appropriate moisture and/or by increasing the water content in components A, B and/or C and/or by adding additional water to the mixture (which is not part of the components A, B and/or C) during step a), for instance by spraying.

The water content of the mixtures obtained by a) is determined in an analogous manner to the determination of the water content of wood-based panels by EN <NUM>:<NUM>. For this, a sample of the respective mixture (ca. <NUM>) is weighed in moist condition (m<NUM>) and after drying (m<NUM>). The mass m<NUM> is determined by drying at <NUM> to constant mass. Water content is calculated as follows: water content [in wt. -%] = [(m<NUM>-m<NUM>)/m<NUM>]•<NUM>.

Water content is calculated as follows: <MAT>.

In the mixture obtained in step a), the water content of the mixture(s) may be from <NUM> to <NUM> wt. -%, preferably from <NUM> to <NUM> wt. -%, particularly preferably from <NUM> to <NUM> wt. -%, very particularly preferably from <NUM> to <NUM> wt. -% by weight, based on the total dry weight of the mixture.

If the lignocellulose-based composite is a multi-layered, preferably a three-layered chipboard, the water content in the mixture obtained in step a) for the surface layers is preferably greater than the water content in the mixtures for the core layer obtained in step a).

Optionally the water content [in wt. -%] in the mixture(s) obtained in step a) for the surface layers is greater than the water content [in wt. -%] in the mixture(s) obtained in step a) for the core layer. In particular, the water content [in wt. -%] in the mixture(s) obtained in step a) for the surface layers is greater than the water content [in wt. -%] in the mixture(s) obtained in step a) for the core layer is <NUM> to <NUM> wt. -% by weight, very particularly preferably from <NUM> to <NUM> wt.

Optionally the water content of the mixture obtained in step a) for the core layer is from <NUM> to <NUM> wt. -%, more preferably from <NUM> to <NUM> wt. -%, particularly preferably from <NUM> to <NUM> wt. -%, very particularly preferably from <NUM> to <NUM> wt. -%, based on the total dry weight of the mixture and the water content of the mixture(s) obtained in step a) for the surface layers is from <NUM> to <NUM> wt. -%, preferably from <NUM> to <NUM> wt. -%, particularly preferably from <NUM> to <NUM> wt. -%, very particularly preferably from <NUM> to <NUM> wt. -%, based on the total dry weight of the mixture(s).

After step b) and before step c) or c') the layer(s) may be pre-compressed at a pressure of <NUM> to <NUM> bar, preferably <NUM> to <NUM> bar, more preferably <NUM> to <NUM> bar, more preferably <NUM> to <NUM> bar. The pre-compressing step may take from <NUM> sec to <NUM> sec, preferably from <NUM> to <NUM> sec, more preferably from <NUM> to <NUM> sec. Usually, the pre-compressing step is done without applying heat to the scattered mat. After the pre-compressing step and prior to process step c) or c'), energy can be introduced into the mat in a preheating step with one or more energy sources of any kind. Suitable energy sources are for example hot air, steam or steam/air mixtures. This increases the temperature of the mat and may change the moisture of the mat. After the optional preheating step, the temperature in the core of the mat may be between <NUM> to <NUM>° C, preferably between <NUM> and <NUM>° C. The preheating with steam and steam/air mixtures can also be conducted in such a way that only the surface-near areas are heated, but the core is not.

Optionally the water content in the lignocellulosic composite obtained in step c) or c') is from <NUM> to <NUM> wt. -% by weight, preferably from <NUM> to <NUM> wt. -%, more preferably from <NUM> to <NUM> wt. -% measured according to EN <NUM>:<NUM>.

From the beginning of scattering until the beginning of precompression, there can for example be an interval of <NUM> to <NUM> sec, preferably <NUM> to <NUM> sec, particularly preferably <NUM> to <NUM> sec. From the beginning of scattering until the beginning of heating and/or pressing, there can for example be an interval of <NUM> to <NUM> sec, preferably <NUM> to <NUM> sec, particularly preferably <NUM> to <NUM> sec.

Precompression and preheating can be carried out by a method known to the person skilled in the art, such as those described in M. Niemz, Holzwerkstoffe and Leime [Wood Materials and Glues], Springer Verlag Heidelberg, <NUM>, pg. <NUM> and <NUM> or in H. Ernst, MDF-Medium-Density Fiberboard, DRW-Verlag, <NUM>, pp. <NUM>, <NUM> and <NUM> or in A. Wagenfuhr, F. Scholz, Taschenbuch der Holztechnik [Handbook of Wood Technology], Fachbuchverlag Leipzig, <NUM>, pg.

