A5040919062- Catalytic Processes in Materials Science
- Machine Learning in Materials Science
- Carbon dioxide utilization in catalysis
- Asymmetric Hydrogenation and Catalysis
- Hydrogen Storage and Materials
- CO2 Reduction Techniques and Catalysts
- Ammonia Synthesis and Nitrogen Reduction
- Nanomaterials for catalytic reactions
- Catalysis for Biomass Conversion
- Electrocatalysts for Energy Conversion
- Electron and X-Ray Spectroscopy Techniques
- Advanced Chemical Physics Studies
- Catalysis and Hydrodesulfurization Studies
- Catalysts for Methane Reforming
- Electronic and Structural Properties of Oxides
- Ionic liquids properties and applications
- Advanced Photocatalysis Techniques
- Catalysis and Oxidation Reactions
- Molecular Junctions and Nanostructures
- Organometallic Complex Synthesis and Catalysis
- Nanocluster Synthesis and Applications
- Graphene research and applications
- Surface Chemistry and Catalysis
- Surface and Thin Film Phenomena
- Quantum, superfluid, helium dynamics
Agency for Science, Technology and Research
2015-2025
Institute of High Performance Computing
2015-2025
University of Wisconsin–Madison
2018-2021
Madison Group (United States)
2018-2019
Institute of Bioengineering and Nanotechnology
2012-2013
Recent developments in machine learning interatomic potentials (MLIPs) have empowered even nonexperts to train MLIPs for accelerating materials simulations. However, reproducibility and independent evaluation of presented MLIP results is hindered by a lack clear standards current literature. In this Perspective, we aim provide guidance on best practices documenting use while walking the reader through development deployment including hardware software requirements, generating training data,...
Hydrogen bonding accelerates many catalytic reactions by orienting intermediates, stabilizing transition states, and even opening reaction pathways. However, most mechanistic studies regarding the decomposition of formic acid (FA), a promising hydrogen storage material, neglect hydrogen-bonding interactions though FA is strong hydrogen-bond donor acceptor. Here, we probe formation bimolecular hydrogen-bonded complexes between formate (FA–HCOO complexes) adsorbed on metal surfaces how these...
Co-promotion of Ag catalysts by Re and Cs leads to ethylene oxide (EO) selectivity higher than that achievable either promoter alone. However, the atomistic electronic mechanisms behind this synergistic co-promotion remain unclear. Here, we shed light on how promote epoxidation elucidating realistic catalyst models using machine learning-accelerated first-principles simulations, characterizing their properties, constructing structure–selectivity relationships. Together with a comprehensive...
Realistically modelling how solvents affect catalytic reactions is a longstanding challenge due to its prohibitive computational cost. Typically, an explicit atomistic treatment of the solvent molecules needed together with molecular dynamics (MD) simulations and enhanced sampling methods. Here, we demonstrate utility machine learning interatomic potentials (MLIPs), coupled active learning, enable fast accurate adsorption on heterogeneous catalysts. MLIPs trained on-the-fly were able...
Abstract The synthesis of quinolines has been achieved through a one‐pot, two‐step tandem reaction catalyzed with AgPd alloy nanoparticles supported on carbon. the coupling ketone primary alcohol hydrogen autotransfer process, which yields α‐alkylated ketones under an Ar flow. These are reacted 2‐aminobenzyl alcohols in modified Friedländer to give polysubstituted moderate good yields.
The adsorption of atomic (H, C, N, O, S) and molecular (OH, CHx, NHx, CO, NO, CN, N2, HNO, NOH, HCN, x = 1–3) species at 1/4 monolayer coverage on an extended Ag(111) surface was studied using periodic density functional theory. Geometries energies were calculated self-consistently the PW91 functional; nonself-consistent RPBE are also provided. We analyze binding energies, geometries, estimated diffusion barriers, harmonic vibrational frequencies, energetic geometric deformation parameters...
