In Operando Identification of In Situ Formed Metalloid Zincδ+ Active Sites for Highly Efficient Electrocatalyzed Carbon Dioxide Reduction
In Operando Identification of In Situ Formed Metalloid Zincδ+ Active Sites for Highly Efficient Electrocatalyzed Carbon Dioxide Reduction
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DOI：
10.1002/anie.202202298
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Yang Hua Gui
中科院分区：
文献类型：
--
作者：
Zhang Xin Yu;Li Wen Jing;Chen Jiacheng;Wu Xue Feng;Liu Yuan Wei;Mao Fangxin;Yuan Hai Yang;Zhu Minghui;Dai Sheng;Wang Hai Feng;Hu P;Sun Chenghua;Liu Peng Fei;Yang Hua Gui
Electrochemical CO2 -to-CO conversion provides a possible way to address problems associated with the greenhouse effect; however, developing low-cost electrocatalysts to mediate high-efficiency CO2 reduction remains a challenge on account of the limited understanding of the nature of the real active sites. Herein, we reveal the Znδ+ metalloid sites as the real active sites of stable nonstoichiometric ZnOx structure derived from Zn2 P2 O7 through operando X-ray absorption fine structure analysis in conjunction with evolutionary-algorithm-based global optimization. Furthermore, theoretical and experimental results demonstrated that Znδ+ metalloid active sites could facilitate the activation of CO2 and the hydrogenation of CO2 , thus accelerating the CO2 -to-CO conversion. Our work establishes a critical fundamental understanding of the origin of the real active center in the zinc-based electrocatalysts for CO2 reduction reaction.