In step c) or c'), the thickness of the mat is (further) reduced. In addition, the temperature of the mat is increased by inputting energy. In the simplest case, a constant pressing force is applied, and the mat is simultaneously heated by means of a constant-power energy source. However, both the inputting of energy and compression by means of a pressing force can take place at respectively different times and in a plurality of stages. The inputting of energy in process step c) can be carried out by heat transfer from heated surfaces, for example press plates, to the mat or by other energy sources for example hot air, steam or steam/air mixtures. The inputting of energy in method step c') can be carried out by high-frequency heating (by applying a high-frequency electrical field) or by a combination of high-frequency heating and heat transfer from heated surfaces.

This pressing can be carried out by any methods known to the person skilled in the art (cf. examples in <NPL>, and "<NPL>). Optionally continuous pressing methods, for example using double band presses, are used.

When step c') involves a combination of high-frequency heating and heat transfer from heated surfaces the heated press plates, preferably have temperatures from in the range of from <NUM> to <NUM>, more preferably from <NUM> to <NUM>, most preferably from <NUM> to <NUM>.

Preferred is a process of the present invention, wherein in said step c') of applying a high-frequency electrical field the temperature at the center of the pressed mat is increased to a maximum temperature in the range of from <NUM> to <NUM>, preferably in the range of from <NUM> to <NUM>, wherein preferably the maximum temperature is reached in less than <NUM>. (d/mm) after the start of applying a high-frequency electrical field, where d is the thickness of the compacted mixture in mm at the end of step c'), more preferably in less than <NUM>. (d/mm), even more preferably in less than <NUM>. (d/mm), most preferably in less than <NUM> ·(d/mm) after the start of applying a high-frequency electrical field, where d is the thickness of the pressed mat in mm at the end of step c'). , if the thickness d of the compacted mixture in mm at the end of step c') is <NUM>, the maximum temperature is preferably reached in less than <NUM>, more preferably in less than <NUM>, even more preferably in less than <NUM>, most preferably in less than <NUM> after the start of applying a high-frequency electrical field.

The term "center of the pressed mat" as used in this text designates the location which is approximately in the middle between the surfaces of the three-dimensional object defined by the pressed mat in step c) or c').

Component A and component B can be added to the lignocellulosic pieces, in particular particles, in step a) either.

An addition of components A and B separately from one another is understood here to mean that component A and component B are added to the lignocellulosic particles in step a) with the aid of separate application devices, for example nozzles or applicator disks. The application devices may be arranged spatially in such a way or in such a time sequence that the addition of component A and component B is effected successively, in any sequence, or simultaneously. Optionally the application devices are arranged such that component A and component B are added simultaneously but not as a mixture to the lignocellulosic particles. In general, this is achieved by virtue of the application devices being in immediate spatial proximity, e.g. the distance between the application devices may be between <NUM> and <NUM>, preferably between <NUM> and <NUM>, more preferably between <NUM> and <NUM>. Optionally the application devices may also be aligned here such that the components mix partly or completely even when they are on the way from the application devices to the lignocellulosic particles.

If the optional component C is used in step a), addition of component A and component B as a mixture means that.

If the optional component C is used in step a), addition of component A and component B separate from one another means that.

When components A, optionally premixed with component C, and component B, optionally premixed with component C are added as a mixture, the resulting mixture is added to the lignocellulosic particles after a waiting time of less than <NUM>, preferably <NUM> or less than <NUM>, preferably <NUM> or less than <NUM>, preferably <NUM> or less than <NUM>, preferably <NUM> or less than <NUM>, more preferably <NUM> or less than <NUM>, <NUM> or most preferably less than <NUM>, <NUM> or less than <NUM>. Waiting time is the time period between the mixing and the addition to the lignocellulosic particle and may be at least <NUM> sec. During the waiting time the mixture of might be exposed to a temperature of <NUM> to <NUM>, preferably <NUM> to <NUM>, preferably <NUM> to <NUM>.

A further aspect of the present invention relates to the use of the lignocellulosic articles made from particles.

In a further preferred use, the lignocellulose-based composite articles are coated on one or more sides, for example, with melamine films, with veneers, with a plastic edge or with paint.

