A5042139840- Electrocatalysts for Energy Conversion
- CO2 Reduction Techniques and Catalysts
- Electrochemical Analysis and Applications
- Ionic liquids properties and applications
- Molecular Junctions and Nanostructures
- Ammonia Synthesis and Nitrogen Reduction
- Catalysis for Biomass Conversion
- Catalytic Processes in Materials Science
- Carbon Dioxide Capture Technologies
- Carbon dioxide utilization in catalysis
- Advanced battery technologies research
- Machine Learning in Materials Science
- Fuel Cells and Related Materials
- Hydrogen Storage and Materials
- Catalysis and Oxidation Reactions
- Advanced Thermoelectric Materials and Devices
- Catalysis and Hydrodesulfurization Studies
- Membrane Separation and Gas Transport
- Catalysts for Methane Reforming
- Advanced Battery Materials and Technologies
- Hybrid Renewable Energy Systems
- Spectroscopy and Quantum Chemical Studies
- Advanced Chemical Physics Studies
- Nanomaterials for catalytic reactions
- Hydrogen embrittlement and corrosion behaviors in metals
Lawrence Livermore National Laboratory
2019-2025
Materials Science & Engineering
2025
Quantum Simulations (United States)
2023
Pacific Northwest National Laboratory
2017-2021
Material Sciences (United States)
2020
Battelle
2019
Pennsylvania State University
2014-2018
Robert Bosch (United States)
2016
Carnegie Mellon University
2011-2012
Electrocatalytic hydrogenation is increasingly studied as an alternative to integrate the use of recycled carbon feedstocks with renewable energy sources. However, abundant empiric observations available have not been correlated fundamental properties substrates and catalysts. In this study, we investigated electrocatalytic a homologues series carboxylic acids, ketones, phenolics, aldehydes on variety metals (Pd, Rh, Ru, Cu, Ni, Zn, Co). We found that rates carbonyl reduction in correlate...
Electrolytic ions are known to impact the rates of electrocatalytic reactions, though a molecular understanding mechanism such is not well understood. We employ density functional theory investigate specific adsorption potassium and iodine on Cu (111), (100) (211) electrode surfaces under CO2 electroreduction (CO2 ER) conditions explore their effect reaction energetics binding strength intermediates. The calculated equilibrium potentials for K* I* (* denotes surface-adsorbed species) suggest...
A detailed mechanistic study of the electrochemical hydrogenation aldehydes is presented toward goal identifying how organic molecules in solution behave at interface with charged surfaces and what best manner to convert them. Specifically, this focuses on designing an electrocatalytic route for ambient-temperature postpyrolysis treatment bio-oil. Aldehyde reductions are needed biomass into fuels or chemicals. combined experimental computational approach taken catalyst design provide...
Formate is an important value-added chemical that can be produced via electrochemical CO2 reduction reactions (CO2RR). Cu2O-based catalysts have previously demonstrated decent activity for formate generation; however, they often suffer from poor stability under reductive conditions. Here, we report a new Cu2O/CuS composite catalyst simultaneously achieves excellent faradaic efficiency of 67.6% and large partial current density 15.3 mA/cm2 at −0.9 V vs RHE formate. Importantly, it maintains...
Engineering the electrolyte microenvironment represents an attractive route to tuning selectivity of electrocatalytic reactions beyond catalyst composition and morphology. However, harnessing full potential this approach requires understanding interplay between voltage, composition, adsorbate binding within electrical double layer, which is absent from usual theoretical approaches. In work, we apply a recently developed density functional theory (DFT)-continuum based on effective screening...
The electrochemical oxidation of alcohols is being explored as a favorable substitute for the oxygen evolution reaction owing to its capability generate high-value products and lower overpotentials. Herein, we present systematic investigation into 5-hydroxymethylfurfural (HMF), model biomass platform chemical, on thin-film nickel catalyst, aiming investigate underlying mechanism shed light role catalyst's microenvironment phase activity product selectivity. Utilizing combined experimental...
We propose the Systems-to-Atoms (S2A) modeling framework that integrates kinetics of reaction chemistry and structural configurations across various length scales with aim establishing a versatile template for multiscale reactive flow problems to predict operando activity catalyst materials. The approach encompasses microkinetic model analyze surface reactions on individual facets nanoparticles coupled computation average rates specific size distributions. Macro-homogeneous are derived as...
We use rigorous group-theoretic techniques and molecular dynamics to investigate the connection between structural symmetry ionic conductivity in garnet family of solid Li-ion electrolytes. identify new ordered phases order-disorder phase transitions that are relevant for optimization. Ionic transport this materials is controlled by frustration Li sublattice caused incommensurability with host structure at noninteger concentrations, while explain regions sharply lower conductivity. Disorder...
DFT calculations demonstrate CO surface poisoning of Pt, Co, Ni, and Fe electrodes during 2 reduction.
The thermodynamic state of H2 adsorbed on Pt in the aqueous phase was determined by kinetic analysis reacting with D2 O to HDO, HD, and , DFT-based ab initio molecular dynamics simulations adsorption Pt(111), Pt(110), nanoparticles. Dissociative is significantly weakened compared at gas-solid interfaces. Water destabilizes H atoms, decreasing heat 19-22 kJ molH2-1 while inducing an additional entropy loss 50-70 J K-1 . Upon dissociative average distance water from surface increases liquid...
In aqueous phase, the rates of hydrogenation aromatic substrates such as phenol on Pt/C and Rh/C are influenced by varying activity hydronium ions. Decreasing pH from 8 to 1 increases rate Pt at 20 bar H2 80 °C 15-fold. This increase is attributed weakening hydrogen binding energy (HBE) metal surface with decreasing pH. A weaker HBE lower also predicted ab initio molecular dynamics simulations, providing atomistic insight into impact electrolyte ion distribution interfacial solvent...
Bridging polymer design with catalyst surface science is a promising direction for tuning and optimizing electrochemical reactors that could impact long-term goals in energy sustainability. Particularly, the interaction between inorganic surfaces organic-based ionomers provides an avenue to both steer reaction selectivity promote activity. Here, we studied role of imidazolium-based electrocatalytic CO2 reduction CO (CO2R) on Ag found they produce no effect CO2R activity yet strongly...
Abstract Although multiple oxide-based solid electrolyte materials with intrinsically high ionic conductivities have emerged, practical processing and synthesis routes introduce grain boundaries other interfaces that can perturb primary conduction channels. To directly probe these effects, we demonstrate an efficient general mesoscopic computational method capable of predicting effective conductivity through a complex polycrystalline microstructure without relying on simplified equivalent...
Abstract Efficient storage of hydrogen is one the biggest challenges towards a potential economy. Hydrogen in liquid carriers an attractive alternative to compression or liquefaction at low temperatures. Liquid can be stored cost-effectively and transportation distribution integrated into existing infrastructures. The development efficient part work International Energy Agency Task 40: Hydrogen-Based Storage. Here, we report state-of-the-art for ammonia closed CO 2 -cycle methanol-based...
Abstract The activity and product selectivity of electrocatalysts for reactions like the carbon dioxide reduction reaction (CO 2 RR) are intimately dependent on catalyst's structure composition. While engineering catalytic surfaces can improve performance, discovering key sets rational design principles remains challenging due to limitations in modeling catalyst stability under operating conditions. Herein, we perform first‐principles density functional calculations adopting implicit...
Trends in the dissociative oxygen adsorption energy and vacancy formation on cubic LaBO(3) SrBO(3) perovskite (001) surfaces (where B = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu) their dependence strain, d-band filling, oxidation state were examined using density functional theory generalized gradient approximation. The effects of strain found to be small compared filling oxidations state. Electronic structure descriptors such as center B-atom identified for trends energy. A chemical correlation...
Density Functional Theory (DFT) based models have been widely applied towards investigating and correlating the reaction mechanism of CO<sub>2</sub> electroreduction (ER) to activity selectivity potential electrocatalysts.
Ethanol is a promising platform molecule for production of variety fuels and chemicals. Of particular interest the middle distillate (i.e., jet diesel blendstock) from renewable ethanol feedstock. State-of-the-art alcohol-to-jet technology requires multiple process steps based on catalytic dehydration to ethylene, followed by multistep oligomerization including n-butene formation then hydrotreatment distillation. Here we report that, over Ag-ZrO2/SBA-16 with balanced metal Lewis acid sites,...
Poly(ethyleneimine) (PEI)-based CO2 sorbents are a promising material class for use in capture applications, particularly direct air (DAC), due to their high amine content and capacities. The sorbent lifetime is key uncertainty the deployment of these materials such as they oxidize under conditions relevant candidate DAC process cycles. Here, we utilize thermogravimetric analysis/differential scanning calorimetry/FTIR spectroscopy characterize nature, rate, quantity volatile species formed...