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.
Highlights
Developed solid-state catalysts can mediate carbon dioxide (CO2) electroreduction to valuable products at high rates and selectivities
We report that incorporation of zinc (Zn) into indium sulfide (In2S3) synthesis enables tuning over its phase and structure, which dramatically improves the long-term stability of the resultant catalyst (ZnIn2S4) the catalyst morphology remains almost unchanged
We had an interest in indium sulfide as a catalyst because S-doped In was shown by Wang and co-workers to be effective for catalyzing CO2 reduction reaction (CO2RR) to formate
Summary
Developed solid-state catalysts can mediate carbon dioxide (CO2) electroreduction to valuable products at high rates and selectivities. 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. The development of catalysts that are active and selective for CO2 reduction reaction (CO2RR), and suppress the competing hydrogen evolution, has been the subject of intensive study This has resulted in a variety of carbon-based products to be synthesized from CO2, such as carbon monoxide (CO)[3], formate (HCOO−)[4], methane[5], and higher hydrocarbons and oxygenates (e.g., ethylene[6], ethanol[7], and n-propanol[8]). We report that incorporation of zinc (Zn) into indium sulfide (In2S3) synthesis enables tuning over its phase and structure, which dramatically improves the long-term stability of the resultant catalyst (ZnIn2S4) the catalyst morphology remains almost unchanged. We achieved nearly 100% CO2-to-formate conversion at a current density of 300 mA cm−2 over 60 h without degradation, corresponding to a high production rate of 8,894 μmol cm−2 h−1
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