jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Gourab Bhaskar | Ranjan Kumar Behera | Volodymyr Gvozdetskyi | Scott L. Carnahan | Raquel A. Ribeiro | Paul Oftedahl | C.H. Ward | P. C. Canfield | Aaron J. Rossini | Wenyu Huang | Julia V. Zaikina
Source: Journal of the American Chemical Society (article, 2023-12-07)
Field: Materials Science — Materials Chemistry

Breaking New Ground: <i>MB</i>ene Route toward Selective Vinyl Double Bond Hydrogenation in Nitroarenes Doping, or incremental substitution of one element for another, is an effective way to tailor a compound's structure as well as its physical and chemical properties. Herein, we replaced up to 30% of Ni with Co in members of the family of layered LiNiB compounds, stabilizing the high-temperature polymorph of LiNiB while the room-temperature polymorph does not form. By studying this layered boride with in situ high-temperature powder diffraction, we obtained a distorted variant of LiNi<sub>0.7</sub>Co<sub>0.3</sub>B featuring a perfect interlayer placement of [Ni<sub>0.7</sub>Co<sub>0.3</sub>B] layers on top of each other─a structural motif not seen before in other borides. Because of the Co doping, LiNi<sub>0.7</sub>Co<sub>0.3</sub>B can undergo a nearly complete topochemical Li deintercalation under ambient conditions, resulting in a metastable boride with the formula Li<sub>0.04</sub>Ni<sub>0.7</sub>Co<sub>0.3</sub>B. Heating of Li<sub>0.04</sub>Ni<sub>0.7</sub>Co<sub>0.3</sub>B in anaerobic conditions led to yet another metastable boride, Li<sub>0.01</sub>Ni<sub>0.7</sub>Co<sub>0.3</sub>B, with a CoB-type crystal structure that cannot be obtained by simple annealing of Ni, Co, and B. No significant alterations of magnetic properties were detected upon Co-doping in the temperature-independent paramagnet LiNi<sub>0.7</sub>Co<sub>0.3</sub>B or its Li-deintercalated counterparts. Finally, Li<sub>0.01</sub>Ni<sub>0.7</sub>Co<sub>0.3</sub>B stands out as an exceptional catalyst for the selective hydrogenation of the vinyl C═C bond in 3-nitrostyrene, even in the presence of other competing functional groups. This research showcases an innovative approach to heterogeneous catalyst design by meticulously synthesizing metastable compounds. Boride ; Chemistry ; Metastability ; Doping ; Annealing (glass) ; Crystal structure ; Catalysis ; Crystallography ; Chemical engineering ; Inorganic chemistry ; Organic chemistry ; Composite material ; Materials science MXene and MAX Phase Materials ; Nanomaterials for catalytic reactions ; Hydrogen Storage and Materials
Authors: Jonas Wolf | Kevinjeorjios Pellumbi | Sarankumar Haridas | Tobias Kull | Julian T. Kleinhaus | Leon Wickert | Ulf‐Peter Apfel | Daniel Siegmund
Source: Chemistry - A European Journal (article, 2023-12-15)
Field: Chemistry — Organic Chemistry

Electroplated Electrodes for Continuous and Mass‐Efficient Electrochemical Hydrogenation Electrocatalytic hydrogenations (ECH) enable the reduction of organic substrates upon usage of electric current and present a sustainable alternative to conventional processes if green electricity is used. Opposed to most current protocols for electrode preparation, this work presents a one-step binder- and additive-free production of silver- and copper-electroplated electrodes. Controlled adjustment of the preparation parameters allows for the tuning of catalyst morphology and its electrochemical properties. Upon optimization of the deposition protocol and carbon support, high faradaic efficiencies of 93 % for the ECH of the Vitamin A- and E-synthon 2-methyl-3-butyn-2-ol (MBY) are achieved that can be maintained at current densities of 240 mA cm<sup>-2</sup> and minimal catalyst loadings of 0.2 mg cm<sup>-2</sup>, corresponding to an unmatched production rate of 1.47 kg<sub>MBE</sub> g<sub>cat</sub> <sup>-1</sup> h<sup>-1</sup>. For a continuous hydrogenation process, the protocol can be directly transferred