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Hydrolase mimic via second coordination sphere engineering in metal-organic frameworks for environmental remediation

Author

Listed:
  • Xin Yuan

    (South China University of Technology)

  • Xiaoling Wu

    (South China University of Technology)

  • Jun Xiong

    (South China University of Technology)

  • Binhang Yan

    (Tsinghua University)

  • Ruichen Gao

    (South China University of Technology)

  • Shuli Liu

    (South China University of Technology)

  • Minhua Zong

    (South China University of Technology)

  • Jun Ge

    (Tsinghua University)

  • Wenyong Lou

    (South China University of Technology)

Abstract

Enzymes achieve high catalytic activity with their elaborate arrangements of amino acid residues in confined optimized spaces. Nevertheless, when exposed to complicated environmental implementation scenarios, including high acidity, organic solvent and high ionic strength, enzymes exhibit low operational stability and poor activity. Here, we report a metal-organic frameworks (MOFs)-based artificial enzyme system via second coordination sphere engineering to achieve high hydrolytic activity under mild conditions. Experiments and theoretical calculations reveal that amide cleavage catalyzed by MOFs follows two distinct catalytic mechanisms, Lewis acid- and hydrogen bonding-mediated hydrolytic processes. The hydrogen bond formed in the secondary coordination sphere exhibits 11-fold higher hydrolytic activity than the Lewis acidic zinc ions. The MOFs exhibit satisfactory degradation performance of toxins and high stability under extreme working conditions, including complicated fermentation broth and high ethanol environments, and display broad substrate specificity. These findings hold great promise for designing artificial enzymes for environmental remediation.

Suggested Citation

  • Xin Yuan & Xiaoling Wu & Jun Xiong & Binhang Yan & Ruichen Gao & Shuli Liu & Minhua Zong & Jun Ge & Wenyong Lou, 2023. "Hydrolase mimic via second coordination sphere engineering in metal-organic frameworks for environmental remediation," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41716-6
    DOI: 10.1038/s41467-023-41716-6
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    1. Sujing Wang & Hong Giang T. Ly & Mohammad Wahiduzzaman & Charlotte Simms & Iurii Dovgaliuk & Antoine Tissot & Guillaume Maurin & Tatjana N. Parac-Vogt & Christian Serre, 2022. "A zirconium metal-organic framework with SOC topological net for catalytic peptide bond hydrolysis," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    2. Kelong Fan & Juqun Xi & Lei Fan & Peixia Wang & Chunhua Zhu & Yan Tang & Xiangdong Xu & Minmin Liang & Bing Jiang & Xiyun Yan & Lizeng Gao, 2018. "In vivo guiding nitrogen-doped carbon nanozyme for tumor catalytic therapy," Nature Communications, Nature, vol. 9(1), pages 1-11, December.
    3. Chao Xie & Longfei Lin & Liang Huang & Zixin Wang & Zhiwei Jiang & Zehui Zhang & Buxing Han, 2021. "Zn-Nx sites on N-doped carbon for aerobic oxidative cleavage and esterification of C(CO)-C bonds," Nature Communications, Nature, vol. 12(1), pages 1-12, December.
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    Cited by:

    1. Yujie Zhang & Jiale Chen & Kaixuan Li & Hongping Wu & Zhanggui Hu & Jiyang Wang & Yicheng Wu & Hongwei Yu, 2024. "LaMg6Ga6S16: a chemical stable divalent lanthanide chalcogenide," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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