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Papers by Jan Rossmeisl

Research paper thumbnail of A Flexible Theory for Catalysis: Learning Alkaline Oxygen Reduction on Complex Solid Solutions within the Ag-Pd-Pt-Ru Composition Space

Compositionally complex materials such as high-entropy alloys and oxides have the potential to be... more Compositionally complex materials such as high-entropy alloys and oxides have the potential to be efficient platforms for catalyst discovery because of the vast chemical space spanned by these novel materials. Identifying the composition of the most active catalyst materials, however, requires unraveling the descriptor-activity relationship, as experimental screening the multitude of possible element ratios quickly becomes a daunting task. In this work, we show that inferred adsorption energy distributions of *OH and *O on complex solid solution surfaces within the space spanned by the system Ag-Pd-Pt-Ru are coupled to the experimentally observed electrocatalytic performance for the oxygen reduction reaction. In total, the catalytic activity of 1582 alloy compositions is predicted with a cross-validated mean absolute error of 0.042 mA/cm2 by applying a theory-derived model with only two adjustable parameters. Trends in the discrepancies between predicted electrochemical performance ...

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Research paper thumbnail of Theoretical Trends in Particle Size Effects for the Oxygen Reduction Reaction

Zeitschrift für Physikalische Chemie, 2007

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Research paper thumbnail of Enzymatic versus Inorganic Oxygen Reduction Catalysts: Comparison of the Energy Levels in a Free-Energy Scheme

Inorganic Chemistry, 2010

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Research paper thumbnail of Steady state oxygen reduction and cyclic voltammetry

Faraday Discussions, 2009

The catalytic activity of Pt and Pt3Ni for the oxygen reduction reaction is investigated by apply... more The catalytic activity of Pt and Pt3Ni for the oxygen reduction reaction is investigated by applying a Sabatier model based on density functional calculations. We investigate the role of adsorbed OH on the activity, by comparing cyclic voltammetry obtained from theory with previously published experimental results with and without molecular oxygen present. We find that the simple Sabatier model predicts both the potential dependence of the OH coverage and the measured current densities seen in experiments, and that it offers an understanding of the oxygen reduction reaction (ORR) at the atomic level. To investigate kinetic effects we develop a simple kinetic model for ORR. Whereas kinetic corrections only matter close to the volcano top, an interesting outcome of the kinetic model is a first order dependence on the oxygen pressure. Importantly, the conclusion obtained from the simple Sabatier model still persists: an intermediate binding of OH corresponds to the highest catalytic activity, i.e. Pt is limited by a too strong OH binding and Pt3Ni is limited by a too weak OH binding.

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Research paper thumbnail of Prediction of solid oxide fuel cell cathode activity with first-principles descriptors

Energy & Environmental Science, 2011

ABSTRACT

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Research paper thumbnail of Oxidative trends of TiO2—hole trapping at anatase and rutile surfaces

Energy & Environmental Science, 2012

ABSTRACT Understanding the nature of photogenerated carriers in a photocatalyst is central to und... more ABSTRACT Understanding the nature of photogenerated carriers in a photocatalyst is central to understanding its photocatalytic performance. Based on density functional theory calculation we show that for TiO2, the most popular photo-catalyst, the electron hole self-trapping leads to band gap states which position is dependent on the type of surface termination. Such variations in hole state energies can lead to differences in photocatalytic activity among rutile and anatase surface facets. We find that the calculated hole state energies correlate with photo-deposition and photo-etching rates. We anticipated that our results can aid the design of more reactive photo-catalysts based on TiO2 and our approach can be utilized for other relevant photo-catalysts as well.

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Research paper thumbnail of Bifunctional anode catalysts for direct methanol fuel cells

Energy & Environmental Science, 2012

ABSTRACT Using the binding energy of OH* and CO* on close-packed surfaces as reactivity descripto... more ABSTRACT Using the binding energy of OH* and CO* on close-packed surfaces as reactivity descriptors, we screen bulk and surface alloy catalysts for methanol electro-oxidation activity. Using these two descriptors, we illustrate that a good methanol electro-oxidation catalyst must have three key properties: (1) the ability to activate methanol, (2) the ability to activate water, and (3) the ability to react off surface intermediates (such as CO* and OH*). Based on this analysis, an alloy catalyst made up of Cu and Pt should have a synergistic effect facilitating the activity towards methanol electro-oxidation. Using these two reactivity descriptors, a surface PtCu3 alloy is proposed to have the best catalytic properties of the Pt–Cu model catalysts tested, similar to those of a Pt–Ru bulk alloy. To validate the model, experiments on a Pt(111) surface modified with different amounts of Cu adatoms are performed. Adding Cu to a Pt(111) surface increases the methanol oxidation current by more than a factor of three, supporting our theoretical predictions for improved electrocatalysts.

