Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 31, Issue 47, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202104716
Keywords
carbon free; earth abundant; hydrogen peroxide; oxygen reduction; selective electrocatalysis
Categories
Funding
- Northern Illinois University
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357., DOE DE-FG02-03ER15457]
- Institute for Catalysis in Energy Processes (ICEP) at Northwestern U
- SHyNE Resource (NSF) [ECCS-2025633]
- MRSEC program (NSF) [DMR-1720139]
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The Chevrel phase chalcogenide Ni2Mo6S8 is a novel active motif for reducing oxygen to H2O2, exhibiting exceptional activity with high selectivity, fast turnover frequencies, and stable crystal structure for continuous H2O2 production.
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 g(cat)(-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 O-2 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 approximate to 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.
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