Carbon Free and Noble Metal Free Ni2Mo6S8 Electrocatalyst for Selective Electrosynthesis of H2O2

Fan Xia, Bomin Li, Yiqi Liu, Yuzi Liu, Siyuan Gao, Ke Lu, Jacob Kaelin, Rongyue Wang, Tobin J. Marks, Yingwen Cheng*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

43 Scopus citations

Abstract

Electrocatalytic two-electron reduction of oxygen is a promising method for producing sustainable H2O2 but lacks low-cost and selective electrocatalysts. Here, the Chevrel phase chalcogenide Ni2Mo6S8 is presented as a novel active motif for reducing oxygen to H2O2 in an aqueous electrolyte. Although it has a low surface area, the Ni2Mo6S8 catalyst exhibits exceptional activity for H2O2 synthesis with >90% H2O2 molar selectivity across a wide potential range. Chemical titration verified successful generation of H2O2 and confirmed rates as high as 90 mmol H2O2 gcat−1 h−1. The outstanding activities are attributed to the ligand and ensemble effects of Ni that promote H2O dissociation and proton-coupled reduction of O2 to HOO*, and the spatial effect of the Chevrel phase structure that isolates Ni active sites to inhibit O O cleavage. The synergy of these effects delivers fast and selective production of H2O2 with high turn-over frequencies of ≈30 s−1. In addition, the Ni2Mo6S8 catalyst has a stable crystal structure that is resistive for oxidation and delivers good catalyst stability for continuous H2O2 production. The described Ni-Mo6S8 active motif can unlock new opportunities for designing Earth-abundant electrocatalysts to tune oxygen reduction for practical H2O2 production.

Original languageEnglish (US)
Article number2104716
JournalAdvanced Functional Materials
Volume31
Issue number47
DOIs
StatePublished - Nov 18 2021

Keywords

  • carbon free
  • earth abundant
  • hydrogen peroxide
  • oxygen reduction
  • selective electrocatalysis

ASJC Scopus subject areas

  • General Chemistry
  • General Materials Science
  • Condensed Matter Physics

Fingerprint

Dive into the research topics of 'Carbon Free and Noble Metal Free Ni2Mo6S8 Electrocatalyst for Selective Electrosynthesis of H2O2'. Together they form a unique fingerprint.

Cite this