4.6 Article

Confined local oxygen gas promotes electrochemical water oxidation to hydrogen peroxide

期刊

NATURE CATALYSIS
卷 3, 期 2, 页码 125-134

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NATURE RESEARCH
DOI: 10.1038/s41929-019-0402-8

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资金

  1. Rice University
  2. J. Evans Attwell-Welch Postdoctoral Fellowship by the Smalley-Curl Institute
  3. VILLUM FONDEN [9455]
  4. University of Calgary's Canada First Research Excellence Fund Program, the Global Research Initiative in Sustainable Low Carbon Unconventional Resources
  5. US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program

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Electrochemical 2e(-) water oxidation is a promising route for renewable H2O2 production but it suffers from low selectivity due to the competing 4e(-) process. Here the authors demonstrate an interfacial engineering approach where the catalyst is coated with a hydrophobic polymer to confine in situ produced O-2 and promote the 2e(-) pathway. Electrochemical two-electron water oxidation is a promising route for renewable and on-site H2O2 generation as an alternative to the anthraquinone process. However, it is currently restricted by low selectivity due to strong competition from the traditional four-electron oxygen evolution reaction, as well as large overpotential and low production rates. Here we report an interfacial engineering approach, where by coating the catalyst with hydrophobic polymers we confine in situ produced O-2 gas to tune the water oxidation reaction pathway. Using carbon catalysts as a model system, we show a significant increase of the intrinsic H2O-to-H2O2 selectivity and activity compared to that of the pristine catalyst. The maximal H2O2 Faradaic efficiency was enhanced by sixfold to 66% with an overpotential of 640 mV, under which a H2O2 production rate of 23.4 mu mol min(-1) cm(-2) (75.2 mA cm(-2) partial current) was achieved. This approach was successfully extended to nickel metal, demonstrating the wide applicability of our local gas confinement concept.

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