jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: M. Lusi
Source: Acta Crystallographica Section A Foundations and Advances (article, 2022-08-23)
Field: Chemistry — Physical and Theoretical Chemistry

Solid solutions as a means to investigate and exploit the structure–property relationships in molecular crystals Current strategies for the rational design of crystal structure and the optimization of their properties rely on the exploitation of known supramolecular interactions and the application of rough practical experimental rules on thumbs.This approach enable the prediction of general structural features but does not allow for fine tuning and properties optimization.On the contrary the continuous stoichiometry variation that is typical of substitutional solid solutions offers a better control of structures and properties.Here a series of solid solutions are presented to control solubility and thermal stability in multidrug solid forms.At the same time, stoichiometry variation in these phases give insight into the relative strength of different supramolecular interactions.In particular, a cocrystals that combines enantiomers of a chiral drug and a multiple chiral conformer exemplifies the potential of these materials to synthetic crystallography and crystal engineering. Exploit ; Property (philosophy) ; Materials science ; Crystallography ; Computer science ; Chemistry ; Computer security ; Epistemology ; Philosophy Crystallography and molecular interactions ; Chemical Thermodynamics and Molecular Structure ; Crystallization and Solubility Studies
Authors: Tomás Torres⊗ | Elisa López-Serrano | Marta Gómez‐Gómez | Luis M. Mateo | Jorge Labella | Giovanni Bottari | Mine Ince
Source: ECS Meeting Abstracts (article, 2022-07-07)
Field: Materials Science — Materials Chemistry

(Invited) Porphyrinoid-Carbon Nanostructure Ensembles and Fused Porphyrin-Graphene Nanoribbons Phthalocyanines (Pcs) have emerged as excellent light harvesting antennas for incorporation into D-A systems, mainly in connection with carbon nanostructures, like endohedral metallofullerenes, SWCNT and graphene, as acceptor or donor moieties, in which the Pc has been attached, covalently or through supramolecular interactions. They are among the few molecules that reveal an intense red and NIR absorption and therefore, constitute also promising dyes in molecular photovoltaics. Pcs have a great chemical versatility, which allows to modify their electronic character and their physicochemical properties by organic synthesis, by introducing substituents in the periphery or modifying the structure of the macrocycle. Most recently they have reached good efficiency values participating as hole transporting materials in Carbon-based Perovskite sensitized solar cells (PSSCs). Pcs are be appropriately designed to adapt well to the electronic levels of the different types of perovskites. Through a rational design, structure-property relationships will be established that will gradually improve the performance of the devices. On the other hand, on-surface synthesis offers a versatile approach to fabricate novel carbon-based nanostructures that cannot be obtained via conventional solution chemistry. Within the family of such nanomaterials, graphene nanoribbons (GNRs) hold a privileged position due to their high potential for different applications. One of the key issues for their application in molecular electronics lies in the fine-tuning of their electronic properties through structural modifications, such as heteroatom doping or the incorporation of non-benzenoid rings. In this context, the covalent fusion of GNRs and porphyrins (Pors) represents a highly appealing strategy. Heteroatom ; Nanotechnology ; Supramolecular chemistry ; Materials science ; Graphene ; Porphyrin ; Nanostructure ; Nanomaterials ; Carbon fibers ; Covalent bond ; Carbon nanotube ; Molecule ; Context (archaeology) ; Chemistry ; Photochemistry ; Composite number ; Ring (chemistry) ; Organic chemistry Porphyrin and Phthalocyanine Chemistry ; Molecular Junctions and Nanostructures ; Fullerene Chemistry and Applications
Authors: Jiang Nan | Guanjie Huang | Shilei Liu | Jing Wang | Yangmin Ma | Xinjun Luan
Source: Research Square (preprint, 2022-12-06)
Field: Chemistry — Organic Chemistry

