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General and Efficient Synthesis of Two-Dimensional Monolayer Mesoporous Materials with Diverse Framework Compositions

  • Xuanyu Yang
    Xuanyu Yang
    Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and iChEM, Fudan University, Shanghai 200433, China
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  • Yanyan Li
    Yanyan Li
    Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and iChEM, Fudan University, Shanghai 200433, China
    More by Yanyan Li
  • Junhao Ma
    Junhao Ma
    Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and iChEM, Fudan University, Shanghai 200433, China
    More by Junhao Ma
  • Yidong Zou
    Yidong Zou
    Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and iChEM, Fudan University, Shanghai 200433, China
    More by Yidong Zou
  • Xinran Zhou
    Xinran Zhou
    Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and iChEM, Fudan University, Shanghai 200433, China
    More by Xinran Zhou
  • Xiaowei Cheng
    Xiaowei Cheng
    Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and iChEM, Fudan University, Shanghai 200433, China
  • Fahad A. Alharthi
    Fahad A. Alharthi
    Department of Chemistry, College of Science, King Saud University, P.O. Box 2455, Riyadh 11451, Saudi Arabia
  • Abdulaziz A. Alghamdi
    Abdulaziz A. Alghamdi
    Department of Chemistry, College of Science, King Saud University, P.O. Box 2455, Riyadh 11451, Saudi Arabia
  • , and 
  • Yonghui Deng*
    Yonghui Deng
    Department of Chemistry, State Key Laboratory of Molecular Engineering of Polymers, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, and iChEM, Fudan University, Shanghai 200433, China
    State Key Lab of Transducer Technology, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, China
    *Email: [email protected]
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Cite this: ACS Appl. Mater. Interfaces 2021, 13, 1, 1222–1233
Publication Date (Web):December 24, 2020
https://doi.org/10.1021/acsami.0c18027
Copyright © 2020 American Chemical Society
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Abstract

Two-dimensional (2D) mesoporous materials have received substantial research interest due to their highly exposed active sites and unusual nanoconfinement effect. However, controllable and efficient synthesis of 2D mesoporous materials and investigation of their intrinsic properties have remained quite rare. Herein, a general and effective surface-limited cooperative assembly (SLCA) method enabled by leveling precursor solutions on KCl crystals via centrifugation is employed to conveniently synthesize two-dimensional (2D) monolayer mesoporous materials with different compositions. This novel strategy is performed in a manner similar to spin coating, not only enabling generation of ultrathin mesostructured composite film on KCl particles and recycling excessive precursor solution but also providing favorable solvent annealing environment for the film to form ordered mesostructures. Taking monolayer mesoporous Ce0.8Zr0.2O2 solid solutions as a sample, they display ultrathin nanosheet morphology with a thickness of ∼20 nm, highly open porous structure, and easily accessible active sites of surface superoxide species. Upon decoration of 2D mesoporous Ce0.8Zr0.2O2 nanosheets with Pt nanoparticles, the obtained catalyst exhibits superior catalytic activity and stability toward CO oxidation with a low onset temperature of 30 °C and a 100% conversion temperature of 95 °C, which are 35–70 °C lower than those for their counterpart materials, namely, three-dimensional (3D) mesoporous Pt/Ce0.8Zr0.2O2. Moreover, their TOFPt value is ∼11.3 times higher than that of 3D mesoporous Pt/Ce0.8Zr0.2O2. Characterizations based on various techniques indicate that such an outstanding catalytic performance is due to the ultrashort distance (20 nm) of mass diffusion, highly exposed active sites, rich surface-chemisorbed oxygen, and the synergistic effect between the Ce0.8Zr0.2O2 matrix and Pt species.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.0c18027.

  • Static contact angle images of the KCl crystal; HRTEM image and XRD patterns of the 2D mesoporous TiO2 nanosheets; HRTEM image and XRD patterns of the 2D mesoporous ZrO2 nanosheets; HRTEM image and XRD patterns of the 2D mesoporous WO3 nanosheets; N2 sorption isotherms of 2D mesoporous Ce0.8Zr0.2O2 nanosheets; XPS results of Ce0.8Zr0.2O2 nanosheet; H2-TPR profiles of the 2D mesoporous Ce0.8Zr0.2O2 nanosheets; HRTEM and XRD patterns of 2D mesoporous Pt/Ce0.8Zr0.2O2 nanosheets; HAADF-STEM image; WAXRD pattern of sample; CO conversion from 20 to 160 °C with 1–50 cycles; HRTEM image of 2D mesoporous Pt/Ce0.8Zr0.2O2 nanosheets after CO oxidation experiments; XPS spectra of bulk mesoporous Pt/Ce0.8Zr0.2O2; selected DRIFT spectra of CO adsorbed on the 2D mesoporous Pt/Ce0.8Zr0.2O2 nanosheets; and turnover frequency, ethylene selectivity, and regeneration test of nonoxidative dehydrogenation of ethane (PDF)

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