4.8 Article

Hollow and Yolk-Shell Co-N-C@SiO2 Nanoreactors: Controllable Synthesis with High Selectivity and Activity for Nitroarene Hydrogenation

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 3, Pages 3624-3630

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b19364

Keywords

nanoreactor; hollow and yolk-shell structure; selective hydrogenation; controllable synthesis; metal organic framework

Funding

  1. National Natural Science Foundation of China [21676155]
  2. China Postdoctoral Science Foundation [2019M660660]
  3. Shuimu Tsinghua Scholar program

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The use of hollow and yolk-shell nanocomposites is an effective route to enhance catalytic performance. A strategy that allows precise control of the nanocomposites was developed to synthesize novel hollow and yolk-shell SiO2 nanoreactors of Co-N-C@SiO2, which used ZIF-67 as the hard template and also as the source for active sites. A size dependence of the nanoreactor structure was observed. Large size of ZIF-67 gave yolk-shell Y-Co-N-C@SiO2 while small size of crystals gave hollow H-Co-N-C@SiO2. The hydrogenation reaction results showed that the Co-N-C@SiO2 catalyst exhibited a high selectivity (>99%) to aniline and gave an activity (35.3 h(-1)) similar to 3.3 times higher than that of Co/SiO2 (11.8 h(-1)). The excellent performance was attributed to that Co nanoparticles were doped in the N-C framework where they formed Co-N-x species and that the HSN had a void structure that had a reduced diffusion limitation.

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