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手性生物晶体中电子自旋与质子转移之间的耦合。

Coupling between electrons' spin and proton transfer in chiral biological crystals.

作者信息

Goren Naama, Pandurangan Perumal, Eisenberg-Domovich Yael, Yochelis Shira, Keren Nir, Ansermet Jean-Philippe, Naaman Ron, Livnah Oded, Ashkenasy Nurit, Paltiel Yossi

机构信息

Department of Applied Physics, Center for nanoscience and Nanotechnology, Hebrew University of Jerusalem, Jerusalem 9190401, Israel.

Department of Materials Engineering, Ilse Katz Institute for Nanoscale Science and Technology, Ben-Gurion University of the Negev, Beer-Sheva 84105, Israel.

出版信息

Proc Natl Acad Sci U S A. 2025 May 13;122(19):e2500584122. doi: 10.1073/pnas.2500584122. Epub 2025 May 8.

DOI:10.1073/pnas.2500584122
PMID:40339126
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12088416/
Abstract

Proton transport plays a fundamental role in many biological and chemical systems. In life, proton transport is crucial for biochemical and physiological functions. It is usually accepted that the main mechanism of proton transfer is a result of hopping between neighboring water molecules and amino acid side chains. It was recently suggested that the proton transfer can be simultaneously coupled with electron transfer. As life is homochiral, proton transfer in biology is occurring in a chiral environment. In this environment, the chiral-induced spin selectivity effect relating to electron transfer and chirality is expected to occur. The present work establishes that the proton transfer is coupled to a specific electron spin polarization in lysozyme crystals, associating proton transfer to electron movement and polarization. To preserve total angular momentum, this motion may be coupled to chiral phonons that propagate in the crystal. Our work shows that the interaction of the electrons' spin and phonons is very significant in proton transfer through lysosome crystals. Injecting the opposite electron spin into the lysosome crystal results in a significant change in proton transfer impedance. This study presents the support for the proton-coupled electron transfer mechanism and indicates the importance of spin polarization in the process.

摘要

质子传输在许多生物和化学系统中起着基础性作用。在生命过程中,质子传输对于生物化学和生理功能至关重要。通常认为,质子转移的主要机制是相邻水分子和氨基酸侧链之间跳跃的结果。最近有人提出,质子转移可以与电子转移同时发生耦合。由于生命是手性的,生物学中的质子转移发生在手性环境中。在这种环境下,预计会出现与电子转移和手性相关的手性诱导自旋选择性效应。目前的工作证实,在溶菌酶晶体中质子转移与特定的电子自旋极化相耦合,将质子转移与电子运动和极化联系起来。为了保持总角动量,这种运动可能与在晶体中传播的手性声子相耦合。我们的工作表明,电子自旋与声子的相互作用在质子通过溶酶体晶体的传输过程中非常重要。向溶酶体晶体中注入相反的电子自旋会导致质子转移阻抗发生显著变化。这项研究为质子耦合电子转移机制提供了支持,并表明了自旋极化在该过程中的重要性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c324/12088416/213b577db9d4/pnas.2500584122fig05.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c324/12088416/fb06278e735e/pnas.2500584122fig01.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c324/12088416/8eb94ccdbfb1/pnas.2500584122fig02.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c324/12088416/7da56b7fa0a3/pnas.2500584122fig03.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c324/12088416/decef381c2e7/pnas.2500584122fig04.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c324/12088416/213b577db9d4/pnas.2500584122fig05.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c324/12088416/fb06278e735e/pnas.2500584122fig01.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c324/12088416/8eb94ccdbfb1/pnas.2500584122fig02.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c324/12088416/7da56b7fa0a3/pnas.2500584122fig03.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c324/12088416/decef381c2e7/pnas.2500584122fig04.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c324/12088416/213b577db9d4/pnas.2500584122fig05.jpg

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本文引用的文献

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Chem Mater. 2024 Nov 20;36(23):11449-11461. doi: 10.1021/acs.chemmater.4c02108. eCollection 2024 Dec 10.
2
Long-Range Proton Channels Constructed via Hierarchical Peptide Self-Assembly.通过分级肽自组装构建的远程质子通道
Adv Mater. 2024 Dec;36(50):e2409248. doi: 10.1002/adma.202409248. Epub 2024 Nov 12.
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Second harmonic generation at a time-varying interface.
时变界面处的二次谐波产生
Nat Commun. 2024 Sep 5;15(1):7752. doi: 10.1038/s41467-024-51588-z.
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Chiral Induced Spin Selectivity.手性诱导自旋选择性
Chem Rev. 2024 Feb 28;124(4):1950-1991. doi: 10.1021/acs.chemrev.3c00661. Epub 2024 Feb 16.
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Phonon-assisted electron-proton transfer in [FeFe] hydrogenases: Topological role of clusters.[FeFe]氢化酶中的声子辅助电子-质子转移:簇的拓扑作用。
Biophys J. 2023 Apr 18;122(8):1557-1567. doi: 10.1016/j.bpj.2023.03.027. Epub 2023 Mar 23.
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Chiral-phonon-activated spin Seebeck effect.手性声子激活的自旋塞贝克效应。
Nat Mater. 2023 Mar;22(3):322-328. doi: 10.1038/s41563-023-01473-9. Epub 2023 Feb 13.
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Detecting nonlocality by second-harmonic generation from a graphene-wrapped nanoparticle.通过石墨烯包裹的纳米颗粒的二次谐波产生来检测非局域性。
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Nonlinear Reaction Coordinate of an Enzyme Catalyzed Proton Transfer Reaction.酶催化质子转移反应的非线性反应坐标
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