into a single-pass operation mode giving a production rate of 1.38 kg<sub>MBE</sub> g<sub>cat</sub> <sup>-1</sup> h<sup>-1</sup>. Subsequently, the substrate spectrum was extended to a total of 17 different C-C-, C-O- and N-O-unsaturated compounds revealing the general applicability of the reported process. Our results lay an important groundwork for the development of electrochemical reactors and electrodes able to directly compete with the palladium-based thermocatalytic state of the art. Electroplating ; Electrochemistry ; Electrode ; Materials science ; Nanotechnology ; Chemical engineering ; Chemistry ; Engineering ; Physical chemistry Nanomaterials for catalytic reactions ; Electrocatalysts for Energy Conversion ; Catalysis for Biomass Conversion
Authors: Carmine Capacchione | Fabia Grisi | Marina Lamberti | Mina Mazzeo | Bárbara Milani | Stefano Milione | Daniela Pappalardo | Cristiano Zuccaccia | Claudio Pellecchia
Source: European Journal of Inorganic Chemistry (article, 2023-01-24)
Field: Materials Science — Biomaterials

Metal Catalyzed Polymerization: From Stereoregular Poly(α‐olefins) to Tailor‐Made Biodegradable/Biorenewable Polymers and Copolymers Abstract Metal catalyzed polymerizations are among the most important chemical reactions, accounting for the production of about 400 million tons per year of polymeric materials, 50 % of which are polyolefins. The CIRCC research units at the University of Salerno, founded by the late Professor Adolfo Zambelli, a coworker of Giulio Natta and a pioneer in the studies of stereospecific polymerization catalysts, has a consolidated expertise in this field. Although often considered a “mature” area of research, olefin polymerization catalysis continues to drive great interest of both industrial and academic scientists. On the other hand, strong political and economic pressure toward the development of “green” and possibly biodegradable alternatives to olefin‐based polymers stimulated our group to direct increasing research efforts in the area of sustainable polymers. In this perspective, we focus on the most recent work from the CIRCC research units involved in homogeneous catalysis for polymerization of a variety of monomers, with the aim to address how the concepts and the expertise developed for olefin polymerization can be applied to the development of different metal‐catalyzed polymerizations and copolymerizations. Of course, although the results are discussed in the frame of the most important literature contributions, a comprehensive review of such a wide and diversified topic is out of the scope of the paper. References to reviews covering the different types of metal catalyzed polymerizations are provided in each chapter. Polymerization ; Chemistry ; Catalysis ; Olefin polymerization ; Polymer ; Polymer science ; Olefin fiber ; Monomer ; Copolymer ; Organic chemistry ; Polymer chemistry biodegradable polymer synthesis and properties ; Carbon dioxide utilization in catalysis ; Organometallic Complex Synthesis and Catalysis
Authors: Iqra Shafiq | Adnan Mustafa | Romaisa Zahid | Rabia Baby | Sarfraz Ahmed | Muhammad Adnan Asghar | Tansir Ahamad | Manawwer Alam | Ataualpa Albert Carmo Braga | Suvash Chandra Ojha
Source: ACS Omega (article, 2023-10-12)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Theoretical Perspective toward Designing of 5-Methylbenzo [1,2-<i>b</i>:3,4-<i>b</i>′:6,5-<i>b</i>″] trithiophene-Based Nonlinear Optical Compounds with Extended Acceptors A series of benzotrithiophene-based compounds (<b>DCTM1</b>-<b>DCTM6</b>) having D<sub>1</sub>-π<sub>1</sub>-D<sub>2</sub>-π<sub>2</sub>-A configuration were designed using a reference molecule (<b>DCTMR</b>) via incorporating pyrrole rings (<i>n</i> = 1-5) as the π-spacer (π<sub>2</sub>). Quantum chemical calculations were performed to determine the impact of the pyrrole ring on the nonlinear optical (NLO) behavior of the