jablonkagroup/rise_ai_scientists huggingface dataset:
Authors: Georgios Giannakakis | Marc‐Eduard Usteri | Aram L. Bugaev | Andrea Ruiz‐Ferrando | Dario Faust Akl | Núria López | Serena Fantasia | Kurt Püntener | Javier Pérez‐Ramírez | Sharon Mitchell
Source: ACS Catalysis (article, 2024-12-17)
Field: Chemistry — Organic Chemistry

Reactivity and Mechanism of Recoverable Pd<sub>1</sub>@C<sub>3</sub>N<sub>4</sub> Single-Atom Catalyst in Buchwald–Hartwig Aminations Buchwald-Hartwig (BH) aminations are crucial for synthesizing arylamine motifs in numerous bioactive molecules and fine chemicals. While homogeneous palladium complexes can be effective catalysts, their high costs and environmental impact motivate the search for alternative approaches. Heterogeneous palladium single-atom catalysts (SAC) offer promising recoverable alternatives in C-C cross-couplings. Yet their use in C-N couplings remains unexplored, and mechanistic insights into amine coupling with aryl halides over solid surfaces that could guide catalyst design are lacking. Here, we demonstrate that palladium atoms coordinated to well-defined heptazinic cavities of graphitic carbon nitride (Pd<sub>1</sub>@C<sub>3</sub>N<sub>4</sub>) deliver practically relevant yields for BH couplings across various aryl halides and amines, exhibiting persistent activity and negligible leaching over several cycles. Notably, Pd<sub>1</sub>@C<sub>3</sub>N<sub>4</sub> shows comparable or superior activity with certain aryl chlorides to bromides, alongside high chemoselectivity for amines over amides. In situ X-ray absorption spectroscopy analyses supported by density functional theory simulations identify the concerted role of the ligand and the C<sub>3</sub>N<sub>4</sub> host in determining the performance, with a Pd(II) nominal oxidation state observed under all coupling conditions. Complementary structural and kinetic studies highlight a distinct reaction mechanism than that typically reported for homogeneous catalysts. These findings offer key insights for designing recyclable SAC for BH coupling, setting the basis for extending the scope toward more complex industrial targets. Aryl ; Chemoselectivity ; Catalysis ; Palladium ; Chemistry ; Halide ; Combinatorial chemistry ; Density functional theory ; Heterogeneous catalysis ; Reactivity (psychology) ; Homogeneous catalysis ; Computational chemistry ; Photochemistry ; Organic chemistry Catalytic Cross-Coupling Reactions ; Nanomaterials for catalytic reactions ; Catalytic C–H Functionalization Methods
Authors: Zilin Wang | Hong Du | Austin M. Evans | Xiaojuan Ni | Jean‐Luc Brédas | Haoyuan Li
Source: Chemical Science (article, 2024-01-01)
Field: Materials Science — Materials Chemistry

Growth of two-dimensional covalent organic frameworks on substrates: insight from microsecond atomistic simulations While growing two-dimensional covalent organic frameworks (2D COFs) on substrates holds promise for producing functional monolayers, the presence of many defects in the resulting crystals often hinders their practical applications. Achieving structural order while suppressing defect formation necessitates a detailed atomic-level understanding. The key lies in understanding the polymerization process with high nano-scale accuracy, which presents significant challenges. Here, we perform microsecond atomistic molecular dynamics simulations to describe the deposition and polymerization of cyclohexa-<i>m</i>-phenylene on metal substrates, closely mimicking experimental conditions. Our improved approach highlights that 2D polymerization occurs through monomer addition and island coalescence, with a pre-bonding stage allowing monomers/oligomers to dynamically adjust their configurations to the expanding island structures. Our results elucidate the mechanisms underlying the formation of vacancy and dislocation defects during 2D polymerization as well as their healing processes. Overall, our findings underscore the significant roles that high surface mobility, effective monomer-substrate anchoring, high framework rigidity, moderate monomer coordination, and low bonding rate play in forming large, extended 2D crystals while suppressing vacancy and dislocation defects. We demonstrate how these factors can be tuned through substrate selection, deposition rate modulation, and temperature control, thereby offering valuable insight for strategically optimizing on-surface 2D polymerizations. Microsecond ; Covalent bond ; Molecular dynamics ; Nanotechnology ; Chemical physics ; Materials science ; Chemistry ; Computational chemistry ; Physics ; Organic chemistry Covalent Organic Framework Applications ; Surface Chemistry and Catalysis ; Block Copolymer Self-Assembly
Authors: Roel Michiels | Nick Gerrits | Erik C. Neyts | Annemie Bogaerts
Source: The Journal of Physical Chemistry C (article, 2024-07-01)
Field: Materials Science — Materials Chemistry

