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Spatially Confined Formation of Single Atoms in Highly Porous Carbon Nitride Nanoreactors

  • Yunpeng Zuo
    Yunpeng Zuo
    Department of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong People’s Republic of China
    More by Yunpeng Zuo
  • Tingting Li
    Tingting Li
    Institute of Surface Micro and Nano Materials, Xuchang University, 461002 Xuchang, Henan, People’s Republic of China
    More by Tingting Li
  • Ning Zhang
    Ning Zhang
    Department of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong People’s Republic of China
    More by Ning Zhang
  • Tianyun Jing
    Tianyun Jing
    School of Materials Science and Engineering, Jiangsu University, 212013 Zhenjiang, People’s Republic of China
    More by Tianyun Jing
  • Dewei Rao*
    Dewei Rao
    School of Materials Science and Engineering, Jiangsu University, 212013 Zhenjiang, People’s Republic of China
    *[email protected]
    More by Dewei Rao
  • Patrik Schmuki
    Patrik Schmuki
    Department of Materials Science, University of Erlangen-Nuremberg, Institute for Surface Science and Corrosion WW4-LKO, Martensstraße 7, D-91058 Erlangen, Germany
    Regional Centre of Advanced Technologies and Materials, Czech Advanced Technology and Research Institute, Palacký University, Křížkovského 511/8, 779 00 Olomouc, Czech Republic
  • Štěpán Kment*
    Štěpán Kment
    Regional Centre of Advanced Technologies and Materials, Czech Advanced Technology and Research Institute, Palacký University, Křížkovského 511/8, 779 00 Olomouc, Czech Republic
    CEET, Nanotechnology Centre, Centre of Energy and Environmental Technologies, VŠB−Technical University of Ostrava, 17. Listopadu 2172/15, 708 00 Ostrava, Poruba, Czech Republic
    *[email protected]
  • Radek Zbořil
    Radek Zbořil
    Regional Centre of Advanced Technologies and Materials, Czech Advanced Technology and Research Institute, Palacký University, Křížkovského 511/8, 779 00 Olomouc, Czech Republic
    CEET, Nanotechnology Centre, Centre of Energy and Environmental Technologies, VŠB−Technical University of Ostrava, 17. Listopadu 2172/15, 708 00 Ostrava, Poruba, Czech Republic
  • , and 
  • Yang Chai*
    Yang Chai
    Department of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong People’s Republic of China
    *[email protected]
    More by Yang Chai
Cite this: ACS Nano 2021, 15, 4, 7790–7798
Publication Date (Web):April 19, 2021
https://doi.org/10.1021/acsnano.1c01872
Copyright © 2021 American Chemical Society

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    Abstract

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    Reducing the size of a catalyst to a single atom (SA) level can dramatically change its physicochemical properties and significantly boost its catalytic activity. However, the massive synthesis of SA catalysts still remains a grand challenge mainly because of the aggregation and nucleation of the generated atoms during the reaction. Here, we design and implement a spatially confined synthetic strategy based on a porous-hollow carbon nitride (p-CN) coordinated with 1-butyl-3-methylimidazole hexafluorophosphate, which can act as a nanoreactor and allow us to obtain metal SA catalysts (p-CN@M SAs). This relatively easy and highly effective method provides a way to massively synthesize single/multiple atoms (p-CN@M SAs, M = Pt, Pd, Cu, Fe, etc.). Moreover, the amorphous NiB-coated p-CN@Pt SAs can further increase the loading amount of Pt SAs to 3.7 wt %. The synthesized p-CN@Pt&NiB electrocatalyst exhibits an extraordinary hydrogen evolution reaction activity with the overpotential of 40.6 mV@10 mA/cm–2 and the Tofel slope of 29.26 mV/dec.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.1c01872.

    • SEM, XRD, Raman, BET, and TEM results of the p-CN. HRTEM images of the p-CN loaded PtNPs. EDS mapping images of the p-CN@Pt and p-CN@S–Pt. STEM images of p-CN@S–Pt. XPS survey pattern of p-CN@S–Pt&NiB. Enlarged SEM images of p-CN@S–Pt&NiB. HER stability test of the obtained catalysts (PDF)

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