Optionally the lignocellulose-based composite articles, for example the chipboard or the fiberboard are used as inner plies for sandwich materials. In this case, the outer plies of the sandwich materials may consist of different materials, for example of metal such as aluminum or stainless steel, or of thin wood-based chipboards or fiberboards, preferably high-density fiberboards (HDF), or of laminates, for example high-pressure laminate (HPL).

Examples of uses of the lignocellulose-based composite article or of the coated lignocellulose-based composites produced therefrom or of the sandwich materials produced therefrom are as material for furniture, for example as material for cabinet side, as shelf in cabinets, as material for bookshelves, as furniture door material, as countertop, as kitchen unit front, as elements in tables, chairs and/or upholstered furniture. Examples of uses of the lignocellulose-based composite article or of the coated lignocellulose-based composites produced therefrom or of the sandwich materials produced therefrom are as building and/or construction material, for example as material for interior fit-out, shopfitting and exhibition stand construction, as material for roof and/or wall paneling, as infill, cladding, floors and/or inner layers of doors, and/or as separating walls.

If the lignocellulose-based composite article is made from beams, lamellas, blanks and/or veneers the weight of binder composition in wt. -% based on the total composite strongly depends on the size of the lignocellulosic beams, lamellas, blanks and/or veneers. Therefore, in such kind of composites the weight of binder composition is usually calculated in mass of binder composition per surface area of the piece to be glued.

Suitable amounts are <NUM> to <NUM>/m<NUM> amino acid polymer(s) A1 and component B1 in total. In the context of these composites the terms glue or adhesive are often used in the prior art instead of binder composition. In the description of the present invention the term binder composition is used for all kind of lignocellulose-based composites articles.

Lignocellulose-based composite articles made from beams, lamellas, blanks and/or veneers may be glulam, plywood, cross laminated timber, solid wood board and/or blockboard.

Alternatively, the composite article made from veneers is a chipboard or fiberboard covered by one or more veneers at least on one side of the board.

A further aspect of the present invention relates to a process for the batchwise or continuous production lignocellulose-based composites, which may be glulam, plywood, cross laminated timber, blockboards or solid wood boards, preferably plywood, comprising the following steps,.

wherein the lignocellulosic pieces are beams, lamellas, blanks and/or veneers.

Pressing in step c) may be at a temperature of <NUM> to <NUM>° C, preferably <NUM> to <NUM>° C, more preferably <NUM> to <NUM>° C and at a pressure of <NUM> to <NUM> bar, preferably <NUM> to <NUM> bar, more preferably <NUM> to <NUM> bar, wherein the temperature is the maximum temperature reached in the binder composition during step c).

The corresponding methods for producing composites made from beams, lamellas, blanks and/or veneers comprising the steps a), b) and c) are generally known to the person skilled in the art, and are described for example in <NPL>.

A further aspect of the present invention relates to a process for the batchwise or continuous production of plywood, comprising the following steps.

Plywood is composed at least of three plies of wood veneers glued on top of each other, wherein the directions of fiber of adjacent plies are arranged in angle of about <NUM>. In the case of three-ply plywood, the back veneer run through a glue spreader, which applies the glue to the upper surface of the back veneer. The core veneer or several veneer stripes placed one beside the other are laid on top of the glued back veneer, and the whole sheet is run through the glue spreader a second time. Thereafter, the face veneer is laid on the top glued core. This glued sheet or several of these glued sheets stacked on top of each other are loaded into a press, for example a multi-opening hot press. The sheets may be pressed at <NUM> to <NUM> and at a pressure of <NUM> to <NUM> bar. Multi-ply plywood, e.g. five-ply of seven-ply plywood, are produced in a similar manner, just with more than one core veneer layers.

The production of blockboards is similar to the process of a three-ply plywood. Instead of the core veneers a sheet is used which is made from several wood blanks glued together.

A further aspect of the present invention relates to the use of the lignocellulosic articles made from beams, lamellas, blanks and/or veneers:
Examples of uses are as material for furniture, for example as construction material for cabinets, as shelves, as furniture door material, as countertop, as kitchen unit front, and/or as elements in tables,.

Examples of uses are as building and construction material, for example as material for interior fitout, shopfitting and/or exhibition stand construction, as material for roof and/or wall paneling, as infill, cladding, floors and/or inner layers of doors, and/or as separating walls, as material for car ports and/or for hall roofs.

