Theoretical Catalysis - Rossmeisl Group

In our group we work with theoretical catalysis. Which is based on atomic scale simulations and dynamics. In this way we have a direct way into the structure, reactions and intermediates at an atomic level.

Professor Jan Rossmeisl is center leader of the Center of Excellence Center for High Entropy Alloy Catalysis (CHEAC).

Research

Our main research fields are:
• Electrocatalysis for various reactions: water splitting, CO2 reduction ect.
• Screening of semi conductor materials

The hypothesis is that when understanding the process on an atomic scale it is possible to improve both the selectivity and minimize the over-potential (energy loss, for electrochemistry) in the reactions. Finally, when materials are found, they will be tested experimentally with our many partners.

For the computer simulations mainly state of the art periodic Density Functional Theory (DFT) are be applied. DFT simulations offer the right trade-off between accuracy and system size for modeling of catalysis interfaces. The quantum mechanics accurately describe the breaking and formation of chemical bonds and it is possible to model up to ~1000 atoms, which is needed for minimizing the finite size effects. For these calculations we apply our own cluster Katla, at KU, which gives us direct and close by super fast calculations.

katlaDB

KatlaDB - Theoretical Catalysis Database

	Competitive Strain Modulation of Oxygen Reduction Reaction in Monolayer Binary Alloy Surfaces
	Prospects of Using High Entropy Oxides for the Oxygen Evolution Reaction
	Impact of Charging in Constant Potential Electrochemistry Modeling
	Adsorbate Resonance Induces Water-Metal Bonds in Electrochemical Interfaces
	Self-Induced Long-Range Surface Strain Improves Oxygen Reduction Reaction
	Coverage, Repulsion, and Reactivity of Hydrogen on High-Entropy Alloys
	N2 dissociation on AuCoFeMoRu high-entropy alloys: Circumventing scaling relations and step dependencies
	Insight into selectivity differences of glycerol electro-oxidation on Pt(111) and Ag(111)
	*Geometry-adaptive catalysts for elevating towards the ideal oxygen electrocatalysis*
	*Enhancing Carbon Dioxide Reduction Performance via Molecular Film-Induced Copper Surface Reconstruction*
	*The Missing Link for Electrochemical CO2 Reduction: Classification of CO vs. HCOOH Selectivity via PCA, Reaction Pathways*
	Lattice oxygen evolution in rutile Ru_1-xNi_xO₂ electrocatalysts
	Ru rich Ru-Mn-O phases for selective suppression of chlorine evolution in sea water electrolysis
	Identifying the best Catalyst for the Oxygen Evolution Reaction through Complementary Experimental and Theoretical Exploration of a High Entropy Oxide Composition Space
	Role of vacancies in structural thermalization of binary and high-entropy alloys
	Cooperative effects drive water oxidation catalysis in cobalt electrocatalysts through the destabilisation of intermediates
	Tailoring the facet distribution on copper with chloride
	Tuning the chemical composition of high-entropy alloys to prevent their dissolution
	Steering carbon dioxide reduction toward C–C coupling using copper electrodes modiﬁed with porous molecular ﬁlms
	Modeling Anion Poisoning during Oxygen Reduction on Pt Near-Surface Alloys
	Unravelling the effects of active site densities and energetics on the water oxidation activity of iridium oxides
	Synergistic effect of p-type and n-type dopants in semiconductors for efficient electrocatalytic water splitting
	CO₂ reduction on Ag-Cu-Pd
	Structure of the (bi)carbonate adlayer on Cu(100) electrodes
	Modeling electrochemical proton adsorption at constant potential with explicit charging
	Following Paths of Maximum Catalytic Activity in the Composition Space of High-Entropy Alloys
	Bridging the Catalyst Reactivity Gap Between Au and Cu for the Reverse Water Gas Shift Reaction
	A Mean Field Model for Oxygen Reduction Electrocatalytic Activity on High-Entropy Alloys
	Predicting Catalytic Activity in Hydrogen Evolution Reaction
	Selectivity and Intrinsic Activity of Functionalized Cu Surfaces: Can the CO2RR be Improved on Cu?
	Formic Acid Oxidation Reaction
	Exploring the Mobility of Cu in Bimetallic Nanocrystals to Promote Atomic-Scale Transformations under a Reactive Gas Environment
	High entropy oxides for the oxygen evolution reaction
	Local order in AgAuCuPdPt high entropy alloy surfaces
	Catalytic CO₂/CO Reduction: Gas, Aqueous and Aprotic phase
	Formation of iridium colloidal nanocrystals: chemical insights from in situ X-ray total scattering experiments
	Bayesian Optimization of High-Entropy Alloy Compositions for Electrocatalytic Oxygen Reduction
	Electrochemical Nitric Oxide Reduction on Metal Surfaces *Correspondence: jan.rossmeisl@chem.ku.dk DOI: (to be provided) Link to zip file containing data and scripts for reproduction: XX (XX MB)
	Rationally tailoring catalysts for the CO oxidation reaction by using DFT calculations We use O on-top and CO on-top adsorption energies to estimate O bridge and O hollow adsorption energies, and predict activation and reaction energies for CO oxidation reactions (COOR).
	The role of catalyst in controlling N2 reduction selectivity: a unified view of nitrogenase and solid electrodes
	Kondo Effect and Spin Coupling in the Retinoic Acid Molecule We investigate the exchange interaction of deprotonated retinoic acid molecules across hydrogen bonds.
	The Role of the Band Gap for the Interaction Energy of Coadsorbed Fragments We investigate the interaction energy of coadsorbed fragments on band gap oxides and we propose to use the band gap as a descriptor of the interaction energy.
	Defect chemistry and electrical conductivity of Sm-doped La_1−xSr_xCoO_3−δ for solid oxide fuel cells We have calculated the electrical conductivity of the SOFC cathode contact material La_1−xSr_xCoO_3−δ at 900 K. Furthermore, we have studied the chemistry of neutral and charged intrinsic and extrinsic defects (dopants) in La_0.5Sr_0.5CoO₃ and calculated the conductivity of the doped systems. In particular, we find that doping with Sm on the La site should enhance the conductivity.
	Single site porphyrine-like structures advantages over metals for selective electrochemical CO₂ reduction The data is supplementary material for the paper, which includes all structures and binding energies calculated. Further, figures have been plotted with labels for all metals and porphyrine-like structures.
	Catalyst design criteria and fundamental limitations in the electrochemical synthesis of dimethyl carbonate We demonstrate how density functional theory (DFT) calculations and experiments advance our understanding of electrocatalytic production of chemicals. Using DFT, we form design criteria for dimethyl carbonate electrosynthesis on metallic surfaces. These criteria allow us to identify copper as an interesting candidate for the electrode material as being selective to dimethyl carbonate while requiring ≈ 1 V lower potential than a gold electrode. Electrode stability issues show that the design criteria presented herein are necessary but not sufficient requirements that the ideal electrode should satisfy.
	Modelling pH and Potential in Dynamic Structures of the Water/Pt(111) Interface on the Atomic Scale We present atomic-scale structures of the Pt(111)/water interface, by calculating distributions of atomic distances as functions of pH. The structure of the Pt(111)/water interface is a particularly interesting model system in electro-catalysis for proton exchange reactions, especially the oxygen reduction reaction in polymer electrolyte membrane fuel cells. Further insight into such reactions requires accurate simulations of the electrolyte structure in the interface. The study displays many interesting details in the behaviour of the electrolyte structure, e.g. that the electrolyte structure average responds to the presence of protons by a H-down water orientation and that hexagonal adsorbed water layers are present only when they are anchored at the surface by HO. New adsorbate configurations were also found at 5/12 ML coverage of HO, suggesting an explanation for reported cyclic voltammetry experiments. The present study is a step towards a more complete understanding of the structure of the electrochemical interface on the atomic scale.
	Electrochemical CO₂ Reduction: A Classification Problem The data is supplementary material for the paper, which includes all structures, binding energies and energy ensembles. Further, plotting script is given to plot Figure 1 of the paper and the layout can be used to also achieve and plots other data from the database.
	Understanding activity and selectivity of metal-nitrogen-doped carbon catalysts for electrochemical reduction of CO₂ The data is supplementary material for the paper, which includes all structures and binding energies calculated. Further, experimental data together with plotting script for Figure 5 in the paper can be downloaded.
	Enhanced Carbon Dioxide Electroreduction to Carbon Monoxide over Defect-Rich Plasma-Activated Silver Catalysts The data is supplementary material for the paper, which includes all structures and binding energies calculated.
	Accessing the Inaccessible: Analyzing the Oxygen Reduction Reaction in the Diffusion Limit A numerical site-blocking model to simulate ORR currents in the absence of mass transport limitatons.
	Fundamental limitation of electrocatalytic methane conversion to methanol A database with all structures and scripts for plotting figures.
	Oxidation of Ethylene Carbonate on Li Metal Oxide Surfaces Contains a database file with structures and energies, and scrips for plotting all figures from the paper.
	Electrocatalytic transformation of HF impurity to H2 and LiF in lithium-ion batteries We have discussed the formation of H2 and LiF from a dissociation of HF in Li-ion batteries. The database contains all the calculations used in the paper to produce the phase diagram of Li and identify trends.
	Climbing the 3D Volcano for the Oxygen Reduction Reaction Using Porphyrin Motifs Contains a database file with structures and energies, and scrips for plotting all figures from the paper.
	Electrochemical CO reduction: A property of the electrochemical interface Contains a .zip file with multiple folders with databases and scrips for plotting figures from the paper.
	High-Entropy Alloys as a Discovery Platform for Electrocatalysis
	Unravelling Mechanistic Reaction Pathways of the Electrochemical CO2 Reduction on Fe-N-C Single-Site Catalysts
	High-Entropy Alloys as Catalyst for the CO2 and CO Reduction Reactions
	Realistic Cyclic Voltammograms from Ab Initio Simulations in Alkaline and Acidic Electrolytes Contains a .zip file with databases and scripts for plotting the figures from the paper.
	pH and anion effects on Cu-phosphate interfaces for CO electroreduction Contains a .zip file with databases and scripts for plotting the figures from the paper.
	Surface Electro-Catalysis on High-Entropy Alloys
	Long‐Range, Directional Ligand Effects in Metallic Alloys A statistical analysis uncovers what atomic positions, near the binding site on the surface of an alloy, exert an electronic effect on the adsorbate–surface bond.
	Capturing the Formation Mechanism of Additive-Mediated Intermetallic PdCu Nanoparticles Files for reproducing the DFT calculations on the stability of the investigated phases of PdCu.
	Three-Dimensional Carbon Electrocatalysts for CO2 or CO Reduction Contains a database file with structures and energies, and scrips for plotting all figures from the paper.
	Insights in the Oxygen Reduction Reaction: From Metallic Electrocatalysts to Diporphyrins Contains a database file with all the structures for the paper.
	Oxygen evolution reaction: a perspective on a decade of atomic scale simulations
	Lattice distortion releasing local surface strain on high-entropy alloys