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Selective hydrogenation via precise hydrogen bond interactions on catalytic scaffolds

Author

Listed:
  • Song Shi

    (University of Delaware
    Chinese Academy of Sciences)

  • Piaoping Yang

    (University of Delaware)

  • Chaochao Dun

    (Lawrence Berkeley National Laboratory)

  • Weiqing Zheng

    (University of Delaware)

  • Jeffrey J. Urban

    (Lawrence Berkeley National Laboratory)

  • Dionisios G. Vlachos

    (University of Delaware)

Abstract

The active site environment in enzymes has been known to affect catalyst performance through weak interactions with a substrate, but precise synthetic control of enzyme inspired heterogeneous catalysts remains challenging. Here, we synthesize hyper-crosslinked porous polymer (HCPs) with solely -OH or -CH3 groups on the polymer scaffold to tune the environment of active sites. Reaction rate measurements, spectroscopic techniques, along with DFT calculations show that HCP-OH catalysts enhance the hydrogenation rate of H-acceptor substrates containing carbonyl groups whereas hydrophobic HCP- CH3 ones promote non-H bond substrate activation. The functional groups go beyond enhancing substrate adsorption to partially activate the C = O bond and tune the catalytic sites. They also expose selectivity control in the hydrogenation of multifunctional substrates through preferential substrate functional group adsorption. The proposed synthetic strategy opens a new class of porous polymers for selective catalysis.

Suggested Citation

  • Song Shi & Piaoping Yang & Chaochao Dun & Weiqing Zheng & Jeffrey J. Urban & Dionisios G. Vlachos, 2023. "Selective hydrogenation via precise hydrogen bond interactions on catalytic scaffolds," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-36015-z
    DOI: 10.1038/s41467-023-36015-z
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    References listed on IDEAS

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    1. Qi Sun & Sai Wang & Briana Aguila & Xiangju Meng & Shengqian Ma & Feng-Shou Xiao, 2018. "Creating solvation environments in heterogeneous catalysts for efficient biomass conversion," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
    2. Shaobo Dai & Lisa-Marie Funk & Fabian Rabe Pappenheim & Viktor Sautner & Mirko Paulikat & Benjamin Schröder & Jon Uranga & Ricardo A. Mata & Kai Tittmann, 2019. "Low-barrier hydrogen bonds in enzyme cooperativity," Nature, Nature, vol. 573(7775), pages 609-613, September.
    3. Rui Lang & Wei Xi & Jin-Cheng Liu & Yi-Tao Cui & Tianbo Li & Adam Fraser Lee & Fang Chen & Yang Chen & Lei Li & Lin Li & Jian Lin & Shu Miao & Xiaoyan Liu & Ai-Qin Wang & Xiaodong Wang & Jun Luo & Bot, 2019. "Non defect-stabilized thermally stable single-atom catalyst," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
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