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LaCeOx coupled N-doped graphene/Ru single-atoms as a binary-site catalyst for efficient hydrogen evolution based on hydrogen spillover
Abstract
Based on the hydrogen spillover effect, versatile binary-site catalysts are promising for the alkaline hydrogen evolution reaction (HER). In which one site can adsorb and dissociate water, while the neighboring site is favorable for liberating hydrogen. Inspired by these possibilities, oxygen vacancy (Ov)-rich LaCeOx coupled N-doped graphene/Ru single-atoms (LaCeOx @NGr/Ru1) was synthesized as an efficient dual-site HER catalyst. It delivered an impressive low overpotential of 22 mV at a current density of 10mAcm–2 and a slight Tafel slope of 40 mV dec–1 in an alkaline medium, outstanding the advanced Ru-based catalysts. Moreover, this promising binary-component catalyst exhibited higher mass activity and longer lasting durability than commercial Pt/C catalyst (20 wt%). Finally, experimental and theoretical investigations provided insights into the HER mechanisms of LaCeOx @NGr/Ru1 based on three indispensable steps: water adsorption and dissociation on Ov-rich LaCeOx, diffusion of generated H* species towards Ce3+-N-Ru1 bridges, and hydrogen evolution on Ru1 sites.
- Authors:
-
[2];
[4];
[3];
[3];
[3]
- Korea Univ., Seoul, (Korea, Republic of); Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Chungnam National Univ., Daejeon (Korea, Republic of)
- Korea Univ., Seoul, (Korea, Republic of)
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 2281333
- Report Number(s):
- BNL-225160-2024-JAAM
Journal ID: ISSN 0926-3373
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Applied Catalysis. B, Environmental
- Additional Journal Information:
- Journal Volume: 343; Journal ID: ISSN 0926-3373
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Hydrogen evolution reaction; LaCeOx; N-doped graphene; Ruthenium; Single-atoms
Citation Formats
Dao, Vandung, Choi, Hyuk, Yadav, Sunny, Jiménez, Juan D., Kim, Chiyeop, Van Nguyen, Tuan, Chen, Kai, Uthirakumar, Periyayya, Van Le, Quyet, Senanayake, Sanjaya D., Kim, Hyun You, and Lee, In-Hwan. LaCeOx coupled N-doped graphene/Ru single-atoms as a binary-site catalyst for efficient hydrogen evolution based on hydrogen spillover. United States: N. p., 2023.
Web. doi:10.1016/j.apcatb.2023.123452.
Dao, Vandung, Choi, Hyuk, Yadav, Sunny, Jiménez, Juan D., Kim, Chiyeop, Van Nguyen, Tuan, Chen, Kai, Uthirakumar, Periyayya, Van Le, Quyet, Senanayake, Sanjaya D., Kim, Hyun You, & Lee, In-Hwan. LaCeOx coupled N-doped graphene/Ru single-atoms as a binary-site catalyst for efficient hydrogen evolution based on hydrogen spillover. United States. https://doi.org/10.1016/j.apcatb.2023.123452
Dao, Vandung, Choi, Hyuk, Yadav, Sunny, Jiménez, Juan D., Kim, Chiyeop, Van Nguyen, Tuan, Chen, Kai, Uthirakumar, Periyayya, Van Le, Quyet, Senanayake, Sanjaya D., Kim, Hyun You, and Lee, In-Hwan. Thu .
"LaCeOx coupled N-doped graphene/Ru single-atoms as a binary-site catalyst for efficient hydrogen evolution based on hydrogen spillover". United States. https://doi.org/10.1016/j.apcatb.2023.123452.
@article{osti_2281333,
title = {LaCeOx coupled N-doped graphene/Ru single-atoms as a binary-site catalyst for efficient hydrogen evolution based on hydrogen spillover},
author = {Dao, Vandung and Choi, Hyuk and Yadav, Sunny and Jiménez, Juan D. and Kim, Chiyeop and Van Nguyen, Tuan and Chen, Kai and Uthirakumar, Periyayya and Van Le, Quyet and Senanayake, Sanjaya D. and Kim, Hyun You and Lee, In-Hwan},
abstractNote = {Based on the hydrogen spillover effect, versatile binary-site catalysts are promising for the alkaline hydrogen evolution reaction (HER). In which one site can adsorb and dissociate water, while the neighboring site is favorable for liberating hydrogen. Inspired by these possibilities, oxygen vacancy (Ov)-rich LaCeOx coupled N-doped graphene/Ru single-atoms (LaCeOx @NGr/Ru1) was synthesized as an efficient dual-site HER catalyst. It delivered an impressive low overpotential of 22 mV at a current density of 10mAcm–2 and a slight Tafel slope of 40 mV dec–1 in an alkaline medium, outstanding the advanced Ru-based catalysts. Moreover, this promising binary-component catalyst exhibited higher mass activity and longer lasting durability than commercial Pt/C catalyst (20 wt%). Finally, experimental and theoretical investigations provided insights into the HER mechanisms of LaCeOx @NGr/Ru1 based on three indispensable steps: water adsorption and dissociation on Ov-rich LaCeOx, diffusion of generated H* species towards Ce3+-N-Ru1 bridges, and hydrogen evolution on Ru1 sites.},
doi = {10.1016/j.apcatb.2023.123452},
journal = {Applied Catalysis. B, Environmental},
number = ,
volume = 343,
place = {United States},
year = {Thu Nov 02 00:00:00 EDT 2023},
month = {Thu Nov 02 00:00:00 EDT 2023}
}
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