LaCeOx coupled N-doped graphene/Ru single-atoms as a binary-site catalyst for efficient hydrogen evolution based on hydrogen spillover

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

doi:10.1016/j.apcatb.2023.123452

Title: LaCeO_x coupled N-doped graphene/Ru single-atoms as a binary-site catalyst for efficient hydrogen evolution based on hydrogen spillover

Journal Article · 01 November 2023 · Applied Catalysis. B, Environmental

DOI: https://doi.org/10.1016/j.apcatb.2023.123452 · OSTI ID:2281333

Dao, Vandung ^[1];

^[2]; Yadav, Sunny ^[3];

^[4]; Kim, Chiyeop ^[3];

^[3]; Chen, Kai ^[3];

^[3]; Van Le, Quyet ^[3]; Senanayake, Sanjaya D. ^[4]; Kim, Hyun You ^[2];

^[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)

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 (O_v)-rich LaCeO_x coupled N-doped graphene/Ru single-atoms (LaCeO_x @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 LaCeO_x @NGr/Ru₁ based on three indispensable steps: water adsorption and dissociation on O_v-rich LaCeO_x, diffusion of generated H* species towards Ce³⁺-N-Ru₁ bridges, and hydrogen evolution on Ru₁ sites.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 2281333

Report Number(s):: BNL--225160-2024-JAAM

Journal Information:: Applied Catalysis. B, Environmental, Journal Name: Applied Catalysis. B, Environmental Vol. 343; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
Hydrogen evolution reaction
LaCeOx
N-doped graphene
Ruthenium
Single-atoms

Title: LaCeOx coupled N-doped graphene/Ru single-atoms as a binary-site catalyst for efficient hydrogen evolution based on hydrogen spillover

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References (70)

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Title: LaCeO_x coupled N-doped graphene/Ru single-atoms as a binary-site catalyst for efficient hydrogen evolution based on hydrogen spillover