above-mentioned chromophores. The optoelectronic properties of the compounds were determined at the MW1PW91/6-311G(d,p) functional. Among all of the derivatives, <b>DCTM5</b> exhibited the least highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) band gap (<i>E</i><sub>g</sub>) 0.968 eV with a high softness of 0.562 eV<sup>-1</sup>, and hence possessed the highest polarizability. Interestingly, transition density matrix (TDM) findings demonstrated that <b>DCTM5</b> with an effective diagonal charge transmission proportion at the acceptor group supports the frontier molecular orbital (FMO) results. Additionally, the exciton binding energy values for <b>DCTM1</b>-<b>DCTM6</b> were found to be less than that for <b>DCTMR</b> and thus, the effective charge transfer was examined in the derivatives. All of the derivatives exhibited effective NLO outcomes with the highest magnitude of linear polarizability ⟨α⟩, and first (β<sub>tot</sub>) and second (γ<sub>tot</sub>) hyperpolarizabilities relative to the parent compound. Nevertheless, the highest β<sub>tot</sub> and γ<sub>tot</sub> were obtained for <b>DTCM1</b> and <b>DTCM6</b>, 7.0440 × 10<sup>-27</sup> and 22.260 × 10<sup>-34</sup> esu, respectively. Hence, through this structural tailoring with a pyrrole spacer, effective NLO materials can be obtained for optoelectronic applications. Polarizability ; HOMO/LUMO ; Molecular orbital ; Chemistry ; Chromophore ; Exciton ; Acceptor ; Molecule ; Computational chemistry ; Band gap ; Pyrrole ; Crystallography ; Photochemistry ; Materials science ; Physics ; Optoelectronics ; Organic chemistry ; Quantum mechanics Nonlinear Optical Materials Research ; Nonlinear Optical Materials Studies ; Organic Chemistry Cycloaddition Reactions
Authors: Jelena Pavlović | Nevenka Rajić
Source: Minerals (article, 2023-06-29)
Field: Materials Science — Materials Chemistry

Clinoptilolite—An Efficient Carrier for Catalytically Active Nano Oxide Particles Many efforts have been devoted to produce green materials and technology to prevent and minimize the adverse effects on the environment and human health caused primarily by population growth and industrial progress. Over the past years, the use of zeolites has attracted considerable attention as both an economically and environmentally friendly option. Zeolites are crystalline, hydrated aluminosilicates with an open-framework structure. Unique structural features make them very useful ion-changers, adsorbents and catalysts. The catalytic use of zeolites has expanded from traditional use in the petrochemical industry and refineries to use in the catalytic degradation of various environmental pollutants and the synthesis of fine chemicals. In recent times, progress on the use of zeolites has been achieved in biomass conversion to fuels and valuable industrial bio-based chemicals. This review highlights the recent advances in the catalytic application of clinoptilolite (CLI), the most abundant and explored natural zeolite. The main goal of the review is to give the current state of CLI applications and insights into CLI catalytic performance, which opens possibilities for a variety of applications. Clinoptilolite ; Petrochemical ; Environmentally friendly ; Catalysis ; Zeolite ; Nanotechnology ; Population ; Waste management ; Environmental science ; Materials science ; Chemistry ; Engineering ; Organic chemistry Mesoporous Materials and Catalysis ; Zeolite Catalysis and Synthesis ; Catalysis for Biomass Conversion
Authors: Silvia Muñoz-Sánchez | Irene Heredero‐Bermejo | F. Javier de la Mata | Sandra García‐Gallego
Source: Chemistry of Materials (article, 2023-12-26)
Field: Chemistry — Organic Chemistry

