Selective CO2 Reductionto Ethylene Mediated by Adaptive Small‐molecule Engineering of Copper‐based Electrocatalysts
Selective CO2 Reductionto Ethylene Mediated by Adaptive Small‐molecule Engineering of Copper‐based Electrocatalysts
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DOI：
10.1002/anie.202315621
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发表时间：
2023
期刊：
影响因子：
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通讯作者：
Dingsheng Wang
中科院分区：
文献类型：
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作者：
Shenghua Chen;Chengliang Ye;Ziwei Wang;Peng Li;Wenjun Jiang;Zechao Zhuang;Jiexin Zhu;Xiaobo Zheng;Shahid Zaman;Honghui Ou;Lei Lv;Lin Tan;Yaqiong Su;Jiang Ouyang;Dingsheng Wang
Electrochemical CO2 reduction reaction (CO2RR) over Cu catalysts exhibits enormous potential for efficiently converting CO2 to ethylene (C2H4). However, achieving high C2H4 selectivity remains a considerable challenge due to the propensity of Cu catalysts to undergo structural reconstruction during CO2RR. Herein, we report an in situ molecule modification strategy that involves tannic acid (TA) molecules adaptive regulating the reconstruction of a Cu‐based material to a pathway that facilitates CO2 reduction to C2H4 products. An excellent Faraday efficiency (FE) of 63.6% on C2H4 with a current density of 497.2 mA cm‐2 in flow cell was achieved, about 6.5 times higher than the pristine Cu catalyst which mainly produce CH4. The in situ X‐ray absorption and Raman studies reveal that the hydroxyl group in TA stabilizes Cuδ+ during the CO2RR. Furthermore, theoretical calculations demonstrate that the partially oxidized Cuδ+/Cu0 interfaces lower the activation energy barrier for CO dimerization, and hydroxyl species stabilize the COH intermediate via hydrogen bonding, thereby promoting C2H4 production. Such molecule engineering modulated electronic structure provides a promising strategy to achieve highly selective CO2 reduction to value‐added chemicals.
