Ru single atom dispersed Cu nanoparticle with dual sites enables outstanding photocatalytic CO2 reduction
Cu-based catalysts are promising candidates for CO2 reduction owing to the favorable energetics of Cu sites for CO2 adsorption and transformation. However, CO2 reduction involving insurmountable activation barriers and various byproducts remains a significant challenge to achieve high activity and s...
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sg-ntu-dr.10356-1810192024-11-11T07:17:46Z Ru single atom dispersed Cu nanoparticle with dual sites enables outstanding photocatalytic CO2 reduction Liu, Lizhen Hu, Jingcong Sheng, Yuan Akhoundzadeh, Hossein Tu, Wenguang Siow, Samuel Wei Jian Ong, Jia Hui Huang, Hongwei Xu, Rong School of Chemistry, Chemical Engineering and Biotechnology C4T CREATE, National Research Foundation Singapore Membrane Technology Centre Nanyang Environment and Water Research Institute Engineering Dual catalytic sites Nanoparticles Cu-based catalysts are promising candidates for CO2 reduction owing to the favorable energetics of Cu sites for CO2 adsorption and transformation. However, CO2 reduction involving insurmountable activation barriers and various byproducts remains a significant challenge to achieve high activity and selectivity. Herein, a photocatalyst constructed with single-Ru-site-on-Cu-nanoparticle on Bi4Ti3O12 exhibits exceptional activity and selectivity for CO2 conversion to CO. The experimental and theoretical results consistently reveal that the Ru-Cu dual sites allow the rapid transfer of photogenerated carriers for closely interacting with CO2 molecules. Importantly, the Ru-Cu dual sites exhibit extremely strong CO2 adsorption ability, and the Gibbs free energy of the rate-determining step (*CO2 to *COOH) has been significantly reduced, synergistically enhancing the entire CO2 conversion process. The optimal BTOCu2Ru0.5 photocatalyst manifests a high performance for selective reduction of CO2 to CO, yielding 10.84 μmol over 15 mg of photocatalyst in 4 h (180.67 μmol·g-1·h-1) under a 300 W Xe lamp without any photosensitizer and sacrificial reagent, outperforming all bismuth-based materials and being one of the best photocatalysts ever reported under similar reaction conditions. This work presents a strategy for the rational design of multiple metal sites toward efficient photocatalytic reduction of CO2. National Research Foundation (NRF) This work was jointly supported by National Key Research and Development Program of China (no. 2022YFB3803600), the National Natural Science Foundation of China (nos. 52272244and 51972288), the Fundamental Research Funds for the Central Universities (2652022202), and Campus for Research Excellence and Technological Enterprise (CREATE) program (C4T CREATE) by the National Research Foundation (NRF), Singapore. 2024-11-11T07:17:45Z 2024-11-11T07:17:45Z 2024 Journal Article Liu, L., Hu, J., Sheng, Y., Akhoundzadeh, H., Tu, W., Siow, S. W. J., Ong, J. H., Huang, H. & Xu, R. (2024). Ru single atom dispersed Cu nanoparticle with dual sites enables outstanding photocatalytic CO2 reduction. ACS Nano, 18, 26271-26280. https://dx.doi.org/10.1021/acsnano.4c08303 1936-0851 https://hdl.handle.net/10356/181019 10.1021/acsnano.4c08303 39270050 2-s2.0-85204216597 18 26271 26280 en CT4 CREATE ACS Nano © 2024 American Chemical Society. All rights reserved. |
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Engineering Dual catalytic sites Nanoparticles Liu, Lizhen Hu, Jingcong Sheng, Yuan Akhoundzadeh, Hossein Tu, Wenguang Siow, Samuel Wei Jian Ong, Jia Hui Huang, Hongwei Xu, Rong Ru single atom dispersed Cu nanoparticle with dual sites enables outstanding photocatalytic CO2 reduction |
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Cu-based catalysts are promising candidates for CO2 reduction owing to the favorable energetics of Cu sites for CO2 adsorption and transformation. However, CO2 reduction involving insurmountable activation barriers and various byproducts remains a significant challenge to achieve high activity and selectivity. Herein, a photocatalyst constructed with single-Ru-site-on-Cu-nanoparticle on Bi4Ti3O12 exhibits exceptional activity and selectivity for CO2 conversion to CO. The experimental and theoretical results consistently reveal that the Ru-Cu dual sites allow the rapid transfer of photogenerated carriers for closely interacting with CO2 molecules. Importantly, the Ru-Cu dual sites exhibit extremely strong CO2 adsorption ability, and the Gibbs free energy of the rate-determining step (*CO2 to *COOH) has been significantly reduced, synergistically enhancing the entire CO2 conversion process. The optimal BTOCu2Ru0.5 photocatalyst manifests a high performance for selective reduction of CO2 to CO, yielding 10.84 μmol over 15 mg of photocatalyst in 4 h (180.67 μmol·g-1·h-1) under a 300 W Xe lamp without any photosensitizer and sacrificial reagent, outperforming all bismuth-based materials and being one of the best photocatalysts ever reported under similar reaction conditions. This work presents a strategy for the rational design of multiple metal sites toward efficient photocatalytic reduction of CO2. |
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School of Chemistry, Chemical Engineering and Biotechnology |
author_facet |
School of Chemistry, Chemical Engineering and Biotechnology Liu, Lizhen Hu, Jingcong Sheng, Yuan Akhoundzadeh, Hossein Tu, Wenguang Siow, Samuel Wei Jian Ong, Jia Hui Huang, Hongwei Xu, Rong |
format |
Article |
author |
Liu, Lizhen Hu, Jingcong Sheng, Yuan Akhoundzadeh, Hossein Tu, Wenguang Siow, Samuel Wei Jian Ong, Jia Hui Huang, Hongwei Xu, Rong |
author_sort |
Liu, Lizhen |
title |
Ru single atom dispersed Cu nanoparticle with dual sites enables outstanding photocatalytic CO2 reduction |
title_short |
Ru single atom dispersed Cu nanoparticle with dual sites enables outstanding photocatalytic CO2 reduction |
title_full |
Ru single atom dispersed Cu nanoparticle with dual sites enables outstanding photocatalytic CO2 reduction |
title_fullStr |
Ru single atom dispersed Cu nanoparticle with dual sites enables outstanding photocatalytic CO2 reduction |
title_full_unstemmed |
Ru single atom dispersed Cu nanoparticle with dual sites enables outstanding photocatalytic CO2 reduction |
title_sort |
ru single atom dispersed cu nanoparticle with dual sites enables outstanding photocatalytic co2 reduction |
publishDate |
2024 |
url |
https://hdl.handle.net/10356/181019 |
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1816858957481771008 |