B4: Theoretical studies on the interaction of excited species with catalyst surfaces

Principal Investigators: T. Jacob

Team

Jacob, Timo (Principal Investigator)

Anton, Josef (Staff)

Description

The aim of this project is to develop a theoretical understanding of surface/plasma interfaces on an atomistic scale. As this involves effects on different time- and length-scales that have to be addressed, a multiscale-approach is developed and adapted that connects quantum-mechanics, molecular dynamics, kinetic Monte-Carlo and thermodynamics in order to investigate the morphology as well as processes at the surface/plasma interface, especially concentrating on plasma-electrolytic reactions. Consequently, the project involves a method development as well as an application part. Regarding the application, we aim at resolving the structure–plasma–activity relationship for plasma-assisted catalytic reactions involving CO2 reduction, the n-butane oxidation and the ammonia synthesis. By varying the plasma parameters in our simulations, we might even be able to optimize the plasma conditions for particular reactions.

Publications

• Understanding the Nitrogen Reduction Reaction Mechanism on CuFeO₂ Photocathodes
  J. Beßner, T. Jacob
  Chem. Eur. J., e202500058 (2025)
  
• In silico characterization of nanoparticles
  B. Kirchhoff, C. K. Jung, D. Gaissmaier, L. Braunwarth, D. Fantauzzia, T. Jacob
  Phys. Chem. Chem. Phys. 25, 13228-13243 (2023)
  
• Metal deposition and electrocatalysis for elucidating structural changes of gold electrodes during cathodic corrosion
  M. M. Elnagar, L. Kibler, T. Jacob
  Green Chem. 25, 6238 (2023)
  
• An Atomistic View of Platinum Cluster Growth on Pristine and Defective Graphene Supports
  J. Bord, B. Kirchhoff, M. Baldofski, C. K. Jung, T. Jacob
  Small 19, 2207484 (2023)
  
• Potential-Dependent Pt(111)/Water Interface: Tackling the Challenge of a Consistent Treatment of Electrochemical Interfaces
  L. Braunwarth, C. K. Jung, T. Jacob
  Chem. Phys. Chem. 24, e202200336 (2023)
  
• An increase in surface hydrophobicity mediates chaperone activity in N-chlorinated RidA
  M. Varatnitskaya, J. Fasel, A. Müller, N. Lupilov, Y. Shi, K. Fuchs, M. Krewing, C. K. Jung, T. Jacob, B. Sitek, J. E. Bandow, K. S. Carroll, E. Hofmann, L. I. Leichert
  Redox Biol. 53, 102332 (2022)
  
• Simulations of the Electrochemical Oxidation of Pt Nanoparticles of Various Shapes
  B. Kirchhoff, C. K. Jung, H. Jonsson, D. Fantauzzi, T. Jacob
  J. Phys. Chem. C 126, 6773 (2022)
  
• Atmospheric Pressure Plasma-Jet Treatment of PAN-Nonwovens - Activation Leading to High Surface Area Carbon Electrodes
  A. Hoffmann, M. Uhl, M. Ceblin, J. Bansmann, T. Jacob, A. J. C. Kühne
  Plasma Process. Polym. 19, e2200114 (2022)
  
• Atmospheric Pressure Plasma-Jet Treatment of Polyacrylonitrile-Nonwovens - Stabilization and Roll-to-Roll Processing
  A. Hoffmann, F. Rohrbach, M. Uhl, M. Ceblin, T. Bauer, M. Mallah, T. Jacob, H. Heuermann, A. J. C. Kühne
  J. Appl. Polym. Sci. 139, e52887 (2022)
  
• Inductive Heating for Research in Electrocatalysis: Theory, Practical Considerations and Examples
  D. Esau, F. Schütt, K. L. Varvaris, L. A. Kibler, Ludwig, T. Jacob, G. Jerkiewicz
  ACS Catal. 12, 9766 (2022)
  