The chips were produced in a disc chipper. Spruce trunk sections (length <NUM>) from Germany were pressed with the long side against a rotating steel disc, into which radially and evenly distributed knife boxes are inserted, each of which consists of a radially arranged cutting knife and several scoring knives positioned at right angles to it. The cutting knife separates the chip from the round wood and the scoring knives simultaneously limit the chip length. Afterwards the produced chips are collected in a bunker and from there they are transported to a cross beater mill (with sieve insert) for re-shredding with regard to chip width. Afterwards the reshredded chips were conveyed to a flash drier and dried at approx. The chips were then screened into two useful fractions (B: ≤ <NUM> x <NUM> and > <NUM> x <NUM>; C: ≤ <NUM> x <NUM>,<NUM> and > <NUM> x <NUM>), a coarse fraction (D: > <NUM> x <NUM>), which is reshredded, and a fine fraction (A: ≤ <NUM> x <NUM>).

Fraction B is used as surface layer chips for three-layered chipboards ("surface layer chips") A mixture of <NUM> wt. -% of fraction B and <NUM> wt. -% of fraction C is used either as core layer chips for three-layered chipboards and as chips for single-layered chipboards ("core layer chips").

The moisture content of the particles (chips or fibers) before application of the binder (was measured according to EN <NUM>:<NUM> by placing the particles in a drying oven at a temperature of (<NUM> ± <NUM>) °C until constant mass has been reached.

The water content of the particle/binder composition mixtures obtained in step a) is determined in an analogous manner. For this, a sample of the respective mixture (ca. <NUM>) is weighed in moist condition (m<NUM>) and after drying (m<NUM>). The mass m<NUM> is determined by drying at <NUM> to constant mass. Water content is calculated as follows: water content [in wt. -%] = [(m<NUM>- m<NUM>)/m<NUM>] • <NUM>.

The press time factor is the press time, which is the time from closing to opening of the press, devided by the target thickness of the board. The target thickness refers to the board at the end of pressing step c) or c') and is adjusted by the press conditions, i.e. by the distance between the top and bottom press plate, which is adjusted by inserting two steel spacing strips in the press (if the hot press was used) or by the automatic distance control (if the HF press was used).

Press time factor [sec/mm] = time from closing to opening of the press [sec] : target thickness of the pressed board [mm]. For example, when a <NUM> chipboard is made with a press time of <NUM> sec, a press time factor of <NUM> sec/mm results.

The density of the boards was measured according to EN <NUM> :<NUM> and is reported as the arithmetic average of ten <NUM> x <NUM> samples of the same board.

Transverse tensile strength of the boards ("internal bond") was determined according to
EN <NUM>:<NUM> and is reported as the arithmetic average of ten <NUM> x <NUM> samples of the same board.

Swelling in thickness after <NUM> of the boards ("<NUM> swelling") was determined according to EN <NUM>:<NUM> and is reported as the arithmetic average often <NUM> x <NUM> samples of the same board.

The binder amounts in the examples according to the present invention are reported as the total weight of the sum of the respective binder components amino acid polymer(s) A1 and component B1 in wt. -% based on the total dry weight of the wood particles (chips or fibers).

The binder amounts in the comparative examples are reported as the total weight of the sum of all binder components in wt. -% (dry weight, which is the weight of the components without any water) based on the total dry weight of the wood particles (chips or fibers).

Formaldehyde emission was determined according to EN <NUM>-<NUM> and is given in [mg(HCHO)/m<NUM>h].

The ratio of amino acid polymer(s) A1 and component B1 refers to the weight ratio of amino acid polymer(s) A1 and component B1.

The NCps are measured by potentiometric titration according to EN ISO <NUM>:<NUM>. The NCps mean the weight of nitrogen of the primary and secondary amine groups per <NUM> of amino acid polymer(s) A1 (given in wt.

Mw was determined by size exclusion chromatography under the following conditions:.

The residual lysine monomer content of the polylysine solution was determined by HPLC/MS analysis under the following conditions:.

• Injection volume: <NUM>µl
• Eluent A: water + <NUM>% formic acid
• Eluent B: water
• Gradient.

• Switching from Eluent A to Eluent B after <NUM>
• Flow: <NUM>/min
• Column HPLC: Primesep C, <NUM> x <NUM>, <NUM>
• Column temperature: <NUM>
• Calibration with solution of L-lysine in water
• Mass spectrometer: Bruker Maxis (q-TOF)
• MS conditions:.

The residual lysine monomer content in amino acid polymer A1 is given as wt. -% monomer based on the total weight of polylysine including the lysine monomer. For instance, the <NUM> wt. -% solution of Polylysine-<NUM> with a lysine monomer content of <NUM> wt. -% contains <NUM> wt. % lysine monomer and <NUM>% wt. -% lysine polymer comprising at least <NUM> condensed lysine units.

A fiber-optic sensor was used in combination with a temperature measuring instrument suitable for measurements in an environment with strong electromagnetic radiation. The instrument is integrated into the control system of the HF press (HLOP <NUM> press from Hoefer Presstechnik GmbH). The sensor of the device is a Teflon-coated glass fiber with a gallium arsenide chip (GaAs chip).

<NUM> of L-lysine solution (<NUM>% in water, ADM) was heated under stirring in an oil bath (external temperature <NUM>). Water was distilled off and the oil bath temperature was increased by <NUM> per hour until a temperature of <NUM> was reached. The reaction mixture was stirred for an additional hour at <NUM> (oil bath temperature) and then pressure was slowly reduced to <NUM> mbar. After reaching the target pressure, distillation was continued for another <NUM>. The product (Polylysine-<NUM>, Mw <NUM>/mol) was hotly poured out of the reaction vessel, crushed after cooling and dissolved in water to give a <NUM> wt. -% solution.

<NUM> of glucose monohydrate and <NUM> of fructose are mixed with <NUM> of water and stirred to a solution.

In a mixer, a mixture of <NUM> of Kaurit glue <NUM> (urea formaldehyde resin, <NUM> % solid content) and <NUM> of ammonium sulfate was sprayed onto <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM>%) while mixing. Subsequently, <NUM> of water was sprayed onto the mixture to adjust the final moisture of the resinated chips while mixing. Thereafter, mixing was continued for <NUM>.

<NUM> of HMDA, <NUM> of glucose monohydrate and <NUM> of fructose were mixed with in <NUM> of water und stirred until all components were fully dissolved. After <NUM> this solution was sprayed in a mixer onto <NUM> (<NUM> dry weight) of spruce surface layer chips (moisture content <NUM>%) while mixing. Thereafter, mixing was continued for <NUM>.

In a mixer, <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water) was sprayed onto <NUM> (<NUM> dry weight) of spruce surface layer chips (moisture content <NUM>%) while mixing. Subsequently, <NUM> of carbohydrate solution CS was sprayed onto the mixture while mixing. Thereafter, mixing was continued for <NUM>.

In a mixer, <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water) was sprayed onto <NUM> (<NUM> dry weight) of spruce surface layer chips (moisture content <NUM>%) while mixing. Subsequently, <NUM> carbohydrate solution CS was sprayed onto the mixture while mixing. Thereafter, mixing was continued for <NUM>.

In a mixer, a mixture of <NUM> of Kaurit glue <NUM> (<NUM> % solid content) and <NUM> of ammonium sulfate, was sprayed onto <NUM> (<NUM> dry weight) of spruce surface layer chips (moisture content <NUM>%) while mixing. Subsequently, <NUM> of water was sprayed onto the mixture to adjust the final moisture of the resinated chips while mixing. Thereafter, mixing was continued for <NUM>.

In a mixer, <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water) was sprayed onto <NUM> (<NUM> dry weight) of spruce surface layer chips (moisture content <NUM>%) while mixing. Subsequently, <NUM> of a xylose solution (<NUM> wt. -% in water) was sprayed onto the mixture while mixing. Thereafter, mixing was continued for <NUM>.

Immediately after resination, <NUM> of resinated surface layer chips, followed by <NUM> of resinated core layer chips, followed by <NUM> of resinated surface layer chips, were scattered into a <NUM>,<NUM> x <NUM> mold and pre-pressed under ambient conditions (<NUM> N/cm<NUM>). Subsequently, the pre-pressed chip mat thus obtained was removed from the mold, transferred into a hot press and pressed to a thickness of <NUM> to give a chipboard (temperature of the press plates <NUM>° C, max pressure <NUM> N/mm<NUM>, presstime <NUM>, <NUM> or <NUM>,board thickness was adjusted by two steel spacing strips which were inserted in the press).

Surprisingly, boards according to the present invention having an excess of polylysine in the surface layer provide an excellent internal bond strength as well a very low formaldehyde emission.

<NUM> single-layer chipboards by pressing in a high-frequency press.

