Process for the production of epoxy silicate foam

Inorganic oxidated silicon compounds will react chemically with an amine and an epoxy compound to produce an epoxy silicate prepolymer that will produce a self-standing foam upon heating.

BACKGROUND OF THE INVENTION 
This invention relates to the production of epoxy silicate foams by the 
chemical reaction of an inorganic oxidated silicon compound with an 
organic amine compound and an epoxy compound. The product produced by this 
invention will be referred to as epoxy silicate foam for the purpose of 
this application. 
Various inorganic silicates and related oxidated silicon compounds such as 
silicoformic acid, hydrated silica, and silicates containing free silicic 
acid groups may be used in this invention. It is preferred that the 
inorganic silicates, silicon dioxide, silica, hydrated silica, and 
mixtures thereof be in the form of a fine granular or powdered compound. 
The silicoformic acid may be produced by the methods of U.S. Pat. Nos. 
3,956,466, 3,993,737, and 3,962,111. 
The silica (SiO.sub.2) and hydrated silica (SiO.sub.2.H.sub.2 O) may be 
produced by any of the commonly known methods. Hydrated silica may be 
produced by reacting an acid with an aqueous solution of sodium silicate, 
thereby producing a silicic gel which is then dried thereby forming a 
hydrated silica. 
Any suitable inorganic silicate may be used in this process. Silicates, 
containing free silicic acid groups are preferred. Many of the common 
silicates may be used in this process such as clay, talc, alkali metal 
silicates, alkaline earth metal silicates, zeolite, magnesium silicate, 
diatomaceous earth, soapstone, tremoline, feldspar, kaolin and other 
silicates. 
The epoxy silicate foam may be produced as rigid foams, semirigid foams, 
soft foams, and rubbery soft foams. The foams may be expanded from 3 to 10 
times the original liquid volume. The epoxy silicate foams have a number 
of diverse applications. They may be molded into useful foam objects. They 
may be foamed in place. They may be used for insulation, floatation, 
strengthening material and packaging material. The epoxy silicate foams 
may be produced in the form of a soft foam which can be used as a 
packaging material to protect fragile objects and is biodegradable. It 
disintegrates when it becomes wet unless modified by additives. 
SUMMARY OF THE INVENTION 
I have discovered that oxidized silicon compounds such as silicon dioxide, 
silicoformic acid, hydrated silica, silica, inorganic silicates, and 
mixtures thereof, when mixed in appropriate proportions with a suitable 
epoxy compound and a suitable catalyst, will react chemically to produce 
an epoxy silicate prepolymer, and when heated or an appropriate catalyst 
added, will produce a self-standing foam. The proportions of the oxidized 
silicon compounds, amine catalyst and epoxy compounds may be varied, for 
example, to produce a foam ranging from a soft rubbery foam, to a soft 
foam, to a semi-rigid foam and to a rigid foam. 
The reactants may be mixed in any suitable proportions, depending upon the 
product characteristics desired. Generally, from about 0.5 to 5 parts by 
weight of oxidized silicon compounds and from 1 to 3 parts by weight of an 
amine compound are mixed with 3 to 5 parts by weight of an epoxy compound. 
The preferred process of this invention is to mix the fine granular 
oxidized silicon compound with an organic diamine and then slowly add the 
epoxy compound while agitating and keeping the temperature below 
70.degree. C until a prepolymer is produced. When it desirable, then the 
epoxy silicate prepolymer may be heated to 80.degree. to 100.degree. C 
while agitating for a few minutes until the foaming process starts. The 
prepolymer expands to 3 to 10 times its liquid volume and produced a free 
standing foam. To improve properties of the foam, it may be heated at 
100.degree. to 150.degree. C for 1 to 2 hours. 
The reactions of this invention may take place under any suitable physical 
condition. While many of the reactions will take place acceptably at 
ambient temperature and pressures, in some cases, better results may be 
obtained at somewhat elevated temperatures and pressures. Preferable, the 
reaction takes place at a temperature between 25.degree. and 100.degree. 
C. On the other hand, where the reaction is exothermic, it may be 
desireable to cool the reaction vessel. With some products it is desirable 
to heat the foam at 100.degree. to 150.degree. C for 1 to 2 hours. 
The exact course of the reactions which take place during the process to 
produce epoxy silicate foams cannot be determined with 100% certainty. The 
exact chemical formulae for the epoxy silicate foams are not known. 
Any suitable epoxy compound may be used in this process. Typical epoxy 
compounds include epichlorohydrin, glycidol, methyl epichlorohydrin, 
1,2-epoxybutane, 1,2-epoxycyclohexane, epoxyethane, 1,2-epoxypropane, 
1-chloro-2,3-epoxypropane, 1:2,3:4-diepoxybutane, 
2:3,6:7-diepoxy-2,6-dimethyl-4-octene, epoxyethylbenzene and mixtures 
thereof. Of these, best results are obtained with epichlorohydrin which 
is, therefore, the preferred epoxy compound. 
Any suitable epoxidized polyhydroxy compounds may be used in this process. 
The epoxides of polyhydroxy compounds are produced by chemically reacting 
a peroxy acid such as peroxyacetic acid, peroxybenzoic acid and peroxyacid 
which are produced by oxidizing organic aldehydes. 
Any suitable epoxidized oils may be used in this process. The epoxidized 
oils are produced by chemically reacting peroxy acids with unsaturated 
vegetable oil such as castor oil. 
Any suitable epoxidized unsaturated organic compounds may be used in this 
process. The epoxidized unsaturated organic compounds are produced by the 
chemical reaction of diolefin or polyolefin compounds with peroxy acid 
compounds to produce epoxy compounds by epoxidation. 
Any suitable epoxidized polyhydroxy compounds produced by the chemical 
reaction of epichlorohydrin with a polyhydroxy compound may be used in 
this process. 
Any suitable epoxidized unsaturated fatty acid may be used in this process. 
The unsaturated fatty acids may be chemically reacted with epichlorohydrin 
or a peroxy acid compound to produce the epoxidized unsaturated fatty 
acid. 
Best results are obtained when the epoxidized unsaturated organic 
compounds, epoxidized polyhydroxy compounds, epoxidized fatty acid, 
phenoxy resins and epoxidized vegetable oils are used with epichlorohydrin 
in the production of epoxy silicate foams. The ratio of the parts by 
weight of epoxidized compounds to the parts by weight of epichlorohydrin 
may be quite varied, ranging from 2 to 1 up to 1 to 2. The epoxidized 
compounds or resins should have 2 or more reactive epoxy groups per 
molecule for the purpose of this invention. 
Any of the epoxy resins may be used which contain 2 or more reactive epoxy 
groups per molecule such as that produced by reacting epichlorohydrin with 
bisphenol A and diglycidyl ether of bisphenol. The epoxy resins with 2 or 
more reactive epoxy groups per molecule are obtained by condensing 
epichlorohydrin with a suitable dihydroxy organic compound. Best results 
are obtained when using bisphenol A [2,2-(4-bis-hydroxy-phenyl)-propane] 
and this is considered to be the preferred hydroxy compound. Other hydroxy 
containing compounds such as resorcinol, hydroquinone glycols, glycerol 
and mixtures thereof may be used in mixture with or in lieu of the hydroxy 
alkanes if desired. Any suitable di(mono-hydroxy) alkane may be chemically 
reacted with epichlorohydrin and used in this invention. Typical 
di(mino-hydroxy) alkanes are: (4,4'-dihydroxy-diphenyl-methane; 2,2-(4 
bis-hydroxy phenyl)-propane; 1,1-(4,4'-dihydroxy-diphenyl)cyclohexane; 
1,1(4,4'-dihydroxy-3,3'-dimethyl-diphenol)-butane; 
2,2-(2,2-dihydroxy-4,4'-di-tert-butyldiphenyl)-propane; 
2,2-(4,4'-dihydroxy-diphenyl)butane; 2,2-(4,4'-dihydroxy-diphenyl)pentane; 
3,3-(4,4'-dihydroxy-diphenyl) pentane; 
2,2-(4,4'-dihydroxy-diphenyl)hexane; 3,3-(4,4'-dihydroxydiphenyl)hexane; 
2,2-(4,4'-dihydroxy-diphenyl)-4-methyl-pentane; 
(dihydroxy-diphenyl)-heptane; 4,4'-(4,4'-dihydroxy-diphenyl)-heptane; 
2,2-(4,4'-dihydroxy-diphenyl)-tri decane; 
2,2-(4,4'-dihydroxy-3'methyl-diphenyl)-propane; 
2,2-(4,4'-dihydroxy-3-methyl-3'-isopropyldiphenyl)butane; 
2,2-(3,5,3',5'-tetra-chloro-4,4'-dihydroxy-diphenyl) propane; 
2,2-(3,5,3',5'-tetrabromo-4,4'-dihydroxy-diphenyl)propane; 
(3,3'-dichloro-4,4'-dihydroxy-diphenyl)-methane; 
(2,2'-dihydroxy-5,5'-difluoro-diphenyl)methane; 
(4,4'-dihydroxy-diphenyl)-phenyl-methane; 
1,1'-4,4'-dihydroxy-diphenyl-1-phenyl-ethane and 
1,1'-(4,4'-dihydroxy-diphenyl)-1-phenyl-ethane. 
Any suitable catalyst may be used to initiate, promote, or modify the 
chemical reaction. Typical catalysts include various mineral acids, Lewis 
acids and organic amine compounds. Organic amines have been found to both 
act as a catalyst and enter into the reaction and become part of the epoxy 
silicate foam. Aliphatic and aromatic amines have been found to be most 
useful. Primary amines are more effective than secondary and tertiary 
amines and are, therefore, perferred. Optimum results have been obtained 
with polyfunctional aliphatic amines such as diethylenetriamine, since the 
reaction takes place rapidly at room temperature to form apparently highly 
cross-linked structures. If desired, complex or adduct amines may be used. 
Typical amines include methylamine, ethylamine, propylamine, 
isopropylamine, butylamine, amylamine, hexylamine, aniline, toluidine 
amine, xylidine amine, phenylenediamine, naphthylamine benzylamine, 
ethylenediamine, tetramethylenediamine, pentamethylenediamine, 
hexamethylenediamine, octamethylenediamine, decamethylenediamine, 
xylylenediamine, piperazine, diethylenetriamine, triethylenetetramine, 
tetraethylenepentamine, and mixtures thereof. The polyamine catalyst may 
first be reacted with dicarboxyl acids, dicarboxyl anhydrides, epoxy 
compounds and carbon disulfide to produce polyamine compounds with 
unreacted amine groups. 
Any suitable modifying or additive compounds may be used in the reaction of 
this invention to vary properties of the product. Typical additives 
include, dicarboxylic anhydrides, dicarboxylic acids, di and polyhydroxy 
compounds, polysulfide polymers, alkali sulfides, sodium polysulfide, 
aminoplasts, phenoplasts, fatty or rosin acids, furfural-ketone resins, 
aldehydes, ketones, dibutyl phthalate, tricresyl phosphate, polyamides, 
fatty acid diamines, styrene oxides, acetonitrile, primary sulfonamides, 
secondary aromatic sulfonamides, disecondary sulfonamides, polymerized 
oils, carbon disulfide, soya bean oil, polyamide resins, wood flour, wood 
fibers, cellulose, lignin, cellulose derivitives, polyester polymers, 
polyether polymers, poly(acrylic acid)polymers, vegetable oils, melamine 
furan compounds vinyl monomers and polymers, phenols, allyl alcohol, allyl 
chloride alkali metal cyanides, urethane polymers, isocyanides, 
diisocyanides, polyisocyanides, thioplasts, furan resins, alginic acid, 
aliphatic dienes, halogenated aliphatic and aromatic compounds, sulfur, 
Thiokol polymers, triallyl cyanurate, heterocyclic vinyl compounds and 
polymers, diethyl oxalate, diallyl phthalate, sulphonated castor oil, 
paraffin oil, and mixtures thereof. 
The amount of modifying or additive compounds and resins may be varied 
greatly from a small amount to up to equal weight of the epoxy silicate 
prepolymer. The modifying or additive compounds and resins may be added in 
the first step in the production of epoxy silicate prepolymers or added 
after the epoxy silicate prepolymers have been produced but before the 
foaming begins. 
The epoxy silicate foams may be modified by adding an alkali compound to 
react with epoxy compounds containing a halide, to improve the strength 
and decrease the hydroscopic properties. The foam becomes more elastic and 
does not tear as easily. The alkali compound is added in the ratio of 
about 0.5 to 1 mol per mol of the epoxy compound containing a halide. The 
alkali compounds include sodium hydroxide, potassium hydroxide, sodium 
oxide, potassium oxide, sodium silicate, sodium polysulfide, sodium 
carbonate, potassium carbonate, sodium cyanide, soda lime, calcium 
hydroxide, alkali metal salts of weak dicarboxyl acids, alkali metal 
phenols, alkali metal polyhydroxy aliphatic and aromatic compounds, alkali 
metal salts of poly(acrylic acid) polymer, alkali metal salts of 
poly(methacrylic acid) polymers, ammonia, ammonia salts of weak acids and 
mixtures thereof. 
Additives may be added to emulsify the mixture, to modify the cells in the 
foam, to regulate the foaming and to stabilize the foam. The mixture may 
be emulsified with alkali soaps, metalic soaps such as zinc stearate and 
calcium stearates and detergents. The cells in the foam may be modified, 
regulated and stabilized by the addition of additives such as metallic 
powders, ethyl cellulose, chlorinated natural rubber, polyvinyl acetate, 
polyvinyl chlorides, metallic salts, alkylated phenoxy polyethoxoxy 
ethanol, sodium dioctyl sulfosuccinate dioctyl calcium sulfosuccinate, 
dioctyl sulfosuccinate, methyl morpholine, diethylethanolamine, dimethyl 
ethanol amine, manganous chloride and mixtures thereof. 