In(OTf)3-Catalyzed Reorganization/Cycloaddition of Two Imine Units and Subsequently Modular Assembly of Acridinium Photocatalysts Imine ; Cycloaddition ; Modular design ; Catalysis ; Chemistry ; Combinatorial chemistry ; Computer science ; Organic chemistry ; Operating system Radical Photochemical Reactions ; Oxidative Organic Chemistry Reactions ; Catalytic C–H Functionalization Methods
Authors: Tzu-Yao Hsu | Roxanne Berthin | Alessandra Serva | Kyle G. Reeves | Mathieu Salanne | Guillaume Jeanmairet
Source: ChemRxiv (preprint, 2022-06-13)
Field: Chemistry — Physical and Theoretical Chemistry

Electron Transfer of Functionalised Quinones in Acetonitrile Quinones are redox active organic molecules that have been proposed as an alternative choice to metal-based materials in electrochemical energy storage devices. Functionalization allows to fine tune not only their chemical stability but also the redox potential and the kinetics of the electron transfer reaction. However, reaction rate constant is not solely determined by the redox species but is also impacted by solvent effects. In this work, we show how the functionalization of benzoquinone with different functional groups impacts the solvent reorganization free energies of electron transfer half-reactions in acetonitrile. The use of molecular density functional theory, whose computational cost for studying electron transfer reaction is considerably reduced compared to state-of-the art molecular dynamics simulations, enables to perform a systematic study. We validate the method by comparing the predictions of the solvation shell structure and the free energy profiles for electron transfer reaction to reference classical molecular dynamics simulations in the case of anthraquinone solvated in acetonitrile. We show that all the studied electron transfer half-reactions follow Marcus’ description, regardless of functional groups. Consequently, the solvent reorganization free energy decreases as the molecular size increases. Electron transfer ; Chemistry ; Acetonitrile ; Redox ; Marcus theory ; Solvation ; Density functional theory ; Chemical physics ; Reaction rate constant ; Electrochemistry ; Molecular dynamics ; Computational chemistry ; Molecule ; Photochemistry ; Physical chemistry ; Kinetics ; Organic chemistry ; Electrode Photochemistry and Electron Transfer Studies ; Free Radicals and Antioxidants ; Organic Chemistry Cycloaddition Reactions
Authors: Alan M. Medina-Gonzalez | Philip Yox | Yunhua Chen | Marquix A. S. Adamson | Bryan A. Rosales | Maranny Svay | Smith, Emily, Selma | Richard D. Schaller | Kui Wu | Aaron Rossini | Kirill Kovnir | Javier Vela
Source: Iowa State University Digital Repository (Iowa State University) (article, 2022-08-10)
Field: Materials Science — Materials Chemistry

Solution-Grown Ternary Semiconductors: Nanostructuring and Stereoelectronic Lone Pair Distortions in I–V–VI2 Materials Alkali pnictogen dichalcogenides─I–V–VI2 or APnCh2─have been identified as promising semiconducting materials for energy conversion devices. However, the controlled nanoscale synthesis and our understanding of the effects of cation ordering and stereochemically active lone pairs on the structures of these ternary compounds remain underdeveloped. Here, we use solution-phase chemistry to synthesize a family of APnCh2 materials, including LiSbSe2, NaSbS2, NaSbSe2, NaBiS2, and NaBiSe2. Our approach utilizes alkali metal hydrides (AH) or carboxylates, A(O2CR), PnPh3, and elemental chalcogens as synthetic precursors and oleylamine or 1-octadecene as solvents. Synthetic manipulation via fine-tuning of reaction temperature enables control over the degree of ordering caused by the Sb 5s2 lone pair-induced distortions in NaSbS2. Pair distribution function analysis demonstrates that the structure of the Sb-containing phases deviates much more from a disordered rock salt structure than that of the Bi-containing phases. This local distortion, induced by the Sb lone pair, leads to a previously unreported noncentrosymmetric NaSbS2 crystal structure, which is additionally supported by second-harmonic generation measurements. Infrared and multinuclear solid-state NMR spectroscopies show that oleylamine or chelating carboxylates and, in some cases, unreacted precursors (LiH and PnPh3) remain bound to the nanocrystalline surfaces. A deeper understanding of the local atomic environment, long-range ordering, surface chemistry, and optoelectronic properties of these materials may speed up their fundamental study and application. Lone pair ; Oleylamine ; Ternary operation ; Pnictogen ; Chalcogen ; Alkali metal ; Nanocrystalline material ; Crystal structure 2D Materials and Applications ; Crystal Structures and Properties ; Chalcogenide Semiconductor Thin Films
Authors: Zohar Eyal | Rachael Deis | Neta Varsano | Nili Dezorella | Katya Rechav | Lothar Houben | Dvir Gur
Source: bioRxiv (Cold Spring Harbor Laboratory) (preprint, 2022-09-30)
Field: Materials Science — Biomaterials

