Electron Donors in the Intertwined Interface Restore Oxy-Substituted Selenides

Yuanhe Sun; Junwei Yang; Wei Zhang; Haitao Li; Mengru Lin; Hao Shi; Yi Gao; Wen Wen; Chunyi Zhi; Xiaolong Li; Daming Zhu

doi:10.1021/jacs.5c08194

Electron Donors in the Intertwined Interface Restore Oxy-Substituted Selenides

Yuanhe Sun (Co-first Author), Junwei Yang (Co-first Author), Wei Zhang (Co-first Author), Haitao Li, Mengru Lin, Hao Shi, Yi Gao, Wen Wen, Chunyi Zhi^*, Xiaolong Li^*, Daming Zhu^*

^*Corresponding author for this work

Department of Materials Science and Engineering

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

2 Citations (Scopus)

Abstract

Nature chose selenium as the antioxidant element center in proteins, permitting the reversible conversion of organic bioenzymes between oxidized and selenized forms. Despite the importance of such antielectronegativity reversibility, it has not yet been demonstrated in inorganic selenides. We report an unexpected example showing that oxy-substituted sites in metal selenides can be restored to selenized forms reversibly by mild electrochemical manipulation in a copper aqueous solution. Synchrotron measurements of the localized lattice and bond structure suggest that copper as an electron donor can transfer extra electrons to oxidized metal centers via the O-V-Se-Cu-bonded bridge path in the deep-intertwined interface to confer rare reversibility. We demonstrate that such reversibility is generalized in vanadium diselenide and manganese diselenides/selenides, offering the possibility of applying promising selenides in widespread aqueous systems. © 2025 American Chemical Society

Original language	English
Pages (from-to)	28151-28160
Journal	Journal of the American Chemical Society
Volume	147
Issue number	31
Online published	25 Jul 2025
DOIs	https://doi.org/10.1021/jacs.5c08194
Publication status	Published - 6 Aug 2025

Funding

Y.S., J.Y., and W.Z. contributed equally to this work. D.Z. acknowledges supports from National Key Research and Development Programme of China (No. 2022YFA1605400), National Natural Science Foundation of China (No. 12275342), Youth Innovation Promotion Association of the Chinese Academy of Sciences (2022293), Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB1170000), and Photon Science Research Center for Carbon Dioxide. Y.S. acknowledges support from the Shanghai Sailing Program (No. 23YF1453500). The authors thank Dr. Zeying Yao and Dr. Zhiguo Ren for their contributions to earlier explorations. The authors thank Prof. Yang Yue for his generous support in TEM characterization. This work was also supported by BL02U2, BL16U1, BL13SSW, BL17B, E-Line (BL20U1), and the User Experiment Assist System of Shanghai Synchrotron Radiation Facility (SSRF). The authors thank all the staff of the above beamlines and systems for their support.

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title = "Electron Donors in the Intertwined Interface Restore Oxy-Substituted Selenides",

abstract = "Nature chose selenium as the antioxidant element center in proteins, permitting the reversible conversion of organic bioenzymes between oxidized and selenized forms. Despite the importