A5003442464- Machine Learning in Materials Science
- Catalytic Processes in Materials Science
- Electrocatalysts for Energy Conversion
- Advanced Chemical Physics Studies
- Catalysis and Oxidation Reactions
- nanoparticles nucleation surface interactions
- Electronic and Structural Properties of Oxides
- Computational Drug Discovery Methods
- Electrochemical Analysis and Applications
- Carbon Dioxide Capture Technologies
- Catalysis and Hydrodesulfurization Studies
- Synthesis and Reactivity of Sulfur-Containing Compounds
- Structural and Chemical Analysis of Organic and Inorganic Compounds
- Advanced Photocatalysis Techniques
- Phenothiazines and Benzothiazines Synthesis and Activities
- Fuel Cells and Related Materials
- Ammonia Synthesis and Nitrogen Reduction
- X-ray Diffraction in Crystallography
- Advanced Materials Characterization Techniques
- Neural Networks and Applications
- Molecular Junctions and Nanostructures
- Scientific Computing and Data Management
- Topic Modeling
- Chemical and Physical Properties of Materials
- Synthesis and Catalytic Reactions
Carnegie Mellon University
2016-2025
National Energy Technology Laboratory
2008-2015
United States Department of Energy
2010-2012
Fritz Haber Institute of the Max Planck Society
2008
University of Delaware
2002-2006
North Carolina State University
1997
University of Hertfordshire
1995
Massachusetts Institute of Technology
1980
Newcastle University
1973
We present a method for calculating the stability of reaction intermediates electrochemical processes on basis electronic structure calculations. used that in combination with detailed density functional calculations to develop description free-energy landscape oxygen reduction over Pt(111) as function applied bias. This allowed us identify origin overpotential found this reaction. Adsorbed and hydroxyl are be very stable at potentials close equilibrium, calculated rate constant activated...
A density functional theory database of hydrogen chemisorption energies on close packed surfaces a number transition and noble metals is presented. The bond are used to understand the trends in exchange current for evolution. volcano curve obtained when measured currents plotted as function calculated adsorption simple kinetic model developed origin volcano. also consistent with Pt being most efficient electrocatalyst © 2005 Electrochemical Society. All rights reserved.
Abstract Trends in electrocatalytic activity of the oxygen evolution reaction (OER) are investigated on basis a large database HO* and HOO* adsorption energies oxide surfaces. The theoretical overpotential was calculated by applying standard density functional theory combination with computational hydrogen electrode (SHE) model. We showed that discovery universal scaling relation between vs HO*, it is possible to analyze free energy diagrams all oxides general way. This gave rise an volcano...
The atomic simulation environment (ASE) is a software package written in the Python programming language with aim of setting up, steering, and analyzing atomistic simulations. In ASE, tasks are fully scripted Python. powerful syntax combined NumPy array library make it possible to perform very complex tasks. For example, sequence calculations may be performed use simple 'for-loop' construction. Calculations energy, forces, stresses other quantities through interfaces many external electronic...
Periodic density functional calculations are used to illustrate how the combination of strain and ligand effects modify electronic surface chemical properties Ni, Pd, Pt monolayers supported on other transition metals. Strain shown change width d band, which subsequently moves up or down in energy maintain a constant band filling. Chemical such as dissociative adsorption hydrogen controlled by changes induced average modification d-band width.
The modification of the electronic and chemical properties Pt(111) surfaces by subsurface 3d transition metals was studied using density-functional theory. In each case investigated, Pt surface d-band broadened lowered in energy interactions with metals, resulting weaker dissociative adsorption energies hydrogen oxygen on these surfaces. magnitude decrease largest for early smallest late metals. some cases, calculated to be endothermic. investigated this study had no lateral strain them,...
Mixed Fe–Ni oxide electrocatalysts for the oxygen evolution reaction in alkaline electrolytes were synthesized using three different approaches: evaporation induced self-assembly, hard templating, and dip-coating. For each synthesis method, a peak activity was observed near 10 mol % Fe content, where mixed metal substantially more active than parent electrocatalysts. X-ray diffraction (XRD) analysis showed formation of NiO/NiFe2O4 phase at low concentrations, Fe2O3 compositions above 25 Fe....
The trends in adsorption energies of the intermediates oxygen reduction and evolution reactions on transition metals their oxides are smoothly captured by number outer electrons. This unique descriptor permits construction predictive adsorption-energy grids explains existence scaling relationships among these compounds.
Benchmarking is a community-based and (preferably) community-driven activity involving consensus-based decisions on how to make reproducible, fair, relevant assessments. In catalysis science, important catalyst performance metrics include activity, selectivity, the deactivation profile, which enable comparisons between new standard catalysts. also requires careful documentation, archiving, sharing of methods measurements, ensure that full value research data can be realized. Beyond these...
Using a combination of low-temperature scanning tunneling microscopy and density functional theory it is demonstrated how the nature an inert host metal alloy can affect thermodynamics kinetics reaction pathway in much more profound way than simply dilution, electronic, or geometric effect. This study reveals that individual, isolated Pd atoms promote ${\mathrm{H}}_{2}$ dissociation spillover onto Cu(111) surface, but same mechanism not observed for identical array Au(111).
We present a first-principles atomistic thermodynamics framework to describe the structure, composition, and segregation profile of an alloy surface in contact with (reactive) environment. The method is illustrated application ${\mathrm{Ag}}_{3}\mathrm{Pd}(111)$ oxygen atmosphere, we analyze trends segregation, adsorption, free energies. observe wide range adsorption energies on various configurations, including binding that stronger than $\mathrm{Pd}(111)$ weaker $\mathrm{Ag}(111)$ surface....
The effects of varying alkaline electrolyte and Fe levels on the performance active-phase structure NiOOH thin films for catalysis oxygen evolution reaction were studied. An effect catalytic was observed. Under purified conditions, current densities followed trend Cs+ > K+ ≈ Na+ Li+ at 1 mA/cm2. Fe-saturated all densities. Voltammetry coupled with Raman spectroscopy studies in LiOH CsOH. spectra fit to Gaussian functions analyzed quantitatively based mean peak positions. Both CsOH promoted...
Systematic prediction of the redox reaction energetics large sets 3d transition metal oxides is imperative to selection oxygen carrier candidates in applications ranging from chemical looping solid oxide fuel cell (SOFC) cathode design. In particular, energetic study vacancy formation unmixed perovskites with La, alkali, and alkaline A-site cations—as well as B-site cations—is a crucial first step understanding tunability afforded by cation doping ABO3 materials. An assessment relative...
A primary amine-functionalized polymeric ion-exchange resin (Lewatit VP OC 1065, Lanxess) was evaluated for use in CO2 capture applications. The characterized by SEM, DRIFTS-IR, N2 adsorption isotherms, and packed bed sorption measurements to determine some of the characteristic properties resin. Capture capacities ranging from 1.85 1.15 mol CO2/kg sorbent were obtained a reactor exposed 10 vol % at temperatures 30 70 °C. capacity stable over 18 adsorption/regeneration cycles. through...
There are known errors in oxidation energies of transition metal oxides caused by an improper treatment their d-electrons. The Hubbard U is the computationally cheapest addition one can use to capture correct reaction energies, but specific oftentimes must be empirically determined only when suitable experimental data exist. We evaluated effect adding a calculated, linear response on predicted adsorption scaling relationships, and activity trends with respect oxygen evolution for set...
The development of machine-learned potentials for catalyst discovery has predominantly been focused on very specific chemistries and material compositions. While they are effective in interpolating between available materials, these approaches struggle to generalize across chemical space. recent curation large-scale data sets offered the opportunity build a universal machine-learning potential, spanning composition If accomplished, said potential could accelerate process variety applications...
The demand for green hydrogen has raised concerns over the availability of iridium used in oxygen evolution reaction catalysts. We identify catalysts with aid a machine learning-aided computational pipeline trained on more than 36,000 mixed metal oxides. accurately predicts Pourbaix decomposition energy (Gpbx) from unrelaxed structures mean absolute error 77 meV per atom, enabling us to screen 2070 new metallic oxides respect their prospective stability under acidic conditions. search...