Cerium Dioxide-Induced Abundant Cu + /Cu 0 Sites for Electrocatalytic Reduction of Carbon Dioxide to C 2+ Products

In recent years, the electrochemical reduction of carbon dioxide (CO RR) has made many advances in C production. Cu /Cu site is beneficial for C-C coupling process, but the oxidation state of copper cannot be well maintained during the reaction process, resulting in a decrease in catalyst activity....

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Veröffentlicht in:ChemSusChem 2024-11, p.e202402097
Hauptverfasser: Wang, Yuwen, Wang, Jiajun, Liu, Shuang, Zhang, Xuan, Jin, Lin, Feng, Lanlan, Kong, Demeng, Zhang, Chenxi, Wei, Yajuan, Zhang, Jingbo
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container_title ChemSusChem
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creator Wang, Yuwen
Wang, Jiajun
Liu, Shuang
Zhang, Xuan
Jin, Lin
Feng, Lanlan
Kong, Demeng
Zhang, Chenxi
Wei, Yajuan
Zhang, Jingbo
description In recent years, the electrochemical reduction of carbon dioxide (CO RR) has made many advances in C production. Cu /Cu site is beneficial for C-C coupling process, but the oxidation state of copper cannot be well maintained during the reaction process, resulting in a decrease in catalyst activity. Based on this consideration, in this work, transition metal oxide CeO with a hollow cube structure and oxygen vacancies was introduced to stabilize and increase Cu /Cu active sites (Ce Cu ). The catalyst exhibits excellent CO RR performance, with FE achieving 73.52 % and j >280 mA/cm at 1.26 V (vs. RHE). Ethanol is the main C product and FE reaches 39 % at 1.26 V. The experimental results indicate that the presence of CeO provides a large number of oxygen vacancies and forming Cu -O -Ce structure by the strong interaction of CeO and Cu NPs. The structure of Cu -O -Ce and abundant oxygen vacancies lay a good foundation for the CO adsorption. Moreover, it increases the content of Cu /Cu sites, effectively inhibiting hydrogen evolution reaction, promoting the C-C coupling interaction, thereby facilitating the generation of C products. The DFT theoretical calculation further demonstrates that Ce Cu is more inclined towards the ethanol pathway, confirming its high selectivity for ethanol.
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Cu /Cu site is beneficial for C-C coupling process, but the oxidation state of copper cannot be well maintained during the reaction process, resulting in a decrease in catalyst activity. Based on this consideration, in this work, transition metal oxide CeO with a hollow cube structure and oxygen vacancies was introduced to stabilize and increase Cu /Cu active sites (Ce Cu ). The catalyst exhibits excellent CO RR performance, with FE achieving 73.52 % and j &gt;280 mA/cm at 1.26 V (vs. RHE). Ethanol is the main C product and FE reaches 39 % at 1.26 V. The experimental results indicate that the presence of CeO provides a large number of oxygen vacancies and forming Cu -O -Ce structure by the strong interaction of CeO and Cu NPs. The structure of Cu -O -Ce and abundant oxygen vacancies lay a good foundation for the CO adsorption. Moreover, it increases the content of Cu /Cu sites, effectively inhibiting hydrogen evolution reaction, promoting the C-C coupling interaction, thereby facilitating the generation of C products. 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title Cerium Dioxide-Induced Abundant Cu + /Cu 0 Sites for Electrocatalytic Reduction of Carbon Dioxide to C 2+ Products
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