Bifunctional Carbosilane Dendrimers for the Design of Multipurpose Hydrogels with Antibacterial Action The emergence of antibiotic resistance is a serious global health problem. There is an incessant demand for new antimicrobial drugs and materials that can address this global issue from different angles. Dendritic hydrogels have appeared as a promising strategy. A family of bifunctional amphiphilic carbosilane dendrimers was designed and employed as nanosized cross-linking points for the synthesis of high-swelling hydrogels using the highly efficient Thiol-Ene <i>click</i> reaction for their preparation. Both stoichiometric and off-stoichiometric conditions were studied, generating hydrogels with pendant hydroxyl or alkene moieties. These hydrogels were found to be tunable antibacterial materials. They can easily be postmodified with relevant antibiotic moieties through covalent attachment on the hydroxyl or alkene pendant groups, generating ammonium-decorated networks with temperature and pH-responsive properties. Additionally, they can efficiently encapsulate drugs with poor solubility in water, like ciprofloxacin, and perform a sustained release over time, as demonstrated in preliminary assays against <i>Staphylococcus aureus</i>. Self-healing hydrogels ; Bifunctional ; Dendrimer ; Amphiphile ; Combinatorial chemistry ; Chemistry ; Alkene ; Click chemistry ; Polymer chemistry ; Materials science ; Polymer ; Organic chemistry ; Copolymer ; Catalysis Antimicrobial agents and applications ; Luminescence and Fluorescent Materials ; Dendrimers and Hyperbranched Polymers
Authors: Soumyashree Jena | Lars Frenzen | Vishal Chugh | Jiajun Wu | Thomas Weyhermüller | Alexander A. Auer | Christophe Werlé
Source: Journal of the American Chemical Society (article, 2023-12-12)
Field: Chemistry — Organic Chemistry

A Cooperative Cobalt-Driven System for One-Carbon Extension in the Synthesis of (<i>Z</i>)-Silyl Enol Ethers from Aldehydes: Unlocking Regio- and Stereoselectivity The research presented herein explores a cobalt-based catalytic system, distinctively featuring a cooperative boron-centric element within its intricate ligand architecture. This system is strategically engineered to enable the integration of a singular carbon atom into aldehydes, a process culminating in the production of (<i>Z</i>)-silyl enol ethers. Beyond offering an efficient one-pot synthesis route, this method adeptly overcomes challenges inherent to conventional techniques, such as the need for large amounts of additives, restrictive functional group tolerance, and extreme reaction temperatures. Initial mechanistic studies suggest the potential role of a cobalt-carbene complex as a catalytically significant species and underscore the importance of the borane segment. Collectively, these observations highlight the potential of this system in advancing complex bond activation pursuits. Chemistry ; Silylation ; Cobalt ; Enol ; Borane ; Stereoselectivity ; Carbene ; Catalysis ; Ligand (biochemistry) ; Organic synthesis ; Carbon fibers ; Combinatorial chemistry ; Organic chemistry ; Receptor Organoboron and organosilicon chemistry ; Catalytic C–H Functionalization Methods ; Catalytic Cross-Coupling Reactions
Authors: Mohammad Salavati
Source: Preprints.org (preprint, 2023-10-13)
Field: Materials Science — Polymers and Plastics

Mechanical Properties of α-Chitin and Chitosan Biocomposite: A Molecular Dynamic Study The mechanical properties of α-chitin and chitosan biocomposite are investigated due to their broad range of potential applications in bioengineering, materials science, and environmental technology. Employing molecular dynamics (MD), and stress-strain analyses, this study comprehensively investigates biopolymers mechanical response and anisotropic mechanical behavior under uniaxial tensile loading conditions in an aqueous environment. Our computational models were validated against existing experimental data, showing high degrees of correspondence. Uniaxial tensile tests revealed that α-chitin exhibits a remarkable ultimate tensile strength (UTS) of 10.07 GPa in the crystalline chain direction (y-axis) at a high