• Atmospheric Pressure Plasma-Jet Treatment of PAN-Nonwovens - Carbonization of Nanofiber Electrodes
  A. Hoffmann, M. Uhl, M. U. Ceblin, F. Rohrbach, J. Bansmann, M. Mallah, H. Heuermann, T. Jacob, A. J. C. Kühne
  C 8, 33 (2022)
  
• Plasma Electrolytic Oxidation (PEO) Process—Processing, Properties, and Applications
  S. Sikdar, P. V. Menezes, R. Maccione, T. Jacob, P. L. Menezes
  Nanomater. 11, 1375 (2021)
  
• Structural evolution of a PtRu catalyst in the oxidation of an organic molecule
  J. E. Mueller, H. Hoffmannová, T. Hiratoko, P. Krtil, T. Jacob
  J. Catal. 398, 89 - 101 (2021)
  
• Influence of surface states on the conductance spectra for Co adsorbed on Cu(111)
  M. S. Tacca, T. Jacob, E. C. Goldberg
  Phys. Rev. B 103, 245419 (2021)
  
• Elastic Collision Based Dynamic Partitioning Scheme for Hybrid Simulations
  B.Kirchhoff, E. Ö. Jónsson, A. O. Dohn, T. Jacob, H. Jónsson
  J. Chem. Theory Comput. 17, 5863–5875 (2021)
  
• The Effect of pH and Anion Adsorption on Formic Acid Oxidation on Au(111) Electrodes
  J. M. Hermann, A. Abdelrahman, T. Jacob, L. A. Kibler
  Electrochim. Acta 385, 138279 (2021)
  
• Thermodynamic Description of Interfaces Applying the 2PT Method on ReaxFF Molecular Dynamics Simulations
  C. K. Jung, L. Braunwarth, A. Sinyavskiy, T. Jacob
  Phys. Rev. B 103, 245419 (2021)
  
• Dielectric barrier discharge plasma treatment affects stability, metal ion coordination, and enzyme activity of bacterial superoxide dismutases
  M. Krewing, C. K. Jung, E. Dobbelstein, B. Schubert, T. Jacob, J. E. Bandow
  Plasma Process. Polym. 17, e2000019 (2020)
  
• Controlled Atmosphere Flame Fusion Single Crystal Growth of non-noble fcc, hcp and bcc metals using Copper, Cobalt and Iron
  F. M. Schütt, D. Esau, K. Liam Varvaris, S. Gelman, J. Björk, J. Rosen, G. Jerkiewicz, T. Jacob
  Angew. Chem. Int. Ed. 59, 13246-13252 (2020)
  
• Controlled-Atmosphere Flame Fusion Growth of Nickel Poly-oriented Spherical Single Crystals - Unravelling Decades of Impossibility
  D. Esau, F. M. Schütt, K. L. Vavaris, J. Björk, T. Jacob, G. Jerkiewicz
  Electrocatalysis 11, 1-13 (2020)
  
• Exploring the Structure-Activity Relationship on Platinum Nanoparticles
  L. Braunwarth, C. K. Jung, T. Jacob
  Topics Catal. 63, 1647 (2020)
  
• Simulations of the Oxidation and Degradation of Platinum Electrocatalysts
  B. Kirchhoff, L. Braunwarth, C. K. Jung, H. Jonsson, D. Fantauzzi, T. Jacob
  Small 16, 1905159 (2020)
  
• Grand Canonical ReaxFF Molecular Dynamics Simulations for Catalytic Reactions
  C. K. Jung, L. Braunwarth, T. Jacob
  Chem. Theory Comput. 15, 5810-5816 (2019)
  

Thesis

• Simon Homann, PhD thesis - 12/2024
  Theoretical studies on the interaction of excited species with catalyst surfaces

Further reading

• Theoretical Studies of Potential-Dependent and Competing Mechanisms of the Electrocatalytic Oxygen Reduction Reaction on Pt(111)
  J.A. Keith, T. Jacob
  Angew. Chem. Int. Ed. 49, 9521-9525 (2010)