Direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites
To tackle significant environmental and energy challenges from increased greenhouse gas emissions in the atmosphere, we propose a method that synergistically combines cost-efficient integrated systems with parallel catalysis to produce high-value chemicals from CO2, NO, and other gases. We employed...
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sg-ntu-dr.10356-1823702025-01-31T15:32:26Z Direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites Sun, Yuntong Dai, Liming Sui, Nicole L. D. Li, Yinghao Tian, Meng Duan, Jingjing Chen, Sheng Lee, Jong-Min School of Chemistry, Chemical Engineering and Biotechnology Nanyang Environment and Water Research Institute Environmental Chemistry and Materials Centre Chemistry Electrosynthesis Symmetry-breaking To tackle significant environmental and energy challenges from increased greenhouse gas emissions in the atmosphere, we propose a method that synergistically combines cost-efficient integrated systems with parallel catalysis to produce high-value chemicals from CO2, NO, and other gases. We employed asymmetrically stretched InO5S with symmetry-breaking indium sites as a highly efficient trifunctional catalysts for NO reduction, CO2 reduction, and O2 reduction. Mechanistic studies reveal that the symmetry-breaking at indium sites substantially improves d-band center interactions and adsorption of intermediates, thereby enhancing trifunctional catalytic activity. Employed in a flow electrolysis system, the catalyst achieves continuous and flexible production of NH3, HCOO-, and H2O2, maintaining over 90% Faradaic efficiency at industrial scales. Notably, the parallel electrolysis device reported in this study effectively produces high-value products like NH4COOH directly from greenhouse gases in pure water, offering an economically efficient solution for small molecule synthesis and unique insights for the sustainable conversion of inexhaustible gases into valuable products. Therefore, this work possesses considerable potential for future practical applications in sustainable industrial processes. Ministry of Education (MOE) Published version This work is funded by the AcRF Tier 1 provided by the Ministry of Education (grant RG105/19) in Singapore, the National Natural Science Foundation of China (grants 52376193, 51888103, 92163124, and 12304084), and the Natural Science Foundation of Jiangsu Province (grants BK20220930 and BK20230097). 2025-01-27T03:55:12Z 2025-01-27T03:55:12Z 2024 Journal Article Sun, Y., Dai, L., Sui, N. L. D., Li, Y., Tian, M., Duan, J., Chen, S. & Lee, J. (2024). Direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites. Proceedings of the National Academy of Sciences of the United States of America, 121(47), e2409620121-. https://dx.doi.org/10.1073/pnas.2409620121 0027-8424 https://hdl.handle.net/10356/182370 10.1073/pnas.2409620121 39546577 2-s2.0-85209703339 47 121 e2409620121 en RG105/19 Proceedings of the National Academy of Sciences of the United States of America © 2024 the Author(s). Published by PNAS. This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND). application/pdf |
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Chemistry Electrosynthesis Symmetry-breaking Sun, Yuntong Dai, Liming Sui, Nicole L. D. Li, Yinghao Tian, Meng Duan, Jingjing Chen, Sheng Lee, Jong-Min Direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites |
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To tackle significant environmental and energy challenges from increased greenhouse gas emissions in the atmosphere, we propose a method that synergistically combines cost-efficient integrated systems with parallel catalysis to produce high-value chemicals from CO2, NO, and other gases. We employed asymmetrically stretched InO5S with symmetry-breaking indium sites as a highly efficient trifunctional catalysts for NO reduction, CO2 reduction, and O2 reduction. Mechanistic studies reveal that the symmetry-breaking at indium sites substantially improves d-band center interactions and adsorption of intermediates, thereby enhancing trifunctional catalytic activity. Employed in a flow electrolysis system, the catalyst achieves continuous and flexible production of NH3, HCOO-, and H2O2, maintaining over 90% Faradaic efficiency at industrial scales. Notably, the parallel electrolysis device reported in this study effectively produces high-value products like NH4COOH directly from greenhouse gases in pure water, offering an economically efficient solution for small molecule synthesis and unique insights for the sustainable conversion of inexhaustible gases into valuable products. Therefore, this work possesses considerable potential for future practical applications in sustainable industrial processes. |
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School of Chemistry, Chemical Engineering and Biotechnology |
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School of Chemistry, Chemical Engineering and Biotechnology Sun, Yuntong Dai, Liming Sui, Nicole L. D. Li, Yinghao Tian, Meng Duan, Jingjing Chen, Sheng Lee, Jong-Min |
format |
Article |
author |
Sun, Yuntong Dai, Liming Sui, Nicole L. D. Li, Yinghao Tian, Meng Duan, Jingjing Chen, Sheng Lee, Jong-Min |
author_sort |
Sun, Yuntong |
title |
Direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites |
title_short |
Direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites |
title_full |
Direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites |
title_fullStr |
Direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites |
title_full_unstemmed |
Direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites |
title_sort |
direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites |
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2025 |
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https://hdl.handle.net/10356/182370 |
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1823108707835183104 |