A5029378576- Spectroscopy and Quantum Chemical Studies
- Electrochemical Analysis and Applications
- CO2 Reduction Techniques and Catalysts
- Electrocatalysts for Energy Conversion
- Ionic liquids properties and applications
- Ammonia Synthesis and Nitrogen Reduction
- Fuel Cells and Related Materials
- Nanopore and Nanochannel Transport Studies
- Copper-based nanomaterials and applications
- Thermodynamic properties of mixtures
- Nanomaterials for catalytic reactions
- Analytical Chemistry and Sensors
- Catalysis and Hydrodesulfurization Studies
- Electrostatics and Colloid Interactions
- Advanced Chemical Physics Studies
- nanoparticles nucleation surface interactions
- Catalysts for Methane Reforming
- Catalysis for Biomass Conversion
Pennsylvania State University
2022-2025
University of Michigan
2024
Water polarizability at a metal interface plays an essential role in electrochemistry. We devise classical molecular dynamics approach with efficient description of polarization and novel ac field method to measure the local dielectric response interfacial water. adlayers next surface exhibit higher-than-bulk in-plane negative out-of-plane constants, latter corresponding physically overscreening applied field. If we account for gap region interface, average constant is quite low (ε_{⊥}≈2),...
<title>Abstract</title> Aqueous nitrate (NO<sup>−</sup><sub>3</sub> ) can be electrocatalytically reduced to value-added or benign products. However, the impact of electrochemical potential on key reaction steps remains poorly understood. Using explicit and analytical grand-canonical density functional theory (eGC-DFT aGC-DFT), we investigate dependence adsorption dissociation pure metals Cu-based single-atom alloys (SAAs). With aGC-DFT, find electrosorption valencies for...
Standard simulation interaction parameters sometimes predict liquid properties at variance with experiment, especially for polar liquids. In this work, we systematically scaled the partial charges of three alkyl alcohols to evaluate whether adjusting charges, and thus electrostatic interactions, can improve agreement experimental values key properties, including dielectric constant, vapor pressure, density, self-diffusion coefficient. Changing also affects structures, which are evaluated...
Despite the importance of CO adsorption in many electrocatalytic reaction mechanisms, there has been little investigation dependence free energy on applied potential. Herein, we report potential-dependent Cu electrodes using a grand-canonical density functional theory approach. We demonstrate that, within working potential range CO2 reduction Cu(111) and Cu(100), strength can change by over 0.1 eV. Our analyses explain through an interfacial capacitance loss upon as well orbital relaxation...
CuO-based catalysts are active for the oxygen evolution reaction (OER), although form of copper OER is still unknown. We combine operando Raman experiments and density functional theory (DFT) electronic structure calculations to determine Cu(O)xOHy present under conditions. spectra show a distinct feature related "Cu3+" species, which only highly oxidizing DFT used produce theoretical standards match unique potentials. This method identifies range Cu3+-containing compounds feature. then...
Acid-catalyzed alcohol dehydration is a key reaction step in biomass upgrading, kinetics of which are significantly affected by mixed aqueous solvents. Computational modeling can provide fundamental understanding solvation effects catalysis, and ultimately predictive tool for optimizing reactivity selectivity. We introduce multiscale method that combines density functional theory (DFT) with classical molecular dynamics (MD) to investigate the effect solvents (water DMSO/GVL/MeCN) on...
Density functional theory (DFT) modeling has been useful to electrocatalyst research, yet simulating the complexities of electrode–electrolyte interface hinders progress in understanding reaction mechanisms and underlying kinetics. Though many approaches incorporating electrochemical double layer (EDL) features DFT calculations have developed, uncertainty interfacial solvent properties distribution ions leave impact EDL on electrocatalytic kinetics unclear. Elucidating sensitivity...
The thermodynamics of hydrogen bonds in aqueous and acidic solutions significantly impacts the kinetics acid reaction chemistry. We utilize this work a multiscale approach, combining density functional theory (DFT) with classical molecular dynamics (MD) to model bond an solution. Using thermodynamic cycles, we split solution phase free energy into its gas counterpart plus solvation energies. validate DFT/MD approach by calculating between two water molecules (H2O-···-H2O), transform H3O+...
Knowledge of the concentration alkali cations in an electrochemical double layer is essential for interpreting and leveraging cation effects electrocatalysis. We systematically study profiles four (Li+, Na+, K+, Cs+) at a Ag(111)-aqueous interface. Using classical molecular dynamics, potential mean force (PMF) approaching metal surface was computed decomposed into contributions from solvent surface. find that hydration shell deformations contribute importantly to free energy near electrode....