期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 140, 期 32, 页码 10270-10281出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b05382
关键词
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资金
- Netherlands Organization for Scientific Research (NWO) [731.015.204 ELECTROGAS]
- Akzo Nobel Chemicals
- Shell Global Solutions
- Magneto Special Anodes (an Evoqua Brand)
- Elson Technologies
The oxygen evolution reaction (OER) and chlorine evolution reaction (CER) are electrochemical processes with high relevance to water splitting for (solar) energy conversion and industrial production of commodity chemicals, respectively. Carrying out the two reactions separately is challenging, since the catalytic intermediates are linked by scaling relations. Optimizing the efficiency of OER over CER in acidic media has proven especially difficult. In this regard, we have investigated the OER versus CER selectivity of manganese oxide (MnOx), a known OER catalyst. Thin films (similar to 5-20 nm) of MnOx were electrodeposited on glassy carbon-supported hydrous iridium oxide (IrOx/GC) in aqueous chloride solutions of pH similar to 0.9. Using rotating ring-disk electrode voltammetry and online electrochemical mass spectrometry, it was found that deposition of MnOx onto IrOx decreases the CER selectivity of the system in the presence of 30 mM Cl- from 86% to less than 7%, making it a highly OER-selective catalyst. Detailed studies of the CER mechanism and ex-situ structure studies using SEM, TEM, and XPS suggest that the MnOx film is in fact not a catalytically active phase, but functions as a permeable overlayer that disfavors the transport of chloride ions.
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