期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 305, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121082
关键词
Nickel sulfide; Anode-cathode exchange; Stable electrocatalysis; Hydrogen generation; Active sites recovery
资金
- National Natural Science Foundation of China [21805187, 21975163]
- Shenzhen Science and Technology Program [KQTD20190929173914967, JCYJ20200109110416441]
A unique anode-cathode interchangeable electrocatalysis strategy is proposed for methanol upgrading reaction (MUR) and hydrogen co-generation in membrane-free electrolyzer, which achieves excellent long-term stability and high Faradaic efficiencies.
Surface re-construction was a common phenomenon for non-oxide compound electrocatalysts in anodic oxidation reaction in alkaline electrolyte but surface deactivation arising from excessive oxidation/hydroxylation was critical hindrance to the long-term stability. Herein, a unique anode-cathode interchangeable electrocatalysis strategy is proposed for methanol upgrading reaction (MUR) and hydrogen co-generation in membrane-free electrolyzer. A periodical electrolysis is taken place for the Ni3S2/CNTs electrode at positive/negative currents over time. Compared with the traditional chronopotentiometry mode, the MUR-HER coupled reactions by periodically switching anode/cathode per hour present an excellent long-term stability at high current densities of & PLUSMN; 100 mA cm(-2), in which the Faradaic efficiencies for both H-2 and value-added formate are greater than 95%. Substantial experimental results and deep theoretical DFT studies signify that the successful application of this strategy is mainly due to the reversible modulation of oxidation/hydroxylation status on Ni3S2 surface, which effectively prevent the surface active structures of electrocatalysts from over-oxidation.
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