In a mixer, <NUM> of water was sprayed within <NUM> to <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM> %) while mixing. Subsequently, a mixture of <NUM> of Kaurit glue <NUM> (<NUM> % solid content), <NUM> of ammonium sulfate and <NUM> of water was sprayed to this mixture within <NUM> while mixing. After completion of the spraying, mixing in the mixer was continued for <NUM> sec.

In a mixer, a mixture of <NUM> of Kaurit glue <NUM> (<NUM> % solid content), <NUM> of ammonium sulfate and <NUM> of water sprayed within <NUM> to <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM> %) while mixing. After completion of the spraying, mixing in the mixer was continued for <NUM> sec.

In a mixer, <NUM> of water was sprayed within <NUM> to <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM> %) while mixing. Subsequently, a mixture of <NUM> of L-lysine, <NUM> of glucose monohydrate, and <NUM> of water was sprayed to this mixture within <NUM> while mixing. After completion of the spraying, mixing in the mixer was continued for <NUM> sec.

In a mixer, a mixture of <NUM> of L-lysine, <NUM> of glucose monohydrate and <NUM> of water sprayed within <NUM> to <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM> %) while mixing. After completion of the spraying, mixing in the mixer was continued for <NUM> sec.

In a mixer, <NUM> of water was sprayed within <NUM> to <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM> %) while mixing. Subsequently, a mixture of <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water), <NUM> of glucose monohydrate, and <NUM> of water was sprayed to this mixture within <NUM> while mixing. After completion of the spraying, mixing in the mixer was continued for <NUM> sec.

In a mixer, a mixture of <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water), <NUM> of glucose monohydrate and <NUM> of water sprayed within <NUM> to <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM> %) while mixing. After completion of the spraying, mixing in the mixer was continued for <NUM> sec.

In a mixer, <NUM> of water was sprayed within <NUM> to <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM> %) while mixing. Subsequently, a mixture of <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water), <NUM> of fructose, and <NUM> of water was sprayed to this mixture within <NUM> while mixing. After completion of the spraying, mixing in the mixer was continued for <NUM> sec.

In a mixer, a mixture of <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water), <NUM> of fructose and <NUM> of water sprayed within <NUM> to <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM> %) while mixing. After completion of the spraying, mixing in the mixer was continued for <NUM> sec.

In a mixer, a mixture of <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water), <NUM> of glucose monohydrate, <NUM> of fructose and <NUM>,<NUM> of water sprayed within <NUM> to <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM> %) while mixing. After completion of the spraying, mixing in the mixer was continued for <NUM> sec.

In a mixer, a mixture of <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water), <NUM> of glucose monohydrate, <NUM> of fructose and <NUM> of water sprayed within <NUM> to <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM> %) while mixing. After completion of the spraying, mixing in the mixer was continued for <NUM> sec.

Immediately after resination, <NUM> of the resinated were scattered into a 30x30 cm mold and pre-pressed under ambient conditions (<NUM> N/mm<NUM>). Subsequently, the pre-pressed chip mat thus obtained was removed from the mold. For monitoring a temperature sensor (GaAs chip) was introduced into the center of said pre-pressed chip mat. Nonwoven separators were then provided to the upper and lower side of the pre-pressed chip mat. The pre-pressed chip mat was inserted in a HLOP <NUM> press from Hoefer Presstechnik GmbH, whereby a birch plywood (thickness <NUM>) was placed between the nonwoven separator and the press plate on each side of the mat. The pre-pressed chip mat was then compacted to <NUM> thickness in the press within a period of <NUM>, and then heated by applying a high-frequency electrical field (<NUM>, anode current <NUM> A) while the press was remaining closed. When the target temperature <NUM> or <NUM> ("HF temperature") was reached in the center of the pressed mat, the press was opened.

Three-layered <NUM> chipboards by pressing in a high-frequency press.

In a mixer, a mixture of <NUM> of Polylysine-<NUM> (<NUM> wt. -% in water), <NUM> of fructose, <NUM> of glucose monohydrate and <NUM> of water was sprayed onto <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM>%) while mixing. Thereafter, mixing was continued for <NUM>.