Biogenic plate-like guanine crystals form via templated nucleation of thin crystal leaflets on amyloid scaffolds Abstract Controlling the morphology of crystalline materials is challenging, as crystals have a strong tendency towards thermodynamically stable structures. Yet, organisms form crystals with distinct morphologies, such as the plate-like guanine crystals produced by many terrestrial and aquatic species for light manipulation. Regulation of crystal morphogenesis was hypothesized to entail physical growth restriction by the surrounding membrane, combined with fine-tuned interactions between organic molecules and the growing crystal. Using cryo electron tomography of developing zebrafish larvae, we found that guanine crystals form via templated nucleation of thin leaflets on preassembled scaffolds made of 20-nm-thick amyloid fibers. These leaflets then merge and coalesce into a single plate-like crystal. Our findings provide new insights into how organisms control the morphology and, thereby, the optical properties of crystals. Nucleation ; Crystal (programming language) ; Guanine ; Crystallography ; Materials science ; Crystallization ; Merge (version control) ; Crystal growth ; Morphology (biology) ; Biophysics ; Nanotechnology ; Chemistry ; Biology ; Biochemistry ; Nucleotide Calcium Carbonate Crystallization and Inhibition ; Paleontology and Stratigraphy of Fossils ; Pickering emulsions and particle stabilization
Authors: Rafael F. A. Gomes | Juliana Gomes Pereira | João M. J. M. Ravasco | João R. Vale | Fausto Queda
Source: ChemRxiv (preprint, 2022-01-10)
Field: Chemistry — Organic Chemistry

