期刊
SMALL
卷 16, 期 23, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202001384
关键词
copper; oxygen reduction reaction; single atoms; unsaturated coordination
类别
资金
- National Natural Science Foundation of China [51873174, 21902150]
- China Industrial Innovation of Key Research and Development Project of Shaanxi Province [2019ZDLGY16-09]
Regulating the coordination environment of atomically dispersed catalysts is vital for catalytic reaction but still remains a challenge. Herein, an ionic exchange strategy is developed to fabricate atomically dispersed copper (Cu) catalysts with controllable coordination structure. In this process, the adsorbed Cu ions exchange with Zn nodes in ZIF-8 under high temperature, resulting in the trapping of Cu atoms within the cavities of the metal-organic framework, and thus forming Cu single-atom catalysts. More importantly, altering pyrolysis temperature can effectively control the structure of active metal center at atomic level. Specifically, higher treatment temperature (900 degrees C) leads to unsaturated Cu-nitrogen architecture (Cu-N-3 moieties) in atomically dispersed Cu catalysts. Electrochemical test indicates atomically dispersed Cu catalysts with Cu-N-3 moieties possess superior oxygen reduction reaction performance than that with higher Cu-nitrogen coordination number (Cu-N-4 moieties), with a higher half-wave potential of 180 mV and the 10 times turnover frequency than that of CuN4. Density functional theory calculation analysis further shows that the low N coordination number of Cu single-atom catalysts (Cu-N-3) is favorable for the formation of O-2* intermediate, and thus boosts the oxygen reduction reaction.
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