期刊
CHEMICAL SCIENCE
卷 13, 期 44, 页码 13172-13177出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2sc04776d
关键词
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资金
- National Key Research and Development Program of China [2020YFB1505801]
- National Natural Science Foundation of China [22025208, 22075300, 22102191]
- DNL Cooperation Fund, CAS [DNL202008]
- Chinese Academy of Sciences
The introduction of single atomic Mn-N auxiliary sites can effectively enhance the CO2 electroreduction to CO by accelerating the reaction steps and improving the catalyst performance, suggesting a promising strategy for large-scale application.
Electrocatalytic CO2 reduction driven by renewable energy has become a promising approach to rebalance the carbon cycle. Atomically dispersed transition metals anchored on N-doped carbon supports (M-N-C) have been considered as the most attractive catalysts to catalyze CO2 to CO. However, the sluggish kinetics of M-N-C limits the large-scale application of this type of catalyst. Here, it is found that the introduction of single atomic Mn-N auxiliary sites could effectively buffer the locally generated OH- on the catalytic interface of the single-atomic Ni-N-C sites, thus accelerating proton-coupled electron transfer (PCET) steps to enhance the CO2 electroreduction to CO. The constructed diatomic Ni/Mn-N-C catalysts show a CO faradaic efficiency of 96.6% and partial CO current density of 13.3 mA cm(-2) at -0.76 V vs. RHE, outperforming that of monometallic single-atomic Ni-N-C or Mn-N-C counterparts. The results suggest that constructing synergistic catalytic sites to regulate the surface local microenvironment might be an attractive strategy for boosting CO2 electroreduction to value-added products.
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