Direct Diels-Alder reaction of chitin derived 3-acetamido-5-acetylfuran The Diels-Alder (DA) reaction of biomass derived furans is an emerging technology for the preparation of new molecular entities and “drop-in” commodity chemicals. In this work we address the challenge of the direct use of electron-poor furanic platforms as dienes through the use of an unexplored chitin derived furan, 3-acetamido-5-acetylfuran (3A5AF). The 3-acetamido group promoted a remarkable increase in the kinetics of the DA allowing for the preparation of 7-oxanorbornenes (7-ONB) at 50 ºC. Partial hydrolysis of the enamide to hemi-acylaminals was possible upon fine tuning of the reaction conditions, disabling retro-DA processes. Finally, DA reaction of the reduced form of 3A5AF allowed quantitative formation of 7-ONB in aqueous condition after 10 minutes. Certanly these are the first steps for expanding the toolbox of chitin derived 3A5AF as diene. Chemistry ; Furan ; Chitin ; Aqueous solution ; Hydrolysis ; Organic chemistry ; Diels–Alder reaction ; Commodity chemicals ; Combinatorial chemistry ; Chitosan ; Catalysis Oxidative Organic Chemistry Reactions ; Synthetic Organic Chemistry Methods ; Catalytic Alkyne Reactions
Authors: James R. Pankhurst | Laia Castilla Amorós | Dragos Stoian | Jan Vávra | Valeria Mantella | Petru P. Albertini | Raffaella Buonsanti
Source: Zenodo (CERN European Organization for Nuclear Research) (article, 2022-06-30)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Copper-Phosphonate Lamella Intermediates Control the Shape of Colloidal Copper Nanocrystals Understanding the structure and behavior of intermediates in chemical reactions is key to developing greater control over the reaction outcome. This principle is particularly important in the synthesis of metal nanocrystals (NC), where the reduction, nucleation and growth of the reaction intermediate will determine the final size and shape of the product. The shape of metal NCs plays a major role in determining their catalytic, photochemical and electronic properties and, thus, the potential applications of the material. In this work, we demonstrate that layered coordination polymers, called lamellae, are reaction intermediates for Cu NCs. Importantly, we discover that the lamella structure can be fine-tuned using organic ligands of different length and that these structural changes control the shape of the final NC. Specifically, we show that short-chain phosphonate ligands generate lamellae that are persistent enough at the reaction temperature to facilitate the soft-templating of Cu nuclei into anisotropic Cu NCs, being primarily triangular plates. In contrast, lamellae formed from long-chain ligands lose their structure and form spherical Cu NCs. The synthetic approach presented here provides a versatile tool for the future development of metal NCs, including other anisotropic structures. Copper ; Lamella (surface anatomy) ; Phosphonate ; Nanocrystal ; Colloid ; Materials science ; Nanoparticle ; Nanotechnology ; Chemical engineering ; Chemistry ; Metallurgy ; Composite material ; Organic chemistry ; Engineering Gold and Silver Nanoparticles Synthesis and Applications ; nanoparticles nucleation surface interactions ; Laser-Ablation Synthesis of Nanoparticles
Authors: Mario A. Saucedo‐Espinosa | Maximilian Breitfeld | Petra S. Dittrich
Source: Angewandte Chemie (article, 2022-12-28)
Field: Chemistry — Electrochemistry

Titelbild: Kontinuierliche Elektrochemische Synthese von Gold‐Nanopartikeln in Nanoliter‐Reaktoren (Angew. Chem. 5/2023) Gold nanoparticles (AuNPs) are employed in numerous applications, including optics, biosensing, and catalysis. In their Communication (e202212459), Petra S. Dittrich et al. demonstrate the stabilizer-free electrochemical synthesis of AuNPs inside nanoliter-sized reactors. AuNPs with sizes in the range of 30 to 100 nm were produced without the need for additional capping agents. This method opens the way to fine-tune the electrochemical production of gold nanoparticles. Gold nanoparticles (AuNPs) are employed in numerous applications, including optics, biosensing, and catalysis. In their Communication (e202212459), Petra S. Dittrich et al. demonstrate the stabilizer-free electrochemical synthesis of AuNPs inside nanoliter-sized reactors. AuNPs with sizes in the range of 30 to 100 nm were produced without the need for additional capping agents. This method opens the way to fine-tune the electrochemical production of gold nanoparticles. Photochemistry N-Heterocyclic Carbenes DNA Nanotechnology Colloidal gold ; Nanotechnology ; Electrochemistry ; Nanoparticle ; Biosensor ; Catalysis ; Chemistry ; Materials science ; Combinatorial chemistry ; Electrode ; Organic chemistry ; Physical chemistry Electrochemical Analysis and Applications ; Nanomaterials for catalytic reactions
Authors: Showkat Rashid | Auqib Rashid | Bilal A. Bhat
Source: Synthetic Communications (article, 2022-10-06)
Field: Chemistry — Organic Chemistry

A scalable and diversity-oriented synthesis of (±)-paeoveitols Gram scale synthesis of (±)-paeoveitol, a nor-diterpene harboring an unusual benzofuran stitched benzopyran 6/5/6/6 tetracyclic ring system, and its analogues, emanating from bench-top reagents is reported. Scandium triflate-mediated inverse electron demand [4 + 2] cycloaddition reaction between pre-synthesized paeoveitol-D analogue (dienophile) and ortho-quinone methide precursor (diene), both resulting from the same starting material delivered (±)-paeoveitol in decent yield. Fine tuning of the synthetic strategy not only helped to procure scalable quantities of natural product but also provided ample scope to look for the diversity-oriented synthesis of its analogues. Chemistry ; Cycloaddition ; Natural product ; Trifluoromethanesulfonate ; Benzofuran ; Yield (engineering) ; Combinatorial chemistry ; Total synthesis ; Diterpene ; Diene ; Scandium ; Ring (chemistry) ; Stereochemistry ; Chemical space ; Organic chemistry ; Catalysis ; Drug discovery Synthesis of Indole Derivatives ; Marine Sponges and Natural Products ; Synthesis of Organic Compounds
Authors: JOSH KEMPPAINEN | IVAN GALLEGOS | AARON KRIEG | GREGORY ODEGARD
Source: American Society for Composites 2022 (article, 2022-09-19)
Field: Materials Science — Materials Chemistry

REACTIVE MOLECULAR DYNAMICS MECHANICAL PROPERTIES PREDICTION OF FURAN RESIN During the reentry of aerospace vehicles into the earth’s atmosphere, the outer shell surface temperature can reach up to 2700°C, which would melt or degrade most materials. The high temperatures that aerospace vehicles face during reentry mean that these vehicles need a thermal protection system (TPS) to shield the rest of the structure and occupants. There are many categories of thermal protection systems and many materials have been used over the years, but the most notable are carbon-carbon composites (CCC). CCCs are usually manufactured by curing a polymer in a fiber preform and then heat-treating the composite until all non-carbon atoms are burnt out. Due to the complexity, it is desired to model the polymerization and carbonization process to fine-tune composite materials. The first step in modeling a CCC involves the polymerization of precursor material, and an atomistic model is to model the polymerization. Therefore, reactive molecular dynamics (MD) has been used to model the polymerization of precursor material. The precursor material selected for benchmarking and validation is furan resin (polyfurfuryl alcohol – PFA). Furan resin has been of interest for CCC ablatives since the 1950s due to its ability to achieve relatively high carbon yields, which reduces the number of carbonization cycles. Furan resin has also found uses in adhesives, corrosion protection, fuel propellants, and foundry molds. In this paper, you will find experimental curing of furan resin and an MD modeling approach for polymerization of furan resin. Materials science ; Carbonization ; Furan ; Polymerization ; Thermosetting polymer ; Curing (chemistry) ; Composite material ; Polymer ; Composite number ; Adhesive ; Chemistry ; Organic chemistry Silicone and Siloxane Chemistry ; Fiber-reinforced polymer composites ; Epoxy Resin Curing Processes
Authors: Rufan Zhou | Mohanned Mohamedali | Yuxuan Ren | Qingye Lu | Nader Mahinpey
Source: SSRN Electronic Journal (article, 2022-01-01)
Field: Materials Science — Materials Chemistry

La-Ce Binary Oxide Catalysts for Low-Temperature Dry Reforming Catalysis ; Carbon dioxide reforming ; Cerium oxide ; Oxide ; Materials science ; Chemical engineering ; Metallurgy ; Chemistry ; Syngas ; Engineering ; Organic chemistry Catalytic Processes in Materials Science
Authors: Joaquin Barroso
Source: Front Matter (preprint, 2022-06-01)
Field: Chemistry — Physical and Theoretical Chemistry

Au(I) Chemistry No.3 – New paper in Dalton Transactions Stabilizing Gold in low oxidation states is a longstanding challenge of organometallic chemistry. To do so, a fine tuning of the electron density provided to an Au atom by a ligand via the formation of a &lt;em&gt; σ &lt;/em&gt; bond. The group of Professor Rong Shang at the University of Nagasaki has accomplished the stabilization of an aurate complex through the use of a boron, nitrogen-containing heterocyclic carbene; Chemistry ; Computer science History and advancements in chemistry
Authors: Joaquı́n Barroso-Flores
Source: Front Matter (article, 2022-06-01)
Field: Chemistry — Organic Chemistry

Au(I) Chemistry No.3 – New paper in Dalton Transactions Stabilizing Gold in low oxidation states is a longstanding challenge of organometallic chemistry. To do so, a fine tuning of the electron density provided to an Au atom by a ligand via the formation of a &lt;em&gt; σ &lt;/em&gt; bond. The group of Professor Rong Shang at the University of Nagasaki has accomplished the stabilization of an aurate complex through the use of a boron, nitrogen-containing heterocyclic carbene; Atom (system on chip) ; Ligand (biochemistry) ; Group 2 organometallic chemistry ; Group (periodic table) ; Organometallic chemistry Organometallic Complex Synthesis and Catalysis ; Inorganic and Organometallic Chemistry ; Catalytic Alkyne Reactions
Authors: Simone Di Noja | Marina Garrido | Lorenzo Gualandi | Giulio Ragazzon
Source: ChemRxiv (preprint, 2022-09-04)
Field: Materials Science — Materials Chemistry

Control on dissipative kinetics reveals the entropically-dominated essence of interlocked molecular machines The operation of nanomachines is fundamentally different from that of their macroscopic counterparts. In particular, the role of solvent is critical, yet rarely associated with machine functionality. Here we study a minimal model of one of the most advanced molecular machines, to gain control on its operation by engineering components and the employed solvent. Operation kinetics was modulated over more than four orders of magnitude, and could be fine-tuned. Leveraging solvent properties, it was possible to realize multiple cycles of the molecular machine operation while monitoring it. Our work expands the capabilities of acid-base powered molecular machines, contributing to the development of systems that leverage solvent properties to expand their functionality. Dissipative system ; Leverage (statistics) ; Solvent ; Kinetics ; Molecular machine ; Computer science ; Base (topology) ; Work (physics) ; Nanotechnology ; Materials science ; Biological system ; Chemistry ; Thermodynamics ; Physics ; Artificial intelligence ; Organic chemistry ; Mathematics Machine Learning in Materials Science ; Photoreceptor and optogenetics research ; Advanced Memory and Neural Computing
Authors: Pylkkänen, R. | Mohammadi, P. | Liljeström, V. | Plazinski, W. | Beaune, G. | Timonen, J. V. I. | Penttilä, M.
Source: HZB Repository (Helmholtz-Zentrum Berlin für Materialien und Energie GmbH (HZB)) (article, 2022-01-01)
Field: Materials Science — Biomaterials

beta 1,3 Glucan synthesis, novel supramolecular self assembly, characterization and application amp; 946; 1,3 Glucans are ubiquitously observed in various biological systems with diverse physio ecological functions, yet their underlying assembly mechanism and multiscale complexation in vitro remains poorly understood. Here, we provide for the first time evidence of unidentified amp; 946; 1,3 glucan supramolecular complexation into intricate hierarchical architectures over several length scales. We mediated these unique assemblies using a recombinantly produced amp; 946; 1,3 glucan phosphorylase Ta1,3BGP by fine tuning solution conditions during particle nucleation and growth. We report a synthesis of interconnected parallel hexagonal lamellae composed of 8 nm thick sheets of highly expanded paracrystals. The architecture consists of amp; 946; 1,3 glucan triple helices with considerable inter intra hydrogen bonding within, as well as in between adjacent triple helices. The results extend our understanding of amp; 946; 1,3 glucan molecular organization and shed light on different aspects of the crystallization processes of biomolecules into structures unseen by nature. The presented versatile synthesis yields new materials for diverse medical and industrial applications Supramolecular chemistry ; Glucan ; Crystallization ; Biomolecule ; Characterization (materials science) ; Nucleation ; Supramolecular assembly ; Self-assembly Supramolecular Self-Assembly in Materials ; Enzyme Production and Characterization ; Polysaccharides and Plant Cell Walls