Stabilizing indium sulfide for CO2 electroreduction to formate at high rate by zinc incorporation
Recently developed solid-state catalysts can mediate carbon dioxide (CO 2 ) 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 agglo...
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| Published in | Nature communications Vol. 12; no. 1; pp. 5835 - 9 |
|---|---|
| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
05.10.2021
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
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| Abstract | Recently developed solid-state catalysts can mediate carbon dioxide (CO
2
) 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 ZnIn
2
S
4
catalyst can reduce CO
2
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 H
2
O to react with CO
2
, yielding HCOO* intermediates—from being dissolved during high-rate electrolysis.
Developing durable catalysts for carbon dioxide reduction to formate at commercial-scale current densities is challenging. This work reports that indium sulfide stabilized through zinc incorporation can produce formate efficiently and quickly at high current densities over long timescales. |
|---|---|
| AbstractList | Developing durable catalysts for carbon dioxide reduction to formate at commercial-scale current densities is challenging. This work reports that indium sulfide stabilized through zinc incorporation can produce formate efficiently and quickly at high current densities over long timescales. Recently developed solid-state catalysts can mediate carbon dioxide (CO 2 ) 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 ZnIn 2 S 4 catalyst can reduce CO 2 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 H 2 O to react with CO 2 , yielding HCOO* intermediates—from being dissolved during high-rate electrolysis. Developing durable catalysts for carbon dioxide reduction to formate at commercial-scale current densities is challenging. This work reports that indium sulfide stabilized through zinc incorporation can produce formate efficiently and quickly at high current densities over long timescales. 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.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. 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.Developing durable catalysts for carbon dioxide reduction to formate at commercial-scale current densities is challenging. This work reports that indium sulfide stabilized through zinc incorporation can produce formate efficiently and quickly at high current densities over long timescales. Recently developed solid-state catalysts can mediate carbon dioxide (CO 2 ) 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 ZnIn 2 S 4 catalyst can reduce CO 2 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 H 2 O to react with CO 2 , yielding HCOO* intermediates—from being dissolved during high-rate electrolysis. |
| ArticleNumber | 5835 |
| Author | Niu, Zhuang-Zhuang Zhang, Xiao-Long Gao, Fei-Yue Yang, Peng-Peng Wu, Zhi-Zheng Liao, Jie Tang, Kai-Bin Chi, Li-Ping Gao, Min-Rui |
| Author_xml | – sequence: 1 givenname: Li-Ping orcidid: 0000-0001-5020-0340 surname: Chi fullname: Chi, Li-Ping organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China – sequence: 2 givenname: Zhuang-Zhuang orcidid: 0000-0002-8412-4953 surname: Niu fullname: Niu, Zhuang-Zhuang organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China – sequence: 3 givenname: Xiao-Long orcidid: 0000-0002-5596-0776 surname: Zhang fullname: Zhang, Xiao-Long organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China – sequence: 4 givenname: Peng-Peng orcidid: 0000-0002-5923-1722 surname: Yang fullname: Yang, Peng-Peng organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China – sequence: 5 givenname: Jie orcidid: 0000-0002-4014-7838 surname: Liao fullname: Liao, Jie organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China – sequence: 6 givenname: Fei-Yue orcidid: 0000-0002-3811-7509 surname: Gao fullname: Gao, Fei-Yue organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China – sequence: 7 givenname: Zhi-Zheng orcidid: 0000-0003-2022-9147 surname: Wu fullname: Wu, Zhi-Zheng organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China – sequence: 8 givenname: Kai-Bin orcidid: 0000-0002-0398-1196 surname: Tang fullname: Tang, Kai-Bin email: kbtang@ustc.edu.cn organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China – sequence: 9 givenname: Min-Rui orcidid: 0000-0002-7805-803X surname: Gao fullname: Gao, Min-Rui email: mgao@ustc.edu.cn organization: Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China |
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| Snippet | Recently developed solid-state catalysts can mediate carbon dioxide (CO
2
) electroreduction to valuable products at high rates and selectivities. However,... Recently developed solid-state catalysts can mediate carbon dioxide (CO2) electroreduction to valuable products at high rates and selectivities. However, under... Developing durable catalysts for carbon dioxide reduction to formate at commercial-scale current densities is challenging. This work reports that indium... |
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| SubjectTerms | 639/301/299/886 639/638/161/886 639/638/298 Carbon dioxide Catalysts Current density Electrolysis Electrowinning Humanities and Social Sciences Indium Intermediates multidisciplinary Science Science (multidisciplinary) Sulfides Sulfur Zinc |
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| Title | Stabilizing indium sulfide for CO2 electroreduction to formate at high rate by zinc incorporation |
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