Nature-Inspired Design of Molybdenum–Selenium Dual-Single-Atom Electrocatalysts for CO2 Reduction

Kaian Sun; Ke Yu; Jinjie FangZewen ZhuangXin TanYue WuLingyou ZengZhongbin ZhuangYuan PanChen Chen

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Nature-Inspired Design of Molybdenum–Selenium Dual-Single-Atom Electrocatalysts for CO2 Reduction

机译：Nature-Inspired Design of Molybdenum–Selenium Dual-Single-Atom Electrocatalysts for CO2 Reduction

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Electrochemical CO_2 reduction (ECR) is becoming an increasingly important technology for achieving carbon neutrality. Inspired by the structure of naturally occurring Mo-dependent enzymes capable of activating CO_2, a heteronuclear Mo–Se dual-single-atom electrocatalyst (MoSA–SeSA) for ECR into CO with a Faradaic efficiency of above 90 over a broad potential window from ?0.4 to ?1.0 V versus reversible hydrogen electrode is demonstrated here. Both operando characterization and theoretical simulation results verify that MoSA acts as central atoms that directly interact with the ECR feedstock and intermediates, whereas the SeSA adjacent to MoSA modulates the electronic structure of MoSA through long-range electron delocalization for inhibiting MoSA poisoning caused by strong CO adsorption. In addition, the SeSAs far from MoSA help suppress the competing hydrogen evolution side reaction and accelerate the CO_2 transport by repelling H_2O. This work provides new insight into the precise regulation and in-depth understanding of multisite synergistic catalysis at the atomic scale.

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《Advanced Materials》 |2022年第44期|2206478.1-2206478.10|共10页
作者
Kaian Sun; Ke Yu; Jinjie FangZewen ZhuangXin TanYue WuLingyou ZengZhongbin ZhuangYuan PanChen Chen;
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Department of Chemistry Tsinghua University Beijing 100084, P. R. China,State Key Laboratory of Heavy Oil Processing China University of Petroleum (East China) Qingdao 266580, P. R. China;

Department of Chemistry Tsinghua University Beijing 100084, P. R. China;

Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029, P. R. ChinaState Key Laboratory of Heavy Oil Processing China University of Petroleum (East China) Qingdao 266580, P. R. ChinaDepartment of Chemistry Tsinghua University Beijing 100084, P. R. China,Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029, P. R. China;

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carbon dioxide reduction; dual single-atoms; electrocatalysts;

Nature-Inspired Design of Molybdenum–Selenium Dual-Single-Atom Electrocatalysts for CO2 Reduction

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