Any suitable isocyanate may be used to improve the epoxy silicate foam such 
as toluene-2,4-diisocyanate, toluene-2,6-diisocyanate, 
diphenylmethane-2,4-diisocyanate, meta-phenylene, diisocyanate, 
triphenylmethane triisocyanate, hexamethylene diisocyanate, 
dichloroxenylene diisocyanate, naphthalene-1,5-diisocyanate, diphenyl 
sulfone-1,4-diisocyanate, 2-nitrodiphenyl-4,4'diisocyanate, fluorene 
diisocyanate, 3,3'-dimethyldiphenylmethane-4,4'-diisocyanate, and mixtures 
thereof. 
The primary object of the present invention is to produce epoxy silicate 
foams. Another object is to produce epoxy silicate foams that may be used 
as an insulation material. Another object is to produce epoxy silicate 
prepolymers that can be heated in a mold and produce a foam that may be 
used to protect fragile objects when shipped, and then, when thrown away, 
will disintegrate.

DESCRIPTION OF PREFERRED EMBODIMENTS 
My invention will be illustrated in greater detail in the specific examples 
which follow, which detail the preferred embodiments of my process. It 
should be understood that the scope of my invention is not limited to the 
specific processes set out in the examples. Parts and percentages are by 
weight, unless otherwise indicated. 
EXAMPLE I 
About 4 parts by weight of fine granular silica and 2 parts by weight of 
diethylenetriamine are mixed, then 3 parts by weight of epichlorohydrin 
are slowly added while agitating at ambient pressure and keeping the 
temperature between ambient temperature and 70.degree. C for 10 to 20 
minutes until a thick, gray-colored liquid is produced, containing epoxy 
silicate prepolymer and silica. The temperature is then elevated to 
80.degree. C to 100.degree. C and foaming begins. It expands to about 8 to 
10 times the original volume to produce a semi-rigid foam. The light gray 
to cream-colored foam becomes soft when cooled. 
The foam has good rebounce properties when compressed. It has poor tear 
resistant properties and deteriorates when wet. The foam is useful in 
protecting fragile articles in packages. The foam is bio-degradable; it 
has good insulation properties. 
EXAMPLE II 
About 2 parts by weight of diethylenetriamine are slowly mixed with 3 parts 
by weight of epichlorohydrin while keeping the temperature between ambient 
temperature and 70.degree. C. The chemical reaction is complete in 10 to 
20 minutes. The mixture is stable over a long period of time, unless the 
temperature is elevated above about 80.degree. C. 
About equal parts by weight of a fine granular silica (SiO.sub.2.xH.sub.2 
O) and said mixture are mixed then heated to 80.degree. to 100.degree. C 
while agitating at ambient pressure. When the temperature of the mixture 
reaches about 80.degree. C it begins to foam and expands to about 8 to 10 
times its original volume, thereby producing a soft, cream colored, epoxy 
silicate foam. 
(a) About equal parts by weight of a fine granular hydrated silica and said 
mixture of reacted epichlorohydrin and diethylenetriamine are mixed then 
heated while agitating under ambient pressure, and as the temperature 
reaches between 80.degree. to 100.degree. C the mixture begins to foam and 
expands to 8 to 10 times its original volume, thereby producing a light 
gray-colored, soft, epoxy silicate foam. 
(b) About equal parts by weight of a fine granular silicate compound (talc) 
and said mixture of chemically reacted epichlorohydrin and 
diethylenetriamine are mixed then heated while agitating under ambient 
pressure, and when the temperature reaches 80.degree. to 100.degree. C the 
mixture begins to foam and expands to 8 to 10 times its original volume, 
thereby producing a cream colored, soft, epoxy silicate foam. 
(c) About 2 parts by weight of a granular sodium metasilicate pentahydrate 
and about 5 parts by weight of said mixture of chemically reacted 
diethylenetriamine epichlorohydrin are mixed then heated while agitating 
at ambient pressure, and when the temperature reaches 80.degree. to 
100.degree. C the mixture begins to foam and expands to 3 to 8 times its 
original volume, thereby producing a white, soft, rubbery, epoxy silicate 
foam. The epoxy silicate foam is then heated in an oven at 100.degree. to 
120.degree. C for 1 to 2 hours. 
EXAMPLE III 
About 2 parts by weight of diethylenetriamine and 3 parts by weight of 
epichlorohydrin are slowly mixed over a period of 10 to 20 minutes while 
agitating and keeping the temperature below 70.degree. C until the mixture 
becomes thick. The exothermic reaction elevates the temperature to between 
80.degree. to 100.degree. C, and the mixture begins to foam, thereby 
expanding to 6 to 8 times its original volume, but, as it begins to cool, 
the foam shrinks to about 2 to 3 times its original volume, thereby 
producing a light yellow, brittle, epoxy foam. 
EXAMPLE IV 
2 parts by weight of ethylenediamine, 1 part by weight of sodium carbonate, 
and 6 parts by weight of epichlorohydrin are slowly mixed, thereby 
producing a light yellow resinous product. The resinous product is heated 
to 80.degree. to 100.degree. C for several minutes but does not foam. 