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Research paper thumbnail of How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels

Energy & Environmental Science, 2010

ABSTRACT Density functional theory calculations explain copper's unique ability to conver... more ABSTRACT Density functional theory calculations explain copper's unique ability to convert CO2 into hydrocarbons, which may open up (photo-)electrochemical routes to fuels.

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Research paper thumbnail of Understanding the electrocatalysis of oxygen reduction on platinum and its alloys

Energy & Environmental Science, 2012

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Research paper thumbnail of Trends in oxygen reduction and methanol activation on transition metal chalcogenides

Electrochimica Acta, 2011

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Research paper thumbnail of Electronic hole localization in rutile and anatase TiO2 – Self-interaction correction in Δ-SCF DFT

Chemical Physics Letters, 2011

ABSTRACT We study electronic hole localization in rutile and anatase titanium dioxide by means of... more ABSTRACT We study electronic hole localization in rutile and anatase titanium dioxide by means of Δ-Self-Consistent Field Density Functional Theory. In order to compare stabilities of the localized and the delocalized hole states we introduce a simple correction to the wrong description of the localization processes within DFT. The correction removes the non-linearity of energy for fractional excitations. We show that the self-trapped and the delocalized hole states have comparable stability in rutile TiO2 whereas in anatase the former is favoured. The theoretical prediction of the adiabatic Potential Energy Surfaces for the hole localization compares well with published photoluminescence measurements.

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Research paper thumbnail of Modeling the electrified solid–liquid interface

Chemical Physics Letters, 2008

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Research paper thumbnail of Avoiding pitfalls in the modeling of electrochemical interfaces

Chemical Physics Letters, 2013

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Research paper thumbnail of Electrolysis of water on (oxidized) metal surfaces

Chemical Physics, 2005

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Research paper thumbnail of Modeling of the symmetry factor of electrochemical proton discharge via the Volmer reaction

Catalysis Today, 2013

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Research paper thumbnail of Atomic-Scale Modeling of Particle Size Effects for the Oxygen Reduction Reaction on Pt

Catalysis Letters, 2011

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Research paper thumbnail of The Influence of Particle Shape and Size on the Activity of Platinum Nanoparticles for Oxygen Reduction Reaction: A Density Functional Theory Study

Catalysis Letters, 2014

ABSTRACT Abstract We present first principle investigation of the influence of platinum nanoparti... more ABSTRACT Abstract We present first principle investigation of the influence of platinum nanoparticle shape and size on the oxygen reduction reaction activity. We compare the activities of nanoparticles with specific shapes (tetrahedron, octahedron, cube and truncated octahedron) with that of equilibrium particle shape at 0.9 V. Furthermore, the influence of support is assessed by looking at the particles with and without support interactions. The equilibrium shape is determined by calculating the changes in surface energies with potential for low-index platinum facets; (111), (100) and (110). This has been done by explicitly taking the coverage of oxygenated species into account. A kinetic model derived from counting the number of sites shows that the theoretical activity obtained for equilibrium particle fits well with experimental data. Particles with ~3 nm diameter are found to possess the highest activity. Graphical Abstract The influence of particle size and shape on the activity of platinum nanoparticles for oxygen reduction reaction has been assessed by means of modelling using the surface free energies of low-indexed platinum facets at 0.9 V. The input data for modelling are obtained from density functional theory calculations.

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Research paper thumbnail of Titelbild: Changing the Activity of Electrocatalysts for Oxygen Reduction by Tuning the Surface Electronic Structure (Angew. Chem. 18/2006)

Angewandte Chemie, 2006

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Research paper thumbnail of Cover Picture: Changing the Activity of Electrocatalysts for Oxygen Reduction by Tuning the Surface Electronic Structure (Angew. Chem. Int. Ed. 18/2006)

Angewandte Chemie International Edition, 2006

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Research paper thumbnail of Scaling Relationships for Adsorption Energies on Transition Metal Oxide, Sulfide, and Nitride Surfaces

Angewandte Chemie International Edition, 2008

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Research paper thumbnail of A Flexible Theory for Catalysis: Learning Alkaline Oxygen Reduction on Complex Solid Solutions within the Ag-Pd-Pt-Ru Composition Space

