Reversely Trapping Isolated Atoms in High Oxidation State for Accelerating the Oxygen Evolution Reaction Kinetics

Yang Li, Tingting Bo, Shouwei Zuo, Guikai Zhang, Xiaojuan Zhao, Wei Zhou, Xin Wu, Guoxiang Zhao, Huawei Huang, Lirong Zheng, Jing Zhang, Huabin Zhang*, Jian Zhang*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

7 Scopus citations

Abstract

Developing efficient electrocatalysts for the oxygen evolution reaction (OER) is paramount to the energy conversion and storage devices. However, the structural complexity of heterogeneous electrocatalysts makes it a great challenge to elucidate the dynamic structural evolution and OER mechanisms. Here, we develop a controllable atom-trapping strategy to extract isolated Mo atom from the amorphous MoOx-decorated CoSe2 (a-MoOx@CoSe2) pre-catalyst into Co-based oxyhydroxide (Mo-CoOOH) through an ultra-fast self-reconstruction process during the OER process. This conceptual advance has been validated by operando characterizations, which reveals that the initially rapid Mo leaching can expedite the dynamic reconstruction of pre-catalyst, and simultaneously trap Mo species in high oxidation state into the lattice of in situ generated CoOOH support. Impressively, the OER kinetics of CoOOH has been greatly accelerated after the reverse decoration of Mo species, in which the Mo-CoOOH affords a markedly decreased overpotential of 297 mV at the current density of 100 mA cm−2. Density functional theory (DFT) calculations demonstrate that the Co species have been greatly activated via the effective electron coupling with Mo species in high oxidation state. These findings open new avenues toward directly synthesizing atomically dispersed electrocatalysts for high-efficiency water splitting.

Original languageEnglish (US)
Article numbere202309341
JournalAngewandte Chemie - International Edition
Volume62
Issue number41
DOIs
StateAccepted/In press - 2023

Keywords

  • Dynamic Structure Evolutions
  • Mo Single Atom
  • Operando Characterization
  • Oxygen Evolution Reaction
  • Reversely Atom-Trapping Strategy

ASJC Scopus subject areas

  • Catalysis
  • General Chemistry

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