4.8 Article

A versatile route to fabricate single atom catalysts with high chemoselectivity and regioselectivity in hydrogenation

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NATURE COMMUNICATIONS
卷 10, 期 -, 页码 -

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NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-019-11619-6

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资金

  1. National Natural Science Foundation of China [21606260, 21576302, 21376278, 21725301, 21821004, 91645115]
  2. National Science Foundation for Distinguished Young Scholars of China [21425627]
  3. NSF of Guangdong Province [2015A030313104]
  4. Fundamental Research Funds for the Central Universities of Sun Yat-sen University [15lgjc33, 16lgpy15]
  5. National Key R&D Program of China [2017YFB0602200]
  6. Features Innovative Projects of Department of Education of Guangdong Province [2016KTSCX003]
  7. Local Innovative and Research Teams Project of Guangdong Pearl Rivers Talents Program [2017BT01C102]

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Preparation of single atom catalysts (SACs) is of broad interest to materials scientists and chemists but remains a formidable challenge. Herein, we develop an efficient approach to synthesize SACs via a precursor-dilution strategy, in which metalloporphyrin (MTPP) with target metals are co-polymerized with diluents (tetraphenylporphyrin, TPP), followed by pyrolysis to N-doped porous carbon supported SACs (M-1/N-C). Twenty-four different SACs, including noble metals and non-noble metals, are successfully prepared. In addition, the synthesis of a series of catalysts with different surface atom densities, bi-metallic sites, and metal aggregation states are achieved. This approach shows remarkable adjustability and generality, providing sufficient freedom to design catalysts at atomic-scale and explore the unique catalytic properties of SACs. As an example, we show that the prepared Pt-1/N-C exhibits superior chemoselectivity and regioselectivity in hydrogenation. It only converts terminal alkynes to alkenes while keeping other reducible functional groups such as alkenyl, nitro group, and even internal alkyne intact.

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