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Physical Origin of Thermostabilization by a Quadruple Mutation for the Adenosine A2a Receptor in the Active State
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    Physical Origin of Thermostabilization by a Quadruple Mutation for the Adenosine A2a Receptor in the Active State
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    • Yuta Kajiwara
      Yuta Kajiwara
      Graduate School of Energy Science, Kyoto University, Uji, Kyoto 611-0011, Japan
    • Satoshi Yasuda
      Satoshi Yasuda
      Graduate School of Science, Chiba University, 1-33 Yayoi-cho, Inage, Chiba 263-8522, Japan
      Molecular Chirality Research Center, Chiba University, 1-33 Yayoi-cho, Inage, Chiba 263-8522, Japan
      Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
    • Simon Hikiri
      Simon Hikiri
      Graduate School of Science, Chiba University, 1-33 Yayoi-cho, Inage, Chiba 263-8522, Japan
      Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
      More by Simon Hikiri
    • Tomohiko Hayashi
      Tomohiko Hayashi
      Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
    • Mitsunori Ikeguchi
      Mitsunori Ikeguchi
      Graduate School of Medical Life Science, Yokohama City University, 1-7-29 Suehiro-cho, Tsurumi-ku, Yokohama 230-0045, Japan
      RIKEN Medical Sciences Innovation Hub Program, 1-7-22 Suehiro-cho, Tsurumi-ku, Yokohama 230-0045, Japan
    • Takeshi Murata*
      Takeshi Murata
      Graduate School of Science, Chiba University, 1-33 Yayoi-cho, Inage, Chiba 263-8522, Japan
      Molecular Chirality Research Center, Chiba University, 1-33 Yayoi-cho, Inage, Chiba 263-8522, Japan
      JST, PRESTO, 1-33 Yayoi-cho, Inage, Chiba 263-8522, Japan
      *E-mail: [email protected]. Tel.: +81-43-290-2794.
    • Masahiro Kinoshita*
      Masahiro Kinoshita
      Institute of Advanced Energy, Kyoto University, Uji, Kyoto 611-0011, Japan
      *E-mail: [email protected]. Tel.: +81-774-38-3503.
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    The Journal of Physical Chemistry B

    Cite this: J. Phys. Chem. B 2018, 122, 16, 4418–4427
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    https://doi.org/10.1021/acs.jpcb.8b00443
    Published April 4, 2018
    Copyright © 2018 American Chemical Society

    Abstract

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    The G protein-coupled receptors (GPCRs) form a large, physiologically important family of membrane proteins and are currently the most attractive targets for drug discovery. We investigate the physical origin of thermostabilization of the adenosine A2a receptor (A2aR) in the active state, which was experimentally achieved by another research group using the four point mutations: L48A, A54L, T65A, and Q89A. The investigation is performed on the basis of our recently developed physics-based free-energy function (FEF), which has been quite successful for the thermodynamics of GPCRs in the inactive state. The experimental condition for solving the wild-type and mutant crystal structures was substantially different from that for comparing their thermostabilities. Therefore, all-atom molecular dynamics simulations are necessitated, which also allows us to account for the structural fluctuations of the membrane protein. We show that the quadruple mutation leads to the enlargement of the solvent–entropy gain upon protein folding. The solvent is formed by hydrocarbon groups constituting nonpolar chains within the lipid bilayer, and the entropy is relevant to the thermal motion of the hydrocarbon groups. From an energetic point of view (e.g., in terms of protein intramolecular hydrogen bonds), the mutation confers no improvement upon the structural stability of A2aR. The reliability of our FEF and the crucial importance of the solvent-entropy effect have thus been demonstrated for a GPCR in the active state. We are now ready to identify thermostabilizing mutations of GPCRs not only in the inactive state but also in the active one.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcb.8b00443.

    • Descriptions of the entropic excluded-volume effect by the solvent, the protein intramolecular hydrogen bonding, the solvent model, the application to GPCR folding, the calculation of the solvent–entropy gain upon GPCR folding, and the calculation of the lowering of the intramolecular electrostatic energy upon GPCR folding (PDF)

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    Cited By

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    This article is cited by 8 publications.

    1. Satoshi Yasuda, Tomoki Akiyama, Keiichi Kojima, Tetsuya Ueta, Tomohiko Hayashi, Satoshi Ogasawara, Satoru Nagatoishi, Kouhei Tsumoto, Naoki Kunishima, Yuki Sudo, Masahiro Kinoshita, Takeshi Murata. Development of an Outward Proton Pumping Rhodopsin with a New Record in Thermostability by Means of Amino Acid Mutations. The Journal of Physical Chemistry B 2022, 126 (5) , 1004-1015. https://doi.org/10.1021/acs.jpcb.1c08684
    2. Satoshi Yasuda, Tomoki Akiyama, Sayaka Nemoto, Tomohiko Hayashi, Tetsuya Ueta, Keiichi Kojima, Takashi Tsukamoto, Satoru Nagatoishi, Kouhei Tsumoto, Yuki Sudo, Masahiro Kinoshita, Takeshi Murata. Methodology for Further Thermostabilization of an Intrinsically Thermostable Membrane Protein Using Amino Acid Mutations with Its Original Function Being Retained. Journal of Chemical Information and Modeling 2020, 60 (3) , 1709-1716. https://doi.org/10.1021/acs.jcim.0c00063
    3. Tomohiko Hayashi, Satoshi Yasuda, Kano Suzuki, Tomoki Akiyama, Kanae Kanehara, Keiichi Kojima, Mikio Tanabe, Ryuichi Kato, Toshiya Senda, Yuki Sudo, Takeshi Murata, Masahiro Kinoshita. How Does a Microbial Rhodopsin RxR Realize Its Exceptionally High Thermostability with the Proton-Pumping Function Being Retained?. The Journal of Physical Chemistry B 2020, 124 (6) , 990-1000. https://doi.org/10.1021/acs.jpcb.9b10700
    4. Taisei Yamamoto, Satoshi Yasuda, Rinshi S. Kasai, Ryosuke Nakano, Simon Hikiri, Kanna Sugaya, Tomohiko Hayashi, Satoshi Ogasawara, Mitsunori Shiroishi, Takahiro K. Fujiwara, Masahiro Kinoshita, Takeshi Murata. A methodology for creating mutants of G‐protein coupled receptors stabilized in active state by combining statistical thermodynamics and evolutionary molecular engineering. Protein Science 2022, 31 (10) https://doi.org/10.1002/pro.4425
    5. Kanna Sugaya, Satoshi Yasuda, Shingo Sato, Chen Sisi, Taisei Yamamoto, Daisuke Umeno, Tomoaki Matsuura, Tomohiko Hayashi, Satoshi Ogasawara, Masahiro Kinoshita, Takeshi Murata. A methodology for creating thermostabilized mutants of G‐protein coupled receptors by combining statistical thermodynamics and evolutionary molecular engineering. Protein Science 2022, 31 (9) https://doi.org/10.1002/pro.4404
    6. Takeshi Murata, Satoshi Yasuda, Tomohiko Hayashi, Masahiro Kinoshita. Theoretical identification of thermostabilizing amino acid mutations for G-protein-coupled receptors. Biophysical Reviews 2020, 12 (2) , 323-332. https://doi.org/10.1007/s12551-020-00678-5
    7. Satoshi Yasuda, Kazuki Kazama, Tomoki Akiyama, Masahiro Kinoshita, Takeshi Murata. Elucidation of cosolvent effects thermostabilizing water-soluble and membrane proteins. Journal of Molecular Liquids 2020, 301 , 112403. https://doi.org/10.1016/j.molliq.2019.112403
    8. Satoshi Yasuda, Tomohiko Hayashi, Yuta Kajiwara, Takeshi Murata, Masahiro Kinoshita. Analyses based on statistical thermodynamics for large difference between thermophilic rhodopsin and xanthorhodopsin in terms of thermostability. The Journal of Chemical Physics 2019, 150 (5) https://doi.org/10.1063/1.5082217

    The Journal of Physical Chemistry B

    Cite this: J. Phys. Chem. B 2018, 122, 16, 4418–4427
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpcb.8b00443
    Published April 4, 2018
    Copyright © 2018 American Chemical Society

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