Plasma Catalysis Modeling: How Ideal Is Atomic Hydrogen for Eley–Rideal? Plasma catalysis is an emerging technology, but a lot of questions about the underlying surface mechanisms remain unanswered. One of these questions is how important Eley-Rideal (ER) reactions are, next to Langmuir-Hinshelwood reactions. Most plasma catalysis kinetic models predict ER reactions to be important and sometimes even vital for the surface chemistry. In this work, we take a critical look at how ER reactions involving H radicals are incorporated in kinetic models describing CO<sub>2</sub> hydrogenation and NH<sub>3</sub> synthesis. To this end, we construct potential energy surface (PES) intersections, similar to elbow plots constructed for dissociative chemisorption. The results of the PES intersections are in agreement with <i>ab initio</i> molecular dynamics (AIMD) findings in literature while being computationally much cheaper. We find that, for the reactions studied here, adsorption is more probable than a reaction via the hot atom (HA) mechanism, which in turn is more probable than a reaction via the ER mechanism. We also conclude that kinetic models of plasma-catalytic systems tend to overestimate the importance of ER reactions. Furthermore, as opposed to what is often assumed in kinetic models, the choice of catalyst will influence the ER reaction probability. Overall, the description of ER reactions is too much "ideal" in models. Based on our findings, we make a number of recommendations on how to incorporate ER reactions in kinetic models to avoid overestimation of their importance. Reactions on surfaces ; Catalysis ; Chemistry ; Radical ; Plasma ; Work (physics) ; Hydrogen ; Computational chemistry ; Thermodynamics ; Organic chemistry ; Physics Catalytic Processes in Materials Science ; Advanced Chemical Physics Studies ; Plasma Applications and Diagnostics
Authors: Katsuhiko Ariga
Source: Responsive materials (article, 2024-05-01)
Field: Materials Science — Materials Chemistry

Responsive materials nanoarchitectonics at interfaces Abstract Advanced materials could perform functions in response to external stimuli. These are responsive materials. In order for us to develop advanced functional systems with a good responsive nature, we need to create a methodology that goes one step further. It is the artificial architecture of functional material systems based on the knowledge of nanotechnology. The task will be fulfilled by the new concept of nanoarchitectonics. Nanoarchitectonics integrates nanotechnology with various material sciences, basic chemistry, microfabrication techniques, and biological processes to architect functional material systems from atomic, molecular, and nanomaterial units. This review will deal with the nanoarchitectonics of responsive materials related with phenomena at interfaces. In order to demonstrate the effectiveness of responsive materials nanoarchitectonics at interfaces for functional systems of various sizes, this review article is organized by size for various functional systems. Specifically, this review has grouped them into (i) molecular level response, (ii) nanodevice level response, (iii) material level response, and (iv) living cell level response. If the social demand for these materials is fully recognized, such development is expected to efficiently progress. This review article would play a role in stimulating such development. Nanotechnology ; Materials science Machine Learning in Materials Science ; Force Microscopy Techniques and Applications ; Nanopore and Nanochannel Transport Studies
Authors: Yuying Zhao | Jincan Zhang | Fengxian Ma | Hongbo Wu | Weizhen Meng | Ying Liu | Yalong Jiao | Aijun Du
Source: Microstructures (article, 2024-05-28)
Field: Materials Science — Materials Chemistry