Immediately after resination, <NUM> of resinated surface layer chips, followed by <NUM> of resinated core layer chips, followed by <NUM> of resinated surface layer chips, were scattered into a <NUM>,<NUM> x <NUM> mold and pre-pressed under ambient conditions (<NUM> N/cm<NUM>). Subsequently, the pre-pressed chip mat thus obtained was removed from the mold. For monitoring a temperature sensor (GaAs chip) was introduced into the center of said pre-pressed chip mat. Nonwoven separators were then provided to the upper and lower side of the pre-pressed chip mat. The pre-pressed chip mat was inserted in a HLOP <NUM> press from Hoefer Presstechnik GmbH, whereby a birch plywood (thickness <NUM>) was placed between the nonwoven separator and the press plate on each side of the mat. The pre-pressed chip mat was then compacted to <NUM> thickness in the press within a period of <NUM>, and then heated by applying a high-frequency electrical field (<NUM>, anode current <NUM> A) while the press was remaining closed. When the target temperature <NUM> or <NUM> ("HF temperature") was reached in the center of the pressed mat, the press was opened.

Three-layered <NUM> chipboards with additional urea.

In a mixer, a mixture of <NUM> of Kaurit glue <NUM> (<NUM> % solid content) and <NUM> of ammonium sulfate was sprayed onto <NUM> (<NUM> dry weight) of spruce core layer chips (moisture content <NUM>%) while mixing. Subsequently, <NUM> of water was sprayed onto the mixture to adjust the final moisture of the resinated chips while mixing. Thereafter, mixing was continued for <NUM>.

In a mixer, a mixture of <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water), <NUM> of fructose and <NUM> of water was sprayed onto <NUM> (<NUM> dry weight) of spruce surface layer chips (moisture content <NUM>%) while mixing. Thereafter, mixing was continued for <NUM>.

In a mixer, a mixture of <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water),<NUM> of urea, <NUM> of fructose and <NUM> of water was sprayed onto <NUM> (<NUM> dry weight) of spruce surface layer chips (moisture content <NUM>%) while mixing. Thereafter, mixing was continued for <NUM>.

In a mixer, a mixture of <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water), <NUM> of urea, <NUM> of fructose and <NUM> of water was sprayed onto <NUM> (<NUM> dry weight) of spruce surface layer chips (moisture content <NUM>%) while mixing. Thereafter, mixing was continued for <NUM>.

In a mixer, a mixture of <NUM> of Polylysine-<NUM> solution (<NUM> wt. -% in water),<NUM> of urea, <NUM> of a fructose and <NUM> of water was sprayed onto <NUM> (<NUM> dry weight) of spruce surface layer chips (moisture content <NUM>%) while mixing. Thereafter, mixing was continued for <NUM>.

In a mixer, a mixture of <NUM> of Kaurit glue <NUM> (<NUM> % solid content),<NUM> of ammonium sulfate and <NUM> of water was sprayed onto <NUM> (<NUM> dry weight) of spruce surface layer chips (moisture content <NUM>%) while mixing. Thereafter, mixing was continued for <NUM>.

Immediately after resination, <NUM> of resinated surface layer chips, followed by <NUM> of resinated core layer chips, followed by <NUM> of resinated surface layer chips, were scattered into a <NUM>,<NUM> x <NUM> mold and pre-pressed under ambient conditions (<NUM> N/cm<NUM>). Subsequently, the pre-pressed chip mat thus obtained was removed from the mold, transferred into a hot press and pressed to a thickness of <NUM> to give a chipboard (temperature of the press plates <NUM>° C, max pressure <NUM> N/mm<NUM>, <NUM> or <NUM> corresponding to a press time factor of <NUM>/mm or <NUM>/mm (board thickness was adjusted by two steel spacing strips which were inserted in the press).

Claim 1:
Use of a binder composition comprising
a) Component A comprising amino acid polymer(s) A1 and
b) Component B comprising component B1 selected from the group consisting of pentoses, hexoses, and disaccharides of pentoses and/or hexoses and mixtures thereof,
wherein the amino acid polymer(s) A1 has(have) a total weight average molecular weight Mw,totalof at least <NUM>/mol and at most <NUM>,<NUM>/mol and wherein the binder composition comprises at least <NUM> wt.-% amino acid polymer(s) A1 based on the total weight of the amino acid polymer(s) A1 and component B1,
for producing a multi-layer particle board comprising a core layer and at least one surface layer, wherein the surface layer comprises said binder composition, and the core layer comprises a binder selected from the group consisting of urea/formaldehyde binder, phenol/formaldehyde binder, melamine/urea/formaldehyde binder, PMDI binder and mixtures thereof.