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Photocatalytic Chemical CO2 Fixation by Cu-BDC [email protected]–Mesoporous-TiO2 under Mild Conditions

  • Zhenxing Li*
    Zhenxing Li
    State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, Beijing Key Laboratory of Biogas Upgrading Utilization, China University of Petroleum (Beijing), Beijing 102249, China
    *E-mail: [email protected] (Z.L.).
    More by Zhenxing Li
  • Junmei Chu
    Junmei Chu
    State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, Beijing Key Laboratory of Biogas Upgrading Utilization, China University of Petroleum (Beijing), Beijing 102249, China
    More by Junmei Chu
  • Dong Meng
    Dong Meng
    Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, United States
    More by Dong Meng
  • Yangyang Wen
    Yangyang Wen
    State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, Beijing Key Laboratory of Biogas Upgrading Utilization, China University of Petroleum (Beijing), Beijing 102249, China
    More by Yangyang Wen
  • Xiaofei Xing
    Xiaofei Xing
    State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, Beijing Key Laboratory of Biogas Upgrading Utilization, China University of Petroleum (Beijing), Beijing 102249, China
    More by Xiaofei Xing
  • He Miao
    He Miao
    State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, Beijing Key Laboratory of Biogas Upgrading Utilization, China University of Petroleum (Beijing), Beijing 102249, China
    More by He Miao
  • Mingliang Hu
    Mingliang Hu
    State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, Beijing Key Laboratory of Biogas Upgrading Utilization, China University of Petroleum (Beijing), Beijing 102249, China
    More by Mingliang Hu
  • Chengcheng Yu
    Chengcheng Yu
    State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, Beijing Key Laboratory of Biogas Upgrading Utilization, China University of Petroleum (Beijing), Beijing 102249, China
  • Zhiting Wei
    Zhiting Wei
    State Key Laboratory of Heavy Oil Processing, College of New Energy and Materials, Beijing Key Laboratory of Biogas Upgrading Utilization, China University of Petroleum (Beijing), Beijing 102249, China
    More by Zhiting Wei
  • Yang Yang
    Yang Yang
    Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, United States
    More by Yang Yang
  • , and 
  • Yongle Li*
    Yongle Li
    Department of Physics, International Center for Quantum and Molecular Structures, and Shanghai Key Laboratory of High Temperature Superconductors, Shanghai University, Shanghai 200444, China
    *E-mail: [email protected] (Y.L.).
    More by Yongle Li
Cite this: ACS Catal. 2019, 9, 9, 8659–8668
Publication Date (Web):August 9, 2019
https://doi.org/10.1021/acscatal.9b02553
Copyright © 2019 American Chemical Society
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Supporting Info (1)»

Abstract

Growing greenhouse gas CO2 is driving the research on the chemical fixation of CO2. Here, the organic reaction of CO2 with benzyl halogen for chemical CO2 fixation under ambient conditions with irradiation of ultraviolet light is successfully catalyzed by Cu-BDC [email protected]–mesoporous-TiO2 ([email protected]–meso-TiO2), which shows high photocatalytic activity for both benzyl chloride and bromide reacting with CO2. Meanwhile, the prepared [email protected]–meso-TiO2 possesses a three-scale porous structure, including macropores, mesopores, and micropores. In the uniform hierarchical structure, the microporous Cu-BDC nanosheet is confined in the macropore of macroporous–mesoporous-TiO2, while the ordered mesoporous structure is in the macroporous walls. This multilevel porous distribution can significantly improve the active surface areas and mass transfer efficiency of [email protected]–meso-TiO2. Therefore, this finding has opened a field of research on photocatalytic chemical CO2 fixation.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acscatal.9b02553.

  • Routes for the chemical fixation of CO2; schematic image of the catalytic reaction device; further SEM image of the PS microspheres; SEM, TEM, SAXRD, WAXRD, XPS, and PL spectrum of macro–meso-TiO2; SEM, CO2 adsorption isotherms, XPS, and UV–vis of Cu-BDC; EDX, FTIR, CO2 adsorption isotherms, DRIFT spectrum of CO2 adsorbed on [email protected]–meso-TiO2 at room temperature and spectra collected with Ar purging, transient photocurrent response, Nyquist plots for EIS, and the PL spectrum of [email protected]–meso-TiO2; SEM and WAXRD for pure TiO2 and [email protected] TiO2; the UV–vis spectrum for [email protected] TiO2; the AFM image of the Cu-BDC nanosheet for [email protected]–meso-TiO2; optimization of the ratio of macro–meso-TiO2 and Cu-BDC of the composite [email protected]–meso-TiO2; optimization of the reaction conditions; screening for the catalysts; control experiment without substrates; potential energy profiles calculated for activating CO2 directly; potential energy profiles for the optimization step from B′ to B spontaneously; reuse of the [email protected]–meso-TiO2 catalyst for the carboxylation of benzyl halide with CO2; SEM, TEM, and XRD of recycled [email protected]–meso-TiO2; computation details and the data; the 1H NMR spectrum and mass spectrum of carboxylation products (PDF)

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