期刊
CHEMCATCHEM
卷 14, 期 18, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.202200538
关键词
Cobalt; Water Oxidation; Regenerable; Stability; Modified carbon cloth
资金
- Futura Foundation
- VR (The Swedish Research Council)
- Swedish National Infrastructure for Computing [SNIC 2020/13-64]
- National Research and Development Agency of Chile - ANID [2018-72190682]
The electrocatalytic activity of a cobalt-containing, water-soluble molecular water oxidation catalyst was reported, and its stability and activity were significantly enhanced by anchoring it onto modified carbon cloth.
The low stability of the electrocatalysts at water oxidation (WO) conditions and the use of expensive noble metals have obstructed large-scale H-2 production from water. Herein, we report the electrocatalytic WO activity of a cobalt-containing, water-soluble molecular WO electrocatalyst [Co-II(mcbp)(OH2)] (1) [mcbp(2-)=2,6-bis(1-methyl-4-(carboxylate)benzimidazol-2-yl)pyridine] in homogeneous conditions (overpotential of 510 mV at pH 7 phosphate buffer) and after anchoring it on pyridine-modified fluorine-doped carbon cloth (PFCC). The formation of cobalt phosphate was identified only after 4 h continuous oxygen evolution in homogeneous conditions. Interestingly, a significant enhancement of the stability and WO activity (current density of 5.4 mA/cm(2) at 1.75 V) was observed for 1 after anchoring onto PFCC, resulting in a turnover (TO) of >3.6x10(3) and average TOF of 0.05 s(-1) at 1.55 V (pH 7) over 20 h. A total TO of >21x10(3) over 8 days was calculated. The electrode allowed regeneration of similar to 85 % of the WO activity electrochemically after 36 h of continuous oxygen evolution.
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