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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Main Authors: Liu, Lizhen, Hu, Jingcong, Sheng, Yuan, Akhoundzadeh, Hossein, Tu, Wenguang, Siow, Samuel Wei Jian, Ong, Jia Hui, Huang, Hongwei, Xu, Rong
Other Authors: School of Chemistry, Chemical Engineering and Biotechnology
Format: Article
Language:English
Published: 2024
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Online Access:https://hdl.handle.net/10356/181019
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Institution: Nanyang Technological University
Language: English
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spelling 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.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering
Dual catalytic sites
Nanoparticles
spellingShingle 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
description 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.
author2 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
_version_ 1816858957481771008