About 4 parts by weight of fine granular silica are mixed with the 
resinous product then heated while agitating, and when the temperature 
reaches 80.degree. to 100.degree. C the mixture expands into a foam of 
about 6 to 8 times its original volume, thereby producing a cream colored, 
soft, epoxy silicate foam. 
EXAMPLE V 
About 2 parts by weight of fine granular silica, 1 part by weight of 
diethylenetriamine and 4 parts by weight of epichlorohydrin are slowly 
mixed while keeping the temperature below 70.degree. C, thereby producing 
a thick liquid epoxy silicate prepolymer. The epoxy silicate propolymer is 
heated to 80.degree. to 100.degree. C and forms a hard, solid resin. 
EXAMPLE VI 
About 2 parts by weight of fine granular magnesium silicate and 2 parts by 
weight of diethylenetriamine are mixed, then 3 parts by weight of 
epichlorohydrin are slowly added while agitating and keeping the 
temperature below 70.degree. C until all the epichlorohydrin has been 
added; then let the temperature rise to 80.degree. to 100.degree. C and 
the mixture expands to 6 to 8 times its original volume, thereby producing 
a dark brown semi-rigid, epoxy silicate foam. 
EXAMPLE VII 
3 parts by weight of epichlorohydrin are slowly added to 2.5 parts by 
weight of 1,6-hexanediamine while agitating at ambient pressure and 
keeping the temperature below 70.degree. C. About 2 parts by weight of 
fine granular silica are added and mixed then heated while agitating at 
ambient pressure to 80.degree. to 100.degree. C, and the mixture begins to 
expand to 4 to 6 times its original volume, thereby producing an epoxy 
silicate foam, semi-rigid and light gray in color. 
EXAMPLE VIII 
2 parts by weight of diethylenetriamine, 1 part by weight of sodium 
hydroxide flakes and 1 part by weight of fine granular silica are mixed, 
then 3 parts by weight of epichlorohydrin are added slowly while agitating 
at ambient pressure while keeping the temperature between ambient 
temperature and 70.degree. C over a period of 10 to 30 minutes, thereby 
producing an epoxy silicate propolymer. The epoxy silicate prepolymer is 
then heated to 80.degree. to 100.degree. C while agitating for a few 
minutes until foaming begins. The foam expands to about 6 to 8 times its 
original volume, thereby producing a soft, cream colored epoxy silicate 
foam. 
EXAMPLE IX 
Production of epoxy silicate foam by using 2 separate mixtures: 
A. one part by weight of sodium hydroxide flakes, 2 parts by weight of 
water, 2 parts by weight of 1,6-hexanediamine and 2 parts by weight of 
epichlorohydrin are mixed then heated to about 70.degree. C for 10 to 30 
minutes, thereby producing a thick gray epoxy prepolymer. 
B. 2 parts by weight of ethylenediamine and 2 parts by weight of fine 
granular silica are mixed, then 3 parts by weight of epichlorohydrin are 
slowly added while agitating at ambient pressure while keeping the 
temperature below 70.degree. C, thereby producing an epoxy silicate 
prepolymer. 
The epoxy prepolymer and the epoxy silicate prepolymer of parts A and B are 
mixed, then a foam regulator, in the amount of 0.01 parts by weight of 
sodium dioctyl sulfosuccinate, are mixed in and then heated to 80.degree. 
to 100.degree. C while agitating until the mixture begins to expand. It 
expands to about 6 to 8 times the original volume, thereby producing a 
gray, semi-rigid epoxy silicate foam. 
EXAMPLE X 
2 parts by weight of fine granules of clay, 3 parts by weight of 
1,6-hexanediamine and 3 parts by weight of epichlorohydrin are mixed then 
agitated at ambient pressure while keeping the temperature between 
25.degree. to 70.degree. C for 10 to 30 minutes, thereby producing an 
epoxy silicate propolymer. The epoxy silicate prepolymer is then heated to 
80.degree. to 100.degree. C while agitating until it begins to expand. It 
expands to about 5 to 8 times its original volume, thereby producing light 
gray, soft epoxy silicate foam. 
EXAMPLE XI 
Production of epoxy silicate foam by using 2 separate mixtures: 
A. 2 parts by weight of epichlorohydrin and 0.25 parts by weight of 
concentrated phosphoric acid are mixed. The mixture is agitated for 10 to 
20 minutes, thereby producing polyepichlorohydrin polymer. About 1 part by 
weight of sodium hydroxide flakes is added to the mixture and heated to 
just above the melting point of sodium hydroxide flakes, thereby producing 
a tan polyepichlorohydrin polymer. 
