| Autor: |
Arulmozhi, N., Hanselman, S.R, Tudor, V., Chen, X., Velden, D. van, Schneider, G.F., Calle-Vallejo, F., Koper, M.T.M. |
| Jazyk: |
angličtina |
| Rok vydání: |
2023 |
| Předmět: |
|
| Zdroj: |
JACS AU, 3(2), 526-535. AMER CHEMICAL SOC |
| DOI: |
10.1021/jacsau.2c00648 |
| Popis: |
The Angstrom-scale space between graphene and its substrate provides an attractive playground for scientific exploration and can lead to breakthrough applications. Here, we report the energetics and kinetics of hydrogen electrosorption on a graphene-covered Pt(111) electrode using electrochemical experiments, in situ spectroscopy, and density functional theory calculations. The graphene overlayer influences the hydrogen adsorption on Pt(111) by shielding the ions from the interface and weakening the Pt–H bond energy. Analysis of the proton permeation resistance with controlled graphene defect density proves that the domain boundary defects and point defects are the pathways for proton permeation in the graphene layer, in agreement with density functional theory (DFT) calculations of the lowest energy proton permeation pathways. Although graphene blocks the interaction of anions with the Pt(111) surfaces, anions do adsorb near the defects: the rate constant for hydrogen permeation is sensitively dependent on anion identity and concentration. This work received partial support from Hitachi, Ltd. and Hitachi High-Technologies Corporation. This work was also partially supported by the Netherlands Organization for Scientific Research (NWO) in the framework of the Solar Fuels Graduate Program. The grants RYC-2015-18996, MDM-2017-0767, and RTI2018-095460-B-I00 were funded by MCIN/AEI/10.13039/501100011033 and by the European Union. This research was also partly funded by Generalitat de Catalunya 2017SGR13. The computational work has been performed under the Project HPC-EUROPA3 (INFRAIA-2016-1-730897), with the support of the EC Research Innovation Action under the H2020 Programme; in particular, S.H. gratefully acknowledges the support of IQTCUB and the computer resources and technical support provided by BSC. The use of supercomputing facilities at SURFsara was sponsored by NWO Physical Sciences, with financial support by NWO. |
| Databáze: |
OpenAIRE |
| Externí odkaz: |
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