Ruthenium Single Atomic Sites Surrounding the Support Pit with Exceptional Photocatalytic Activity.

Autor: Tao Y; Department of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China., Guan J; Department of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China., Zhang J; Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering Wenzhou University, Wenzhou, 325035, China., Hu S; Department of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China., Ma R; Department of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China., Zheng H; Department of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China., Gong J; Department of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China., Zhuang Z; Department of Chemistry, Tsinghua University, Beijing, 100084, China.; Department of Chemical Engineering, Columbia University, New York, NY 10027, USA., Liu S; School of Materials Science and Engineering, Anhui University, Anhui, 230601, China., Ou H; Department of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China.; School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi An Shi, Xi'an, 710049, China., Wang D; Department of Chemistry, Tsinghua University, Beijing, 100084, China., Xiong Y; Department of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 May 21; Vol. 63 (21), pp. e202400625. Date of Electronic Publication: 2024 Apr 22.
DOI: 10.1002/anie.202400625
Abstrakt: Single-metal atomic sites and vacancies can accelerate the transfer of photogenerated electrons and enhance photocatalytic performance in photocatalysis. In this study, a series of nickel hydroxide nanoboards (Ni(OH) x NBs) with different loadings of single-atomic Ru sites (w-SA-Ru/Ni(OH) x ) were synthesized via a photoreduction strategy. In such catalysts, single-atomic Ru sites are anchored to the vacancies surrounding the pits. Notably, the SA-Ru/Ni(OH) x with 0.60 wt % Ru loading (0.60-SA-Ru/Ni(OH) x ) exhibits the highest catalytic performance (27.6 mmol g -1  h -1 ) during the photocatalytic reduction of CO 2 (CO 2 RR). Either superfluous (0.64 wt %, 18.9 mmol g -1  h -1 ; 3.35 wt %, 9.4 mmol -1  h -1 ) or scarce (0.06 wt %, 15.8 mmol g -1  h -1 ; 0.29 wt %, 21.95 mmol g -1  h -1 ; 0.58 wt %, 23.4 mmol g -1  h -1 ) of Ru sites have negative effect on its catalytic properties. Density functional theory (DFT) calculations combined with experimental results revealed that CO 2 can be adsorbed in the pits; single-atomic Ru sites can help with the conversion of as-adsorbed CO 2 and lower the energy of *COOH formation accelerating the reaction; the excessive single-atomic Ru sites occupy vacancies that retard the completion of CO 2 RR.
(© 2024 Wiley-VCH GmbH.)
Databáze: MEDLINE
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