Stabilizing indium sulfide for CO2 electroreduction to formate at high rate by zinc incorporation

Li-Ping Chi, Zhuang-Zhuang Niu, Xiao-Long Zhang, Peng-Peng Yang, Jie Liao, Fei-Yue Gao, Zhi-Zheng Wu, Kai-Bin Tang () and Min-Rui Gao ()
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Li-Ping Chi: University of Science and Technology of China
Zhuang-Zhuang Niu: University of Science and Technology of China
Xiao-Long Zhang: University of Science and Technology of China
Peng-Peng Yang: University of Science and Technology of China
Jie Liao: University of Science and Technology of China
Fei-Yue Gao: University of Science and Technology of China
Zhi-Zheng Wu: University of Science and Technology of China
Kai-Bin Tang: University of Science and Technology of China
Min-Rui Gao: University of Science and Technology of China

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Recently developed solid-state catalysts can mediate carbon dioxide (CO2) electroreduction to valuable products at high rates and selectivities. However, under commercially relevant current densities of > 200 milliamperes per square centimeter (mA cm−2), catalysts often undergo particle agglomeration, active-phase change, and/or element dissolution, making the long-term operational stability a considerable challenge. Here we report an indium sulfide catalyst that is stabilized by adding zinc in the structure and shows dramatically improved stability. The obtained ZnIn2S4 catalyst can reduce CO2 to formate with 99.3% Faradaic efficiency at 300 mA cm−2 over 60 h of continuous operation without decay. By contrast, similarly synthesized indium sulfide without zinc participation deteriorates quickly under the same conditions. Combining experimental and theoretical studies, we unveil that the introduction of zinc largely enhances the covalency of In-S bonds, which “locks” sulfur—a catalytic site that can activate H2O to react with CO2, yielding HCOO* intermediates—from being dissolved during high-rate electrolysis.

Date: 2021
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DOI: 10.1038/s41467-021-26124-y

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