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Elucidating the role of metal ions in carbonic anhydrase catalysis

Author

Listed:
  • Jin Kyun Kim

    (Department of Physics, Ulsan National Institute of Science and Technology (UNIST))

  • Cheol Lee

    (Department of Physics, Ulsan National Institute of Science and Technology (UNIST))

  • Seon Woo Lim

    (Department of Physics, Ulsan National Institute of Science and Technology (UNIST))

  • Aniruddha Adhikari

    (Department of Physics, Ulsan National Institute of Science and Technology (UNIST))

  • Jacob T. Andring

    (Department of Biochemistry and Molecular Biology, College of Medicine, University of Florida)

  • Robert McKenna

    (Department of Biochemistry and Molecular Biology, College of Medicine, University of Florida)

  • Cheol-Min Ghim

    (Department of Physics, Ulsan National Institute of Science and Technology (UNIST))

  • Chae Un Kim

    (Department of Physics, Ulsan National Institute of Science and Technology (UNIST))

Abstract

Why metalloenzymes often show dramatic changes in their catalytic activity when subjected to chemically similar but non-native metal substitutions is a long-standing puzzle. Here, we report on the catalytic roles of metal ions in a model metalloenzyme system, human carbonic anhydrase II (CA II). Through a comparative study on the intermediate states of the zinc-bound native CA II and non-native metal-substituted CA IIs, we demonstrate that the characteristic metal ion coordination geometries (tetrahedral for Zn2+, tetrahedral to octahedral conversion for Co2+, octahedral for Ni2+, and trigonal bipyramidal for Cu2+) directly modulate the catalytic efficacy. In addition, we reveal that the metal ions have a long-range (~10 Å) electrostatic effect on restructuring water network in the active site. Our study provides evidence that the metal ions in metalloenzymes have a crucial impact on the catalytic mechanism beyond their primary chemical properties.

Suggested Citation

  • Jin Kyun Kim & Cheol Lee & Seon Woo Lim & Aniruddha Adhikari & Jacob T. Andring & Robert McKenna & Cheol-Min Ghim & Chae Un Kim, 2020. "Elucidating the role of metal ions in carbonic anhydrase catalysis," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-18425-5
    DOI: 10.1038/s41467-020-18425-5
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    Cited by:

    1. Seoyoon Kim & Eojin Kim & Mingyu Park & Seong Ho Kim & Byung-Gyu Kim & Seungjin Na & Victor W. Sadongo & W. C. Bhashini Wijesinghe & Yu-Gon Eom & Gwangsu Yoon & Hannah Jeong & Eunhye Hwang & Chaiheon , 2024. "Hidden route of protein damage through oxygen-confined photooxidation," Nature Communications, Nature, vol. 15(1), pages 1-19, December.

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