Compositionally complex materials such as high-entropy alloys and oxides have the potential to be... more Compositionally complex materials such as high-entropy alloys and oxides have the potential to be efficient platforms for catalyst discovery because of the vast chemical space spanned by these novel materials. Identifying the composition of the most active catalyst materials, however, requires unraveling the descriptor-activity relationship, as experimental screening the multitude of possible element ratios quickly becomes a daunting task. In this work, we show that inferred adsorption energy distributions of *OH and *O on complex solid solution surfaces within the space spanned by the system Ag-Pd-Pt-Ru are coupled to the experimentally observed electrocatalytic performance for the oxygen reduction reaction. In total, the catalytic activity of 1582 alloy compositions is predicted with a cross-validated mean absolute error of 0.042 mA/cm2 by applying a theory-derived model with only two adjustable parameters. Trends in the discrepancies between predicted electrochemical performance ...

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Research paper thumbnail of Theoretical Trends in Particle Size Effects for the Oxygen Reduction Reaction

Zeitschrift für Physikalische Chemie, 2007

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Research paper thumbnail of Enzymatic versus Inorganic Oxygen Reduction Catalysts: Comparison of the Energy Levels in a Free-Energy Scheme

Inorganic Chemistry, 2010

Bookmarks Related papers MentionsView impact

Research paper thumbnail of Steady state oxygen reduction and cyclic voltammetry

Faraday Discussions, 2009

The catalytic activity of Pt and Pt3Ni for the oxygen reduction reaction is investigated by apply... more The catalytic activity of Pt and Pt3Ni for the oxygen reduction reaction is investigated by applying a Sabatier model based on density functional calculations. We investigate the role of adsorbed OH on the activity, by comparing cyclic voltammetry obtained from theory with previously published experimental results with and without molecular oxygen present. We find that the simple Sabatier model predicts both the potential dependence of the OH coverage and the measured current densities seen in experiments, and that it offers an understanding of the oxygen reduction reaction (ORR) at the atomic level. To investigate kinetic effects we develop a simple kinetic model for ORR. Whereas kinetic corrections only matter close to the volcano top, an interesting outcome of the kinetic model is a first order dependence on the oxygen pressure. Importantly, the conclusion obtained from the simple Sabatier model still persists: an intermediate binding of OH corresponds to the highest catalytic activity, i.e. Pt is limited by a too strong OH binding and Pt3Ni is limited by a too weak OH binding.

Bookmarks Related papers MentionsView impact

Research paper thumbnail of Prediction of solid oxide fuel cell cathode activity with first-principles descriptors

Energy & Environmental Science, 2011

ABSTRACT

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Research paper thumbnail of Oxidative trends of TiO2—hole trapping at anatase and rutile surfaces

Energy & Environmental Science, 2012

ABSTRACT Understanding the nature of photogenerated carriers in a photocatalyst is central to und... more ABSTRACT Understanding the nature of photogenerated carriers in a photocatalyst is central to understanding its photocatalytic performance. Based on density functional theory calculation we show that for TiO2, the most popular photo-catalyst, the electron hole self-trapping leads to band gap states which position is dependent on the type of surface termination. Such variations in hole state energies can lead to differences in photocatalytic activity among rutile and anatase surface facets. We find that the calculated hole state energies correlate with photo-deposition and photo-etching rates. We anticipated that our results can aid the design of more reactive photo-catalysts based on TiO2 and our approach can be utilized for other relevant photo-catalysts as well.

Bookmarks Related papers MentionsView impact

Research paper thumbnail of Bifunctional anode catalysts for direct methanol fuel cells

Energy & Environmental Science, 2012

ABSTRACT Using the binding energy of OH* and CO* on close-packed surfaces as reactivity descripto... more ABSTRACT Using the binding energy of OH* and CO* on close-packed surfaces as reactivity descriptors, we screen bulk and surface alloy catalysts for methanol electro-oxidation activity. Using these two descriptors, we illustrate that a good methanol electro-oxidation catalyst must have three key properties: (1) the ability to activate methanol, (2) the ability to activate water, and (3) the ability to react off surface intermediates (such as CO* and OH*). Based on this analysis, an alloy catalyst made up of Cu and Pt should have a synergistic effect facilitating the activity towards methanol electro-oxidation. Using these two reactivity descriptors, a surface PtCu3 alloy is proposed to have the best catalytic properties of the Pt–Cu model catalysts tested, similar to those of a Pt–Ru bulk alloy. To validate the model, experiments on a Pt(111) surface modified with different amounts of Cu adatoms are performed. Adding Cu to a Pt(111) surface increases the methanol oxidation current by more than a factor of three, supporting our theoretical predictions for improved electrocatalysts.

