Insights into solvent and surface charge effects on Volmer step kinetics on Pt (111)
| Author(s) | Wilson, Jon C. | |
| Author(s) | Caratzoulas, Stavros | |
| Author(s) | Vlachos, Dionisios G. | |
| Author(s) | Yan, Yushan | |
| Date Accessioned | 2023-08-08T17:44:40Z | |
| Date Available | 2023-08-08T17:44:40Z | |
| Publication Date | 2023-04-25 | |
| Description | The version of record of this article, first published in Nature Communications, is available online at Publisher’s website: https://doi.org/10.1038/s41467-023-37935-6. © The Author(s) 2023 | |
| Abstract | The mechanism of pH-dependent hydrogen oxidation and evolution kinetics is still a matter of significant debate. To make progress, we study the Volmer step kinetics on platinum (111) using classical molecular dynamics simulations with an embedded Anderson-Newns Hamiltonian for the redox process and constant potential electrodes. We investigate how negative electrode electrostatic potential affects Volmer step kinetics. We find that the redox solvent reorganization energy is insensitive to changes in interfacial field strength. The negatively charged surface attracts adsorbed H as well as H+, increasing hydrogen binding energy, but also trapping H+ in the double layer. While more negative electrostatic potential in the double layer accelerates the oxidation charge transfer, it becomes difficult for the proton to move to the bulk. Conversely, reduction becomes more difficult because the transition state occurs farther from equilibrium solvation polarization. Our results help to clarify how the charged surface plays a role in hydrogen electrocatalysis kinetics. | |
| Sponsor | This research used resources of the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility located at Lawrence Berkeley National Laboratory, operated under Contract No. DE-AC02-05CH11231 using NERSC award m1893 for years 2021-2022. This research was supported in part through the use of DARWIN computing system: DARWIN – A Resource for Computational and Data-intensive Research at the University of Delaware and in the Delaware Region, which is supported by NSF under Grant Number: 1919839. This work was supported as part of the Catalysis Center for Energy Innovation, an Energy Frontier Research Center funded by the US Dept. of Energy, Office of Science, Office of Basic Energy Sciences under award number DE-SC0001004. | |
| Citation | Wilson, J.C., Caratzoulas, S., Vlachos, D.G. et al. Insights into solvent and surface charge effects on Volmer step kinetics on Pt (111). Nat Commun 14, 2384 (2023). https://doi.org/10.1038/s41467-023-37935-6 | |
| ISSN | 2041-1723 | |
| URL | https://udspace.udel.edu/handle/19716/33057 | |
| Language | en_US | |
| Publisher | Nature Communications | |
| dc.rights.uri | http://creativecommons.org/licenses/by/4.0/ | |
| Keywords | catalytic mechanisms | |
| Keywords | electrochemistry | |
| Keywords | energy | |
| Keywords | reaction mechanisms | |
| Title | Insights into solvent and surface charge effects on Volmer step kinetics on Pt (111) | |
| Type | Article |
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