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 CO<sub>2</sub>, NO, and other gases. We employed asymmetrically stretched InO<sub>5</sub>S with symmetry-breaking indium sites as a highly efficient trifunctional catalysts for NO reduction, CO<sub>2</sub> reduction, and O<sub>2</sub> 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 NH<sub>3</sub>, HCOO<sup>-</sup>, and H<sub>2</sub>O<sub>2</sub>, maintaining over 90% Faradaic efficiency at industrial scales. Notably, the parallel electrolysis device reported in this study effectively produces high-value products like NH<sub>4</sub>COOH 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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Publication Details

Journal
Proceedings of the National Academy of Sciences
Published
2024-11-15
DOI
https://doi.org/10.1073/pnas.2409620121
Citations
13
Primary Topic
Ammonia Synthesis and Nitrogen Reduction
Type
article
Field-Weighted Citation Impact
1.39

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article

Direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites

Yuntong Sun, Liming Dai, Jingjing Duan, Nicole L. D. Sui et al.
13 citations
Proceedings of the National Academy of Sciences
Ammonia Synthesis and Nitrogen Reduction
1.39
article

Direct parallel electrosynthesis of high-value chemicals from atmospheric components on symmetry-breaking indium sites

Yuntong Sun, Liming Dai, Jingjing Duan, Nicole L. D. Sui, Sheng Chen, Jong Min Lee, Yinghao Li
article en
13 citations

Abstract

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 CO<sub>2</sub>, NO, and other gases. We employed asymmetrically stretched InO<sub>5</sub>S with symmetry-breaking indium sites as a highly efficient trifunctional catalysts for NO reduction, CO<sub>2</sub> reduction, and O<sub>2</sub> 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 NH<sub>3</sub>, HCOO<sup>-</sup>, and H<sub>2</sub>O<sub>2</sub>, maintaining over 90% Faradaic efficiency at industrial scales. Notably, the parallel electrolysis device reported in this study effectively produces high-value products like NH<sub>4</sub>COOH 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.

Proceedings of the National Academy of SciencesVol. 121(47)
Nanyang Technological University (SG), Nanjing University of Science and Technology (CN)
Ministry of Education - Singapore, Nanyang Technological University, National Natural Science Foundation of China, Government of Jiangsu Province, Natural Science Foundation of Jiangsu Province, Nanjing University of Science and Technology, Nanjing University
Industry, innovation and infrastructure, Responsible consumption and production
Openalex Percentile: Top 19%
Ammonia Synthesis and Nitrogen Reduction
1.39
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