Theoretical Catalysis

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.

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 - Theoretical Catalysis Database

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). 

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 La1−xSrxCoO3−δ for solid oxide fuel cells
We have calculated the electrical conductivity of the SOFC cathode contact material La1−xSrxCoO3−δ at 900 K. Furthermore, we have studied the chemistry of neutral and charged intrinsic and extrinsic defects (dopants) in La0.5Sr0.5CoO3 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

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

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

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
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
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
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
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 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.

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.

Lattice distortion releasing local surface strain on high-entropy alloys