Visible-light-switched electron transfer over single porphyrin-metal atom center for highly selective electroreduction of carbon dioxide

Deren Yang, Hongde Yu, Ting He, Shouwei Zuo, Xiaozhi Liu, Haozhou Yang, Bing Ni, Haoyi Li, Lin Gu, Dong Wang and Xun Wang ()
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Deren Yang: Tsinghua University
Hongde Yu: Tsinghua University
Ting He: Tsinghua University
Shouwei Zuo: Institute of High Energy Physics, Chinese Academy of Sciences
Xiaozhi Liu: Institute of Physics, Chinese Academy of Sciences
Haozhou Yang: Tsinghua University
Bing Ni: Tsinghua University
Haoyi Li: Tsinghua University
Lin Gu: Institute of Physics, Chinese Academy of Sciences
Dong Wang: Tsinghua University
Xun Wang: Tsinghua University

Nature Communications, 2019, vol. 10, issue 1, 1-10

Abstract: Abstract External fields are introduced to catalytic processes to improve catalytic activities. The light field effect plays an important role in electrocatalytic processes, but is not fully understood. Here we report a series of photo-coupled electrocatalysts for CO2 reduction by mimicking the structure of chlorophyll. The porphyrin-Au catalyst exhibits a high turnover frequency of 37,069 h−1 at −1.1 V and CO Faradaic efficiency (FE) of 94.2% at −0.9 V. Under visible light, the electrocatalyst reaches similar turnover frequency and FE with potential reduced by ~ 130 mV. Interestingly, the light-induced positive shifts of 20, 100, and 130 mV for porphyrin-Co, porphyrin-Cu, and porphyrin-Au electrocatalysts are consistent with their energy gaps of 0, 1.5, and 1.7 eV, respectively, suggesting the porphyrin not only serves as a ligand but also as a photoswitch to regulate electron transfer pathway to the metal center.

Date: 2019
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DOI: 10.1038/s41467-019-11817-2

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