Bookmarks Related papers MentionsView impact

Research paper thumbnail of How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels

Energy & Environmental Science, 2010

ABSTRACT Density functional theory calculations explain copper's unique ability to conver... more ABSTRACT Density functional theory calculations explain copper's unique ability to convert CO2 into hydrocarbons, which may open up (photo-)electrochemical routes to fuels.

Bookmarks Related papers MentionsView impact

Research paper thumbnail of Understanding the electrocatalysis of oxygen reduction on platinum and its alloys

Energy & Environmental Science, 2012

Bookmarks Related papers MentionsView impact

Research paper thumbnail of Trends in oxygen reduction and methanol activation on transition metal chalcogenides

Electrochimica Acta, 2011

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Research paper thumbnail of Electronic hole localization in rutile and anatase TiO2 – Self-interaction correction in Δ-SCF DFT

Chemical Physics Letters, 2011

ABSTRACT We study electronic hole localization in rutile and anatase titanium dioxide by means of... more ABSTRACT We study electronic hole localization in rutile and anatase titanium dioxide by means of Δ-Self-Consistent Field Density Functional Theory. In order to compare stabilities of the localized and the delocalized hole states we introduce a simple correction to the wrong description of the localization processes within DFT. The correction removes the non-linearity of energy for fractional excitations. We show that the self-trapped and the delocalized hole states have comparable stability in rutile TiO2 whereas in anatase the former is favoured. The theoretical prediction of the adiabatic Potential Energy Surfaces for the hole localization compares well with published photoluminescence measurements.

Bookmarks Related papers MentionsView impact

Research paper thumbnail of Modeling the electrified solid–liquid interface

Chemical Physics Letters, 2008

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Research paper thumbnail of Avoiding pitfalls in the modeling of electrochemical interfaces

Chemical Physics Letters, 2013

Bookmarks Related papers MentionsView impact

Research paper thumbnail of Electrolysis of water on (oxidized) metal surfaces

Chemical Physics, 2005

Bookmarks Related papers MentionsView impact

Research paper thumbnail of Modeling of the symmetry factor of electrochemical proton discharge via the Volmer reaction

Catalysis Today, 2013

Bookmarks Related papers MentionsView impact

Research paper thumbnail of Atomic-Scale Modeling of Particle Size Effects for the Oxygen Reduction Reaction on Pt

Catalysis Letters, 2011

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Research paper thumbnail of The Influence of Particle Shape and Size on the Activity of Platinum Nanoparticles for Oxygen Reduction Reaction: A Density Functional Theory Study

Catalysis Letters, 2014

ABSTRACT Abstract We present first principle investigation of the influence of platinum nanoparti... more ABSTRACT Abstract We present first principle investigation of the influence of platinum nanoparticle shape and size on the oxygen reduction reaction activity. We compare the activities of nanoparticles with specific shapes (tetrahedron, octahedron, cube and truncated octahedron) with that of equilibrium particle shape at 0.9 V. Furthermore, the influence of support is assessed by looking at the particles with and without support interactions. The equilibrium shape is determined by calculating the changes in surface energies with potential for low-index platinum facets; (111), (100) and (110). This has been done by explicitly taking the coverage of oxygenated species into account. A kinetic model derived from counting the number of sites shows that the theoretical activity obtained for equilibrium particle fits well with experimental data. Particles with ~3 nm diameter are found to possess the highest activity. Graphical Abstract The influence of particle size and shape on the activity of platinum nanoparticles for oxygen reduction reaction has been assessed by means of modelling using the surface free energies of low-indexed platinum facets at 0.9 V. The input data for modelling are obtained from density functional theory calculations.

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Research paper thumbnail of Titelbild: Changing the Activity of Electrocatalysts for Oxygen Reduction by Tuning the Surface Electronic Structure (Angew. Chem. 18/2006)

Angewandte Chemie, 2006

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Research paper thumbnail of Cover Picture: Changing the Activity of Electrocatalysts for Oxygen Reduction by Tuning the Surface Electronic Structure (Angew. Chem. Int. Ed. 18/2006)

Angewandte Chemie International Edition, 2006

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Research paper thumbnail of Scaling Relationships for Adsorption Energies on Transition Metal Oxide, Sulfide, and Nitride Surfaces

Angewandte Chemie International Edition, 2008

Bookmarks Related papers MentionsView impact