Semimetallic Bismuthene with Edge-Rich Dangling Bonds: Broad-Spectrum-Driven and Edge-Confined Electron Enhancement Boosting CO 2 Hydrogenation Reduction.

Autor: Wang B; School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang, 212013, P. R. China.; Department of Physics, Department of Materials Science and Engineering, and Department of Biomedical Engineering, City University of Hong Kong, Kowloon, Hong Kong, 999077, P. R. China., Chen H; Beijing National Laboratory for Condensed Matter Physics, CAS Key Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, P. R. China., Zhang W; School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang, 212013, P. R. China., Liu H; Beijing National Laboratory for Condensed Matter Physics, CAS Key Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, P. R. China., Zheng Z; State Key Laboratory of Crystal Materials, Institute of Crystal Materials, Shandong University, Jinan, 250100, P. R. China., Huang F; Department of Information Engineering, Electronics, and Telecommunications, Sapienza University of Rome, Piazzale Aldo Moro 5, Roma, 00185, Italy., Liu J; School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang, 212013, P. R. China.; Department of Physics, Department of Materials Science and Engineering, and Department of Biomedical Engineering, City University of Hong Kong, Kowloon, Hong Kong, 999077, P. R. China., Liu G; School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang, 212013, P. R. China., Yan X; School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang, 212013, P. R. China., Weng YX; Beijing National Laboratory for Condensed Matter Physics, CAS Key Laboratory of Soft Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, P. R. China., Li H; School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang, 212013, P. R. China., She Y; College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, Zhejiang, 310014, P. R. China., Chu PK; Department of Physics, Department of Materials Science and Engineering, and Department of Biomedical Engineering, City University of Hong Kong, Kowloon, Hong Kong, 999077, P. R. China., Xia J; School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, 301 Xuefu Road, Zhenjiang, 212013, P. R. China.
Jazyk: angličtina
Zdroj: Advanced materials (Deerfield Beach, Fla.) [Adv Mater] 2024 May; Vol. 36 (19), pp. e2312676. Date of Electronic Publication: 2024 Feb 11.
DOI: 10.1002/adma.202312676
Abstrakt: Broad-spectrum-driven high-performance artificial photosynthesis is quite challenging. Herein, atomically ultrathin bismuthene with semimetallic properties is designed and demonstrated for broad-spectrum (ultraviolet-visible-near infrared light) (UV-vis-NIR)-driven photocatalytic CO 2 hydrogenation. The trap states in the bandgap produced by edge dangling bonds prolong the lifetime of the photogenerated electrons from 90 ps in bulk Bi to 1650 ps in bismuthine, and excited-state electrons are enriched at the edge of bismuthine. The edge dangling bonds of bismuthene as the active sites for adsorption/activation of CO 2 increase the hybridization ability of the Bi 6p orbital and O 2p orbital to significantly reduce the catalytic reaction energy barrier and promote the formation of C─H bonds until the generation of CH 4 . Under λ ≥ 400 nm and λ ≥ 550 nm irradiation, the utilization ratios of photogenerated electron reduction CO 2 hydrogenation to CO and CH 4 for bismuthene are 58.24 and 300.50 times higher than those of bulk Bi, respectively. Moreover, bismuthene can extend the CO 2 hydrogenation reaction to the near-infrared region (λ ≥ 700 nm). This pioneering work employs the single semimetal element as an artificial photosynthetic catalyst to produce a broad spectral response.
(© 2024 The Authors. Advanced Materials published by Wiley‐VCH GmbH.)
Databáze: MEDLINE
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