Computational exploration of two-dimensional vacancy-free boridene sheet and its derivatives: high stabilities and the promise for hydrogen evolution reaction The recent synthesis of a two-dimensional (2D) MBene sheet, referred to as the boridene sheet (Mo4B6Tz), has ignited considerable interest in exploring 2D transition metal borides. Boridene has an ordered arrangement of metal vacancies, which are pivotal to its stability. Employing first-principles calculations, we explored the stable phases, electronic properties and catalytic abilities of boridene with different vacancy concentrations (Vm). Our results demonstrate that Vm significantly influences the cohesive energies of boridene sheets. Phonon spectrum and ab initio molecular dynamics simulations reveal the high stability of the vacancy-free boridene Mo6B6T6 (T = O, -OH), underscoring their potential for experimental realization. Substituting Mo atoms with Nb, Ta, or W enhances the structural stability of boridene sheets, leading to the identification of four stable variants: Nb6B6F6, Ta6B6F6, Ta6B6O6, and W6B6O6. These boridene sheets exhibit metallic behavior, with five structures displaying near-zero Gibbs free energy for hydrogen atom adsorption, indicating their potential as catalysts for the hydrogen evolution reaction. The uncovering of vacancy-free boridenes and their 2D derivatives greatly broadens the scope of the MBene family. Vacancy defect ; Hydrogen ; Materials science ; Computational chemistry ; Chemistry ; Crystallography ; Organic chemistry MXene and MAX Phase Materials ; Boron and Carbon Nanomaterials Research ; Inorganic Chemistry and Materials
Authors: Samadhan Kapse | Maria Voccia | Francesc Viñes | Francesc Illas
Source: Journal of Molecular Modeling (article, 2024-05-07)
Field: Materials Science — Materials Chemistry

Chemical bonding and electronic properties along Group 13 metal oxides Periodic density functional theory was used to predict the atomic structure of the materials of interest. Structure optimization was carried out using the PBE functional, using a plane wave basis set and the PAW representation of the atomic cores, using the VASP code. Next, the electronic properties were computed by carrying out single point calculations employing PBE, PBE + U functionals using VASP and also with PBE and the hybrid HSE06 functionals using the FHI-AIMS software. For the hybrid HSE06, the impact of the screening parameter, ω, and mixing parameter, α, on the calculated band gap has also been assessed. Density functional theory ; Hybrid functional ; Band gap ; Electronic structure ; Oxide ; Context (archaeology) ; Materials science ; Electronic band ; Electronic band structure ; Crystal structure ; Metal ; Computational chemistry ; Chemistry ; Crystallography ; Physics ; Condensed matter physics ; Optoelectronics Machine Learning in Materials Science ; Ga2O3 and related materials ; Inorganic Chemistry and Materials
Authors: H.-Q. Jin | Kenneth M. Merz
Source: Journal of Chemical Theory and Computation (article, 2024-09-09)
Field: Chemistry — Organic Chemistry

Partial to Total Generation of 3D Transition-Metal Complexes The design of transition-metal complexes (TMCs) has drawn much attention over the years because of their important applications as metallodrugs and functional materials. In this work, we present an extension of our recently reported approach, LigandDiff [Jin et al. <i>J. Chem. Theory Comput.</i> <b>20</b>, 4377(2024)]. The new model, which we call multi-LigandDiff, is more flexible and greatly outperforms its predecessor. This scaffold-based diffusion model allows de novo ligand design with either existing ligands or without any ligand. Moreover, it allows users to predefine the denticity of the generated ligand. Our results indicate that multi-LigandDiff can generate well-defined ligands and is transferable to multiple transition metals and coordination geometries. In terms of its application, multi-LigandDiff successfully designed 338 Fe(II) spin-crossover (SCO) complexes from only 47 experimentally validated SCO complexes. And these generated complexes are configurationally diverse and structurally reasonable. Overall, the results show that multi-LigandDiff is an ideal tool to design novel TMCs from scratch. Transition metal ; Nanotechnology ; Transition (genetics) ; Extension (predicate logic) ; Computer science ; Chemistry ; Materials science ; Organic chemistry ; Catalysis Organometallic Complex Synthesis and Catalysis ; Asymmetric Hydrogenation and Catalysis ; Molecular Junctions and Nanostructures
Authors: Wenjie Li | Zhendong Hao | Shihai Cao | Silin Chen | Xue Wang | Huimin Yin | Xuewei Tao | Yuming Dai | Cong Yuan | Jia Ju
Source: Small (review, 2024-08-13)
Field: Materials Science — Materials Chemistry

Unraveling the Mechanism of Covalent Organic Frameworks‐Based Functional Separators in High‐Energy Batteries Covalent organic frameworks (COFs) are promising porous materials due to their high specific surface area, adjustable structure, highly ordered nanochannels, and abundant functional groups, which brings about wide applications in the field of gas adsorption, hydrogen storage, optics, and so forth. In recent years, COFs have attracted considerable attention in electrochemical energy storage and conversion. Specifically, COF-based functional separators are ideal candidates for addressing the ionic transport-related issues in high-energy batteries, such as dendritic formation and shuttle effect. Therefore, it is necessary to make a comprehensive understanding of the mechanism of COFs in functional separators. In this review, the advantages, applications as well as synthesis of COFs are firstly presented. Then, the mechanism of COFs in functional separators for high-energy batteries is summarized in detail, including pore channels regulating ionic transport, functional groups regulating ionic transport, adsorption effect, and catalytic effect. Finally, the application prospect of COFs-based separators in high-energy batteries is proposed. This review may provide new insights into the design of functional separators for advanced electrochemical energy storage and conversion systems. Mechanism (biology) ; Covalent bond ; Materials science ; Nanotechnology ; Chemical engineering ; Chemistry ; Organic chemistry ; Engineering ; Physics Covalent Organic Framework Applications ; Advancements in Battery Materials ; Advanced Battery Materials and Technologies
Authors: Colette Abimana | Abdulhakeem Bello | Revocatus L. Machunda | Yusufu Abeid Chande Jande
Source: Journal of Renewable Energy (review, 2024-01-01)
Field: Materials Science — Electronic, Optical and Magnetic Materials

Understanding the Factors Influencing the Properties of Biomass‐Derived Porous Carbon and Their Impacts on Electrical Double‐Layer Capacitor Electrodes: A Comprehensive Review The use of biomass as carbon precursors has been extensively investigated, with a particular emphasis on examining the properties of derived porous carbon and its application in electrical double‐layer capacitors (EDLCs). Biomass‐derived porous carbon‐based electrodes have shown promising properties that can improve the efficiency of EDLCs. However, despite the extensive research in this field, no definitive solution has been proposed. This review investigates in depth three main factors that impact the electrochemical performance of derived porous carbon‐based electrodes: (1) the initial properties of raw biomass as carbon precursors, (2) operating conditions, and (3) physicochemical properties of biomass‐derived porous carbon materials. Examined operating conditions include synthesis techniques, activating agents, the mass ratio of the activating agent to the raw biomass as porous carbon precursors, carbonization/activation duration, operating temperature, and the mass of the active material in the electrode. The surface morphology and surface functional groups were used to evaluate the physicochemical properties of derived porous carbon materials. Multiple factors influence the properties of porous carbon derived from biomass and, consequently, the efficiency of the electrodes made from these materials. This study reveals that the properties of porous carbon‐based electrodes derived from biomass vary from one biomass to another and are affected by various parameters, conditions, and synthesis techniques. Therefore, it is impossible to rely exclusively on a single factor to improve the electrochemical performance of EDLC electrodes. A thorough consideration of the multiple factors is required to optimize the properties and performance of the electrodes. Capacitor ; Materials science ; Porosity ; Electrode ; Carbon fibers ; Biomass (ecology) ; Layer (electronics) ; Supercapacitor ; Chemical engineering ; Nanotechnology ; Engineering physics ; Composite material ; Environmental science ; Electrical engineering ; Engineering ; Chemistry ; Electrochemistry ; Geology ; Oceanography ; Voltage ; Composite number Supercapacitor Materials and Fabrication ; Conducting polymers and applications ; Advancements in Battery Materials
Authors: Long‐Qing Chen | Nele Moelans
Source: MRS Bulletin (article, 2024-06-01)
Field: Materials Science — Materials Chemistry

Phase-field method of materials microstructures and properties Field (mathematics) ; Phase (matter) ; Characterization (materials science) ; Microstructure ; Computer science ; Mesoscale meteorology ; Focus (optics) ; Nanotechnology ; Phase field models ; Materials science ; Systems engineering ; Biochemical engineering ; Engineering ; Physics Solidification and crystal growth phenomena ; Aluminum Alloy Microstructure Properties ; nanoparticles nucleation surface interactions
Authors: Kelly L. Vernon | Tipsiri Pungsrisai | Oluwasegun J. Wahab | Sasha E. Alden | Yaxu Zhong | Myung-Hoon Choi | Ekta Verma | Anne K. Bentley | Kathleen O. Bailey | Sara E. Skrabalak | Xingchen Ye | Katherine A. Willets | Lane A. Baker
Source: ACS electrochemistry. (article, 2024-10-08)
Field: Chemistry — Electrochemistry

Optically Transparent Carbon Electrodes for Single Entity Electrochemistry We demonstrate the application and benefit of optically transparent carbon electrodes (OTCEs) for single entity nanoelectrochemistry. OTCEs are prepared by pyrolyzing thin photoresist films on fused quartz coverslips to create conductive, transparent, thin films. Optical, electrical, topographical, and electrochemical properties of OTCEs are characterized to evaluate their suitability for single entity electrochemistry. Nanoscale electrochemical imaging of the OTCEs using scanning electrochemical cell microscopy (SECCM) revealed uniform electrochemical activity for reduction of the hexaammineruthenium(III) redox complex, that was comparable to Au-coated glass, and in contrast to the heterogeneity observed with commonly used indium tin oxide (ITO) substrates. Additionally, we demonstrate the utility of the prepared OTCEs for correlative SECCM-scanning electron microscopy studies of the hydrogen evolution reaction at the surface of Au nanocubes. Lastly, we demonstrate the benefit of OTCEs for optoelectrochemical experiments by optically monitoring the electrodissolution of Au nanocrystals. These results establish OTCE as a viable transparent support electrode for multimode electrochemical and optical microscopy of nanocrystals and other entities. Materials science ; Electrochemistry ; Indium tin oxide ; Electrode ; Scanning electrochemical microscopy ; Scanning electron microscope ; Nanotechnology ; Electrochemical cell ; Nanocrystal ; Glassy carbon ; Optical microscope ; Thin film ; Chemical engineering ; Chemistry ; Cyclic voltammetry ; Composite material Electrochemical Analysis and Applications ; Electrochemical sensors and biosensors ; Electrocatalysts for Energy Conversion
Authors: Ana Cuevas | Antonia A. Dominguez | Javier Zamudio‐García | V. Vega | Ana Silvia González | David Marrero‐López | V.M. Prida | J. Benavente
Source: Materials (article, 2024-03-20)
Field: Materials Science — Materials Chemistry

Optical and Electrochemical Properties of a Nanostructured ZnO Thin Layer Deposited on a Nanoporous Alumina Structure via Atomic Layer Deposition This study explores the optical and electrochemical properties of a ZnO coating layer deposited on a nanoporous alumina structure (NPAS) for potential multifunctional applications. The NPAS, synthesized through an electrochemical anodization process, displays well-defined nanochannels with a high aspect ratio (~3000). The ZnO coating, achieved via atomic layer deposition, enables the tuning of the pore diameter and porosity of the NPAS, thereby influencing both the optical and electrochemical interfacial properties. A comprehensive characterization using photoluminescence, spectroscopy ellipsometry and impedance spectroscopy (with the sample in contact with NaCl solutions) provides insights into optical and electrochemical parameters, including the refractive index, absorption coefficient, and electrolyte-ZnO/NPAS interface processes. This research demonstrates potential for tailoring the optical and interfacial properties of nanoporous structures by selecting appropriate coating materials, thus opening avenues for their utilization in various technological applications. Nanoporous ; Materials science ; Atomic layer deposition ; Dielectric spectroscopy ; Coating ; Layer (electronics) ; Anodizing ; Chemical engineering ; Electrochemistry ; Electrolyte ; Ellipsometry ; Thin film ; Photoluminescence ; Nanotechnology ; Porosity ; Deposition (geology) ; Composite material ; Aluminium ; Optoelectronics ; Electrode ; Chemistry Anodic Oxide Films and Nanostructures ; Semiconductor materials and devices ; Ga2O3 and related materials