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

Vandung Dao, Hyuk Choi, Sunny Yadav, Juan D. Jiménez, Chiyeop Kim, Tuan Van Nguyen, Kai Chen, Periyayya Uthirakumar, Quyet Van Le, Sanjaya D. Senanayake, Hyun You Kim, In Hwan Lee

Research output: Contribution to journalArticlepeer-review

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 10 mA cm−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%). 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.

Original languageEnglish
Article number123452
JournalApplied Catalysis B: Environmental
Volume343
DOIs
Publication statusPublished - 2024 Apr

Bibliographical note

Publisher Copyright:
© 2023 Elsevier B.V.

Keywords

  • Hydrogen evolution reaction
  • LaCeO
  • N-doped graphene
  • Ruthenium
  • Single-atoms

ASJC Scopus subject areas

  • Catalysis
  • General Environmental Science
  • Process Chemistry and Technology

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