Ru-loaded pyrrolic-N-doped extensively graphitized porous carbon for high performance electrochemical hydrogen evolution
Abstract
Herein, we report a novel methodology for preparation of new N-doped extensively graphitized porous carbon (N-GPC) as a new catalyst support for Ru nanoparticles (NPs) with dramatically improved hydrogen evolution reaction (HER) activity. Our method is remarkably simple: pyrolyzing g-C3N4 in the presence of Mg metal. Here, we show that Mg plays marvelous dual roles as a reducing agent to graphitize the g-C3N4 precursor at low temperature and as a precursor for Mg3N2, which generates network-structured porous carbon as a new porogen. This offers highly robust graphitized carbon with high electrical conductivity, network-structured high porosity, and proper N content, most desired as a catalyst support. As-prepared Ru/N-GPC catalyst shows a remarkably low overpotential of 9.6 mV (vs. RHE) at 10 mA/cm2, which is near ideal, providing 12 times faster hydrogen production rate than state-of-the-art Pt/C. We explain the atomistic basis for this low overpotential and superb stability via Grand canonical quantum mechanics calculations. These calculations show that pyrrolic-N in the support strengthens the coupling to the Ru NP while weakening the binding of H to Ru NP to accelerate the Tafel step.
Additional Information
© 2023 Elsevier. This work was generously supported by the National Research Foundation (2019R1A2C2086770 and 2023K2A9A2A23000259) funded by the Korea Ministry of Science, ICT & Future Planning. Authors would also like to thank the Korean Basic Science Institute (KBSI) at Jeonju and Daejeon for electron microscope analysis. T.H.Y., S.K., and W.A.G. thank ONR (N00014–19-1–2081) for support. The computations presented here were conducted in the Resnick High Performance Center, a facility supported by Resnick Sustainability Institute. CRediT authorship contribution statement. Cheol-Hwan Shin: Conceptualization, Methodology, Investigation, Formal analysis, Visualization, Writing – original draft, Writing – review & editing. Ted H. Yu: Formal analysis, Methodology, Visualization, Writing – original draft. Ha-Young Lee: Formal analysis, Data curation. Byeong-June Lee: Formal analysis, Data curation. Soonho Kwon: Formal analysis, Data curation. William A. Goddard III: Project administration, Funding acquisition, Conceptualization, Supervision, Writing – review & editing. Jong-Sung Yu: Project administration, Funding acquisition, Conceptualization, Supervision, Writing – review & editing. Data Availability. Data will be made available on request. Computational data were uploaded to github: https://github.com/tedhyu/Ru_HER. The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Jong-Sung Yu reports financial support was provided by National Research Foundation of Korea. Jong-Sung Yu reports a relationship with National Research Foundation of Korea that includes: funding grants. The authors declare that they have no other known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.Additional details
- Eprint ID
- 121756
- Resolver ID
- CaltechAUTHORS:20230607-309304000.1
- National Research Foundation of Korea
- 2019R1A2C2086770
- National Research Foundation of Korea
- 2023K2A9A2A23000259
- Ministry of Science, ICT and Future Planning (Korea)
- Office of Naval Research (ONR)
- N00014–19-1–2081
- Resnick Sustainability Institute
- Created
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2023-06-08Created from EPrint's datestamp field
- Updated
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2023-06-09Created from EPrint's last_modified field
- Caltech groups
- Resnick Sustainability Institute
- Other Numbering System Name
- WAG
- Other Numbering System Identifier
- 1573