strain rate of 0.636, compared to a significantly lower UTS of 2.78 GPa in the perpendicular direction (x-axis) at a lower strain rate of 0.066. The biocomposite nanostructure, encompassing randomly distributed chitosan, reduced stiffness, maintaining remarkable flexibility as α-chitin, with a UTS of 5.03 GPa in the y-axis and 2.34 GPa in the x-axis. Further, the directional elastic modules for α-chitin were calculated as 51.76 GPa and 39.76 GPa in the x and y directions, respectively. In contrast, these values for the α-chitin-chitosan biocomposite were estimated as 31.66 GPa and 26.00 GPa, respectively. The findings provide valuable insights into the distinct mechanical properties of α-chitin and chitosan biocomposite, making a substantial contribution to optimizing these materials for specialized applications. Biocomposite ; Ultimate tensile strength ; Chitin ; Chitosan ; Materials science ; Composite material ; Anisotropy ; Strain (injury) ; Chemical engineering ; Composite number ; Physics Natural Fiber Reinforced Composites ; Advanced Cellulose Research Studies ; Silk-based biomaterials and applications
Authors: Nasrin Attari | Robert Hausler
Source: International Journal of Environmental Pollution and Remediation (article, 2023-01-01)
Field: Materials Science — Biomaterials

Cradle-to-Gate Life Cycle Assessment of Cellulose-Based Membrane Manufacturing Process Polymer nanocomposite membrane is an innovative and promising approach with a broad spectrum of potential applications in filtration processes.In spite of this, membrane production procedures are far from environmentally friendly and sustainable.A comprehensive understanding of its environmental impacts, covering the life cycle of the used materials and the fabrication process, is crucial for its long-term sustainable success.This research aims to elaborate and implement a decision-making tool for greener membrane fabrication process.The environmental impacts of synthesizing one batch of Nanocomposite cellulose nanofibrils/cellulose acetate membrane using 50 gr polymer dope solution by electrospinning technique was determined based on a life cycle assessment methodology.The eco-sufficiency and sustainability of the electrospinning method were evaluated through a cradleto-gate life cycle assessment (LCA) adopting the Cumulative Energy Demand (CED), and IMPACT2002+ impact assessment methods.According to CED assessment, the majority of energy consumed during electrospun membrane synthesis, amounting to 382 MJ, was consumed by the production of cellulose nanofibers.This is related to non-renewable fossil energy consumed in Ethanol production.As per IMPACT2002+ impact assessment, cellulose acetate and cellulose nanofiber manufacturing, and medium voltage electricity are the main contributors to the overall midpoint environmental impacts.A number of hotspots in the membrane production process were identified, and measures were suggested for reducing the environmental impact of membrane production. Cellulose ; Process (computing) ; Life-cycle assessment ; Manufacturing process ; Process engineering ; Membrane ; Materials science ; Manufacturing engineering ; Computer science ; Chemistry ; Chemical engineering ; Engineering ; Composite material ; Biochemistry ; Programming language ; Economics ; Production (economics) biodegradable polymer synthesis and properties ; Recycling and Waste Management Techniques ; Advanced Cellulose Research Studies
Authors: Slavomíra Šterbinská | Mariia Holub | Erik Čižmár | Juraj Černák | Lawrence Rocco Falvello | Milagros Tomás
Source: Crystal Growth & Design (article, 2023-05-26)
Field: Materials Science — Electronic, Optical and Magnetic Materials

An Old Crystallization Technique as a Fast, Facile, and Adaptable Method for Obtaining Single Crystals of Unstable “Li<sub>2</sub>TCNQF<sub>4</sub>” and New Compounds of TCNQ or TCNQF<sub>4</sub>: Syntheses, Crystal Structures, and Magnetic Properties Detailed structural information is essential for understanding the properties of TCNQ and TCNQF<sub>4</sub> compounds (TCNQ = 7,7,8,8-tetracyanoquinodimethane; TCNQF<sub>4</sub> = 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane). The ineludible requirement of obtaining crystals of a size and quality sufficient to yield a successful X-ray diffraction analysis has been challenging to satisfy because of the instability of many of these compounds in solution. Crystals of two new complexes of TCNQ, [<i>trans</i>-M(2<i>ampy</i>)<sub>2</sub>(TCNQ)<sub>2</sub>] [M = Ni (<b>1</b>), Zn (<b>2</b>); 2ampy = 2-aminomethylpyridine], as well as unstable [Li<sub>2</sub>(TCNQF<sub>4</sub>)(CH<sub>3</sub>CN)<sub>4</sub>]·CH<sub>3</sub>CN (<b>3</b>), can be prepared in minutes by a horizontal diffusion technique and can be harvested easily for X-ray structural studies. Compound <b>3</b>, previously described as "Li<sub>2</sub>TCNQF<sub>4</sub>," forms a one-dimensional (1D) ribbon. Compounds <b>1</b> and <b>2</b> can also be obtained as microcrystalline solids from methanolic solutions of MCl<sub>2</sub>/LiTCNQ/2<i>ampy</i>. Their variable-temperature magnetic studies confirmed a contribution of strongly antiferromagnetically coupled pairs of TCNQ<sup>•-</sup> anion radicals at higher temperatures with exchange coupling <i>J</i>/<i>k</i><sub>B</sub> = -1206 K and <i>J</i>/<i>k</i><sub>B</sub> = -1369 K for <b>1</b> and <b>2</b>, respectively, estimated using a spin dimer model. The presence of magnetically active anisotropic Ni(II) atoms with <i>S</i> = 1 in <b>1</b> was confirmed, and the magnetic behavior of <b>1</b>, representing an infinite chain of alternating <i>S</i> = 1 sites and <i>S</i> = 1/2 dimers, was described by a spin-ring model suggesting ferromagnetic exchange coupling between Ni(II) sites and anion radicals. Tetracyanoquinodimethane ; Crystallography ; Chemistry ; Electron paramagnetic resonance ; Ferromagnetism ; Microcrystalline ; Dimer ; Yield (engineering) ; Crystallization ; Ion ; Materials science ; Condensed matter physics ; Molecule ; Nuclear magnetic resonance ; Organic chemistry ; Physics Organic and Molecular Conductors Research ; Magnetism in coordination complexes ; Advanced NMR Techniques and Applications
Authors: Benedek Stadler | Hilary Meng | Sara Belazregue | Leah Webster | Alberto Collauto | Keelan M. Byrne | Tobias Krämer | F. Mark Chadwick
Source: Organometallics (article, 2023-03-13)
Field: Chemistry — Organic Chemistry

PCP Pincer Complexes of Titanium in the +3 and +4 Oxidation States Ti(IV) and Ti(III) complexes using the <sup>tBu</sup>PCP ligand have been synthesized (<sup>tBu</sup>PCP = C<sub>6</sub>H<sub>3</sub>-2,6-(CH<sub>2</sub>P<sup>t</sup>Bu<sub>2</sub>)<sub>2</sub>). The [<sup>tBu</sup>PCP]Li synthon can be reacted with TiCl<sub>4</sub>(THF)<sub>2</sub> to form (<sup>tBu</sup>PCP)TiCl<sub>3</sub> (<b>1</b>) in limited yields due to significant reduction of the titanium synthon. The Ti(III) complex (<sup>tBu</sup>PCP)TiCl<sub>2</sub> (<b>2</b>) has been further characterized. This can have half an equivalent of halide abstracted to form [{(<sup>tBu</sup>PCP)TiCl}<sub>2</sub>{μ-Cl}][B(C<sub>6</sub>F<sub>5</sub>)<sub>4</sub>] (<b>3</b>) and can also be methylated, forming (<sup>tBu</sup>PCP)TiMe<sub>2</sub> (<b>4</b>). All the Ti(III) complexes have been characterized using EPR and X-ray crystallography, giving insight into their electronic structures, which are further supported by DFT calculations. Synthon ; Chemistry ; Pincer movement ; Electron paramagnetic resonance ; Titanium ; Ligand (biochemistry) ; Halide ; Crystallography ; Stereochemistry ; Medicinal chemistry ; Inorganic chemistry ; Catalysis ; Organic chemistry Organometallic Complex Synthesis and Catalysis ; Synthesis and characterization of novel inorganic/organometallic compounds ; Organoboron and organosilicon chemistry