B. about 2 parts by weight of ethylenediamine and 2 parts by weight of fine 
granular silica are mixed, then 3 parts by weight of epichlorohydrin are 
slowly added while agitating at ambient pressure while keeping the 
temperature below 70.degree. C, thereby producing an epoxy silicate 
prepolymer. 
The tan polyepichlorohydrin produced in B are mixed then agitated while 
heating to 80.degree. to 100.degree. C until the mixture expands to 5 to 8 
times its original volume and then is heated in an oven at 80.degree. to 
120.degree. C for 1 to 2 hours, thereby producing a semi-rigid, light gray 
colored, tough epoxy silicate foam. 
EXAMPLE XII 
2 parts by weight of diethylenetriamine, 1 part by weight of fine granular 
hydrated silica, 1 part by weight of fine granular silica, and 4 parts by 
weight of diglycedyl ether of bisphenol epoxy resin containing 2 or more 
reactive epoxy groups per molecule are mixed then heated to 80.degree. to 
100.degree. C while agitating at ambient pressure for 3 to 10 minutes 
until the mixture begins to expand, thereby producing a cream colored, 
rigid epoxy silicate foam. 
EXAMPLE XIII 
2 parts by weight of diethylenetriamine, 4 parts by weight of bisphenol A 
epoxy resin with 2 or more reactive epoxy groups per molecule and 2 parts 
by weight of fine granular talc powder are mixed then heated to 80.degree. 
to 100.degree. C while agitating for 3 to 10 minutes until the mixture 
begins to expand, thereby producing a cream colored, rigid epoxy silicate 
foam which has expanded 5 to 8 times its original liquid volume. The foam 
may be used to strengthen hollow objects and for insulation. 
EXAMPLE XIV 
2 parts by weight of triethylenetetramine, 3 parts by weight of 
epichlorohydrin, 2 parts by weight of a fine granular silicoformic acid 
and hydrated silica mixture, and epoxidized castor oil containing 2 or 
more reactive epoxy groups per molecule are slowly mixed and then agitated 
for 10 to 20 minutes while keeping the temperature between 25.degree. to 
70.degree. C. The mixture is then heated to 80.degree. to 100.degree. C 
while agitating for 3 to 10 minutes until the mixture begins to expand, 
thereby producing a cream colored, soft, tough epoxy silicate foam. 
EXAMPLE XV 
About 1 part by weight of diethylenetriamine, 1 part by weight of 
caprolactam, 2 parts by weight of a fine granular silica, 1 part by weight 
of sodium polysulfide, and 1 part by weight of 1,2-epoxypropane are mixed; 
then 2 parts by weight of epichlorohydrin are slowly added while agitating 
for 10 to 20 minutes, at ambient pressure, thereby producing an epoxy 
silicate prepolymer. The epoxy silicate prepolymer is then poured into a 
mold then heated to 80.degree. to 100.degree. C while agitating for 3 to 
10 minutes until the mixture begins to expand, thereby producing a soft, 
rubbery, light yellow colored, epoxy silicate foam which has expanded 6 to 
8 times its original liquid volume. 
EXAMPLE XVI 
About 1 part by weight of sodium hydroxide flakes and about 1 part by 
weight of sulfur are mixed then heated to above the melting temperature of 
sulfur while agitating for 10 to 20 minutes. To the above mixture is added 
2 parts by weight of a fine granular silica, and 2 parts by weight of an 
amino-terminated polymerized oil resin; then 4 parts by weight of 
epichlorohydrin are slowly added while agitating at ambient pressure for 
10 to 20 minutes while keeping the temperature between 25.degree. to 
70.degree. C. The mixture is then heated to 80.degree. to 100.degree. C 
while agitating for 3 to 10 minutes until the mixture begins to expand, 
thereby producing a light yellow, rubbery, soft epoxy silicate foam. 
EXAMPLE XVII 
About 2 parts by weight of a fine granular silica, 2 parts by weight of 
ethylenediamine and 1 part by weight of sodium hydroxide flakes are mixed 
then heated to just below the boiling temperature of ethylenediamine for 
20 to 40 minutes at ambient pressure, thereby producing an aminosilicate 
compound. Then 2 parts by weight of an epoxidized unsaturated fatty acid 
containing 2 or more active epoxy groups per molecule and 3 parts by 
weight of epichlorohydrin are slowly mixed with the aminosilicate compound 
and agitated at ambient pressure for 10 to 20 minutes while keeping the 
temperature between 25.degree. to 70.degree. C, thereby producing an epoxy 
silicate prepolymer. The epoxy silicate prepolymer is then heated while 
agitating to a temperature of 80.degree. to 100.degree. C until the 
mixture begins to expand; it expands 6 to 10 times its original volume, 
thereby producing a cream colored, soft, epoxy silicate foam. 
