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

Autor: Sun Y; School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, Singapore 637459, Singapore., Dai L; Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering, Nanjing University of Science and Technology, Nanjing 210094, China., Sui NLD; School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, Singapore 637459, Singapore.; Environmental Chemistry and Materials Centre, Nanyang Environment & Water Research Institute, Interdisciplinary Graduate Programme, Nanyang Technological University, Singapore 637141, Singapore., Li Y; School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, Singapore 637459, Singapore., Tian M; Interdisciplinary Center for Fundamental and Frontier Sciences, Nanjing University of Science and Technology, Jiangyin, Jiangsu 214443, China., Duan J; Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering, Nanjing University of Science and Technology, Nanjing 210094, China., Chen S; Key Laboratory for Soft Chemistry and Functional Materials, School of Chemistry and Chemical Engineering, School of Energy and Power Engineering, Nanjing University of Science and Technology, Nanjing 210094, China., Lee JM; School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, Singapore 637459, Singapore.
Jazyk: angličtina
Zdroj: Proceedings of the National Academy of Sciences of the United States of America [Proc Natl Acad Sci U S A] 2024 Nov 19; Vol. 121 (47), pp. e2409620121. Date of Electronic Publication: 2024 Nov 15.
DOI: 10.1073/pnas.2409620121
Abstrakt: 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 2 , NO, and other gases. We employed asymmetrically stretched InO 5 S with symmetry-breaking indium sites as a highly efficient trifunctional catalysts for NO reduction, CO 2 reduction, and O 2 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 3 , HCOO - , and H 2 O 2 , maintaining over 90% Faradaic efficiency at industrial scales. Notably, the parallel electrolysis device reported in this study effectively produces high-value products like NH 4 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.
Competing Interests: Competing interests statement:The authors declare no competing interest.
Databáze: MEDLINE
Externí odkaz: