期刊
ADVANCED MATERIALS INTERFACES
卷 8, 期 8, 页码 -出版社
WILEY
DOI: 10.1002/admi.202001360
关键词
electrode design; hydrogen peroxide; single‐ atom catalysts; sites tailoring; two‐ electron oxygen reduction reaction
资金
- National Natural Science Foundation of China (NSFC)
- National Key Research and Development Project [2018YFB1502401, 2018YFA0702002]
- Royal Society [NAF\R1\191294]
- Newton Fund through the Newton Advanced Fellowship award [NAF\R1\191294]
- Program for Changjiang Scholars and Innovation Research Team in the University [IRT1205]
- Fundamental Research Funds for the Central Universities
- Ministry of Finance
- Ministry of Education of PRC
- China Scholarship Council [201906880018]
By characterizing the methods and reaction mechanisms of ORR via two-electron and four-electron transfer pathways, the role of binding strength between OOH intermediate and active sites in determining the activity and selectivity towards H2O2 production is revealed and illustrated.
Electrochemical reduction of oxygen is considered as a new strategy to achieve decentralized preparation of hydrogen peroxide (H2O2) in a green manner. As a promising new type of catalytic material, carbon-based single-atom catalysts can achieve wide-range adjustments of the electronic structure of the active metal centers while also maximize the utilization of metal atoms, toward electrochemical production of H2O2 from the selective two-electron transfer oxygen reduction reaction (ORR). Herein, starting from the reviewing of characterizing methods and reaction mechanisms of ORR via two-electron and four-electron transfer pathways, the vital role of binding strength between OOH intermediate and active sites in determining the activity and selectivity towards H2O2 production is revealed and illustrated. Currently reported carbon-based single-atom catalysts for H2O2 production are systematically summarized and critically reviewed. Moreover, with the underpinning chemistry to improve the overall efficiency, three aspects concerning the central metal atoms, coordinated atoms, and environmental atoms are comprehensively analyzed. Based on the understanding of the most current progresses, some predictions for future H2O2 production via electrochemical routes are offered, which include catalyst designs at atomic levels, new synthesis strategies and characterization techniques, as well as interfacial superwetting interaction engineering at electrode and device levels.
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