Ru Single Atom Dispersed Cu Nanoparticle with Dual Sites Enables Outstanding Photocatalytic CO2 Reduction

• Published in: ACS nano 2024-09, Vol.18 (38), p.26271-26280
• Main Authors: Liu, Lizhen, Hu, Jingcong, Sheng, Yuan, Akhoundzadeh, Hossein, Tu, Wenguang, Siow, Wei Jian Samuel, Ong, Jia Hui, Huang, Hongwei, Xu, Rong
• Format: Article
• Language: English
• ISSN: 1936-0851; 1936-086X; 1936-086X
• DOI: 10.1021/acsnano.4c08303

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.