EXAMPLE XVIII 
About 2 parts by weight of fine granular silica, 2 parts by weight of 
diethylenetriamine, 2 parts by weight of allyl chloride, and 1 part by 
weight of potassium hydroxide are mixed; then about 3 parts by weight of 
epichlorohydrin are slowly added while agitating and keeping the 
temperature between 25.degree. to 70.degree. C for 10 to 20 minutes at 
ambient pressure, thereby producing an epoxy silicate prepolymer. The 
epoxy silicate prepolymer is then heated to 80.degree. to 100.degree. C 
while agitating until the mixture begins to expand; it expands 6 to 10 
times its original volume, thereby producing a soft, rubbery, cream 
colored epoxy silicate foam. 
EXAMPLE XIX 
About 1.5 parts by weight of fine granular diatomaceous earth, 2 parts by 
weight of sulfate lignin as produced by the Kraft process (soda process) 
and 2 parts by weight of ethylenediamine are mixed; then 3 parts by weight 
of epichlorohydrin are slowly added while agitating at ambient pressure 
and keeping the temperature between 25.degree. to 70.degree. C for 10 to 
20 minutes until the reaction is substantially complete, thereby producing 
an epoxy silicate prepolymer. The epoxy silicate prepolymer is then heated 
to 80.degree. to 100.degree. C while agitating until the mixture begins to 
expand. The mixture expands 6 to 10 times its original volume thereby 
producing a brown, soft, epoxy silicate foam. 
This epoxy silicate foam may be utilized for insulation and for the 
protection of fragile products in shipping. 
EXAMPLE XX 
About 3 parts by weight of fine granular pectolin, 1 part by weight of 
sodium salt of sulfite lignin, 1 parts by weight of calcium sulfite lignin 
and 2 parts by weight of diethylenetriamine are mixed; then 4 parts by 
weight of epichlorohydrin are slowly added while agitating and keeping the 
temperature between 25.degree. to 70.degree. C for 10 to 20 minutes, 
thereby producing an epoxy silicate prepolymer. The epoxy silicate 
prepolymer is poured into a mold then heated to 80.degree. to 100.degree. 
C while agitating until the mixture begins to expand, thereby producing a 
brown, soft, epoxy silicate foam. 
EXAMPLE XXI 
About 2 parts by weight of fine granular hydrated silica, 2 parts by weight 
of a liquid (300 to 1500 poises) polyester resin (produced by chemically 
reacting 15 mols of diethylene glycol and 1 mol of trimethylol propane 
with 15 mols of adipic acid) and 2 parts by weight of diethylenetriamine 
are mixed; then 3 parts by weight of epichlorohydrin are slowly added 
while agitating for 10 to 20 minutes at ambient pressure and keeping the 
temperature between 25.degree. to 70.degree. C, thereby producing a light 
gray, thick liquid, epoxy silicate prepolymer. The epoxy silicate 
prepolymer is poured into a mold then heated to 80.degree. to 100.degree. 
C while agitating until the mixture begins to expand, thereby producing a 
soft, cream colored, rubbery epoxy silicate foam. The foam is then heated 
at 100.degree. to 150.degree. C for 1 to 2 hours. 
EXAMPLE XXII 
About 2 parts by weight of fine granular silica, 2 parts by weight of a 
liquid (300 to 1500 poises) polyester containing 4 mols of glycerol, 3 
mols of adipic acid and 0.5 mols of phthalic anhydride, and 2 parts by 
weight of diethylenetriamine are mixed; then 3.5 parts by weight of 
epichlorohydrin are slowly added while agitating and keeping the 
temperature between 25.degree. to 70.degree. C for 10 to 20 minutes, 
thereby producing a thick, light gray, liquid, epoxy silicate prepolymer. 
About 0.01 parts by weight of dioctyl sulfosuccinate are mixed in the 
epoxy silicate propolymer and is then heated to 80.degree. to 100.degree. 
C while agitating for a few minutes until the mixture begins to expand. 
The mixture expands 6 to 10 times its original volume, thereby producing a 
cream colored, semirigid, epoxy silicate foam. The foam is then heated to 
100.degree. to 150.degree. C for 1 to 2 hours. 
EXAMPLE XXIII 
About 2 parts by weight of fine granular silica, 1.5 parts by weight of a 
polyester resin (containing 1 mol of phthalic anhydride, 3 mols of maleic 
anhydride, 4 mols of ethylene glycol and 2 mols of styrene), 1 part by 
weight of ethylenediamine and 1 part by weight of 1,6-hexanediamine are 
mixed; then 4 parts by weight of epichlorohydrin are slowly added while 
agitating and keeping the temperature between 25.degree. to 70.degree. C 
for 10 to 20 minutes, thereby producing a thick, light gray, liquid, epoxy 
silicate prepolymer. The epoxy silicate prepolymer is then poured into a 
mold then heated to 80.degree. to 100.degree. C while agitating; in 3 to 5 
minutes the mixture begins to expand; the agitating is stopped and the 
mixture expands to 6 to 10 times its original volume, thereby producing a 
cream colored, soft, epoxy silicate foam. The foam is then heated to 
100.degree. C to 150.degree. C for 1 to 2 hours. 
EXAMPLE XXIV 
2 parts by weight of a fine granular silica, 2 parts by weight of 
diethylenetriamine, 1 to 2 parts by weight of polyethylene glycol (200 to 
500 molecular weight), 1 part by weight of sodium hydroxide flakes are 
mixed; then 3 parts by weight of epichlorohydrin are slowly added while 
agitating and keeping the temperature between 25.degree. to 70.degree. C 
for 10 to 20 minutes at ambient pressure, thereby producing an epoxy 
silicate prepolymer. The epoxy silicate prepolymer is then heated to 
80.degree. to 100.degree. C while agitating until the mixture expands. The 
mixture expands 6 to 8 times its original volume, thereby producing a 
soft, cream colored, epoxy silicate foam. 
EXAMPLE XXV 
About 0.5 parts by weight of fine granular silica, 3 parts by weight of 
1,6-hexanediamine, 2 parts by weight of epichlorohydrin, 2 parts by weight 
of 1:2,3:4-diepoxybutane, 1 part by weight of sodium hydroxide flakes and 
1 to 2 parts by weight of castor oil are mixed then agitated while keeping 
the temperature between 25.degree. to 70.degree. C for 10 to 20 minutes. 
The temperature is then raised to 80.degree. to 100.degree. C for 3 to 5 
minutes, and the mixture expands 6 to 10 times its original volume, 
thereby producing a cream colored semirigid epoxy silicate foam. 
EXAMPLE XXVI 
Epoxy silicate foam is produced by the following steps: 
(a) 3 parts by weight of a fine granular silica, 2 parts by weight of 
diethylenetriamine, and 1 part by weight of maleic anhydride are mixed; 
then 3 parts by weight of epichlorohydrin are slowly added while agitating 
and keeping the temperature between 25.degree. to 70.degree. C for 10 to 
20 minutes, thereby producing an epoxy silicate prepolymer; 
(b) 1 to 2 parts by weight of toluene diisocyanate (80% 2,4 and 20% 2,6) 
and 2 parts by weight of epichlorohydrin are mixed then added slowly to 
the epoxy silicate prepolymer produced in part (a) while agitating and 
keeping the temperature between 25.degree. to 70.degree. C for 10 to 20 
minutes; the temperature is then increased to 80.degree. to 100.degree. C 
until the mixture begins to expand, thereby producing a tan colored, 
semirigid epoxy silicate foam that has expanded to 6 to 10 times its 
original volume. 
EXAMPLE XXVII 
About 1 to 2 parts by weight of unsaturated fatty acid, 0.5 parts by weight 
of sodium hydroxide flakes and 1 part by weight of epichlorohydrin are 
mixed then heated to just below the boiling temperature of epichlorohydrin 
for about 30 minutes. About 2 parts by weight of fine granular silica and 
2 parts by weight of ethylenediamine are added to the mixture; then 3 
parts by weight of epichlorohydrin are slowly added while agitating for 10 
to 20 minutes while keeping the temperature between 25.degree. and 
70.degree. C, thereby producing a light gray colored epoxy silicate 
prepolymer. The epoxy silicate prepolymer is then heated to 80.degree. to 
100.degree. C while agitating until the mixture begins to expand. The 
mixture expands to 6 to 10 times its original volume to produce a cream 
colored soft epoxy silicate foam. 
EXAMPLE XXVIII 
About 1 part by weight of glycerol, 0.5 parts by weight of sodium hydroxide 
flakes and 1 part by weight of epichlorohydrin are mixed then heated to 
just below the boiling temperature of epichlorohydrin while agitating for 
about 30 minutes. 2 parts by weight of diethylenetriamine and 2 parts by 
weight of fine granular silica are added and mixed with the epoxidized 
glycerol; then 3 parts by weight of epichlorohydrin are slowly added while 
agitating for 10 to 20 minutes and keeping the temperature between 
25.degree. to 70.degree. C, thereby producing an epoxy silicate 
prepolymer. The epoxy silicate prepolymer is then heated to 80.degree. to 
100.degree. C while agitating for 3 to 10 minutes until the mixture begins 
to expand. The mixture expands to 6 to 10 times its original volume, 
thereby producing an epoxy silicate foam. 
Although specific conditions and ingredients have been described in 
conjunction with the above examples of preferred embodiments, these may be 
varied and other reagents and additives may be used, where suitable, as 
described above, with similar results. 
Other modifications and applications of this invention will occur to those 
skilled in the art upon reading this disclosure. These are intended to be 
included within the scope of this invention as defined in the appended 
claims.