Abstract A CO 2 ‐mediated hydrogen storage energy cycle is a promising way to implement economy, but the exploration of efficient catalysts achieve this process remains challenging. Herein, sub‐nanometer Pd–Mn clusters were encaged within silicalite‐1 (S‐1) zeolites by ligand‐protected method under direct hydrothermal conditions. The obtained zeolite‐encaged metallic nanocatalysts exhibited extraordinary catalytic activity and durability in both hydrogenation into formate formic acid (FA)...
The demand for harmless and efficient energy sources is remarkably expanding, particularly after the increased awareness of global warming, greenhouse gas emissions, immense fossil fuel consumption, so forth. Formic acid considered a potential candidate as an carrier reversible hydrogen storage owing to its decomposition (H2) carbon dioxide (CO2) in presence suitable catalysts. However, selective formic using classical heterogeneous catalysis still challenging because most catalysts which...
The dehydrogenation of formic acid can provide an efficient pathway for hydrogen generation in the presence a suitable catalyst. Homogeneous catalysts have been extensively studied and utilized highly active selective processes compared to conventional heterogeneous catalysis, which often shows lower reactivity selectivity. However, latter is preferred practical applications, considering its easy separation recyclability. By incorporating homogeneous organometallic complex on appropriate...
Hydrogen bonding interactions alter the nanoscale reaction mechanisms of many chemistries. Yet, it remains unclear how they affect heterogeneously catalyzed decomposition formic acid (FA), a intense interest since FA is promising hydrogen carrier. Here, we elucidate affects for on Cu(111) by combining first-principles density functional theory calculations to calculate energetics, Latin-hypercube sampling stable high-coverage adsorbate configurations, and coverage self-consistent mean-field...
Thermodynamic/kinetic isotope effects for H<sub>2</sub>/D<sub>2</sub> dissociative adsorption calculated on metal surfaces offer a means to identify active sites.
Hydrogen isotope effects are influenced by adsorbate coverage: at high coverages, lower than low coverages. This helps to rationalize observed effects, allowing more precise elucidation of reaction mechanisms.
Abstract A CO 2 ‐mediated hydrogen storage energy cycle is a promising way to implement economy, but the exploration of efficient catalysts achieve this process remains challenging. Herein, sub‐nanometer Pd–Mn clusters were encaged within silicalite‐1 (S‐1) zeolites by ligand‐protected method under direct hydrothermal conditions. The obtained zeolite‐encaged metallic nanocatalysts exhibited extraordinary catalytic activity and durability in both hydrogenation into formate formic acid (FA)...
Formic acid (HCOOH or FA) is a clean, safe, and renewable hydrogen storage material. Although Au catalysts decompose vapor-phase FA with high activity selectivity toward hydrogen, the active site reaction mechanism remain unclear. Here, we show that subnanometric Au18 cluster (0.8 nm in diameter) likely species for decomposition. We performed coverage self-consistent, density functional theory-based kinetic Monte Carlo simulations of decomposition on gas-phase clusters, predicting 100%...
Evolution of the molecular orbitals during CO–CO coupling on Cu(100) surface and identification corresponding frontier orbitals.
Abstract The diverse coordination environments on the surfaces of discrete, three-dimensional (3D) nanoclusters contribute significantly to their unique catalytic properties. Identifying numerous adsorption sites and diffusion paths these clusters is however tedious time-consuming, especially for large, asymmetric nanoclusters. Here, we present a simple, automated method constructing approximate 2D potential energy atomic species 3D with minimal human intervention. These fully characterize...
Isotopes are indispensable tools for elucidating catalytic reaction mechanisms. Yet, computational isotopic studies in heterogeneous catalysis remain scarce, especially when compared with other subfields of chemistry. In this review, we discuss isotope effects from a viewpoint, focusing specifically on catalysts. First, review methods predicting kinetic and equilibrium individual elementary steps, as well simulating the apparent multistep reactions. Second, influence often-neglected...