Photocatalytic CO Conversion of MWO Directly from the Air with High Selectivity: Insight into Full Spectrum-Induced Reaction Mechanism.

Authors:
Xiaoyong Wu
Xiaoyong Wu
Institute of Multidisciplinary Research for Advanced Materials
Japan
Dr. Yuan Li, MD,PhD,MBA
Dr. Yuan Li, MD,PhD,MBA
West China Hospital, Sichuan University
Professor
Chengdu, Sichuan | China
Gaoke Zhang
Gaoke Zhang
Wuhan University of Technology
China
Hong Chen
Hong Chen
Peking University People's Hospital
China
Mr. Jun Li, B.S.
Mr. Jun Li, B.S.
Huazhong Agricultural University
China
Kai Wang
Kai Wang
College of Public Health
United States
Yang Pan
Yang Pan
University of Science and Technology of China
China
Yan Zhao
Yan Zhao
State Key Laboratory of Hybrid Rice
China

J Am Chem Soc 2019 Apr 15;141(13):5267-5274. Epub 2019 Mar 15.

School of Environmental Science and Engineering , Southern University of Science and Technology , 1088 Xueyuan Road , Shenzhen 518055 , China.

Natural photosynthesis is a solar light-driven process utilized by plants to convert CO and water into carbohydrate molecules. The goal of artificial photosynthesis is the reduction of CO directly from air into high purity value-added products at atmospheric pressure. However, its realization, combined with deep mechanism investigation, is a huge challenge. Herein, we demonstrate that hexagonal tungsten bronze MWO (M = K, Rb, Cs) series with {010} facets, prepared by a peculiar "water-controllable releasing" solvothermal method, showed excellent full spectrum (UV, visible, and NIR lights)-induced photocatalytic CO reduction performance directly from the air at ambient pressure. Particularly, after 4 h near-infrared light irradiation, ca. 4.32% CO in the air could be converted into CHOH with 98.35% selectivity for RbWO. The experiments and theoretical calculations unveiled that the introduced alkali metal atom occupied the tunnel of hexagonal structure and donated more free electrons to reconstruct the electronic structure of MWO, which can enhance the polaron transition, modify the energy band structure, selectively adsorb CO rather than O from the air, decrease the activation energy of CO reaction, and finally make the effective CO reduction in the air a reality. This work may provide a new possibility for the practical application of artificial photosynthesis.

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Source
http://pubs.acs.org/doi/10.1021/jacs.8b12928
Publisher Site
http://dx.doi.org/10.1021/jacs.8b12928DOI Listing
April 2019
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