期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 36, 页码 12711-12716出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201907399
关键词
CO2 reduction; electrocatalysis; orbital reordering; single-site catalysts; 2D materials
资金
- National Key Basic Research Program of China [2014CB931801, 2016YFA0200700]
- National Natural Science Foundation of China [21721002, 21475029]
- Frontier Science Key Project of Chinese Academy of Sciences [QYZDJ-SSW-SLH038]
- Strategic Priority Research Program of Chinese Academy of Sciences [XDA09040100]
- K. C. Wong Education Foundation
The single-site catalyst (SSC) characteristic of atomically dispersed active centers will not only maximize the catalytic activity, but also provide a promising platform for establishing the structure-activity relationship. However, arbitrary arrangements of active sites in the existed SSCs make it difficult for mechanism understanding and performance optimization. Now, a well-defined ultrathin SSC is fabricated by assembly of metal-porphyrin molecules, which enables the precise identification of the active sites for d-orbital energy engineering. The activity of as-assembled products for electrocatalytic CO2 reduction is significantly promoted via lifting up the energy level of metal dz2 orbitals, exhibiting a remarkable Faradaic efficiency of 96 % at the overpotential of 500 mV. Furthermore, a turnover frequency of 4.21 s(-1) is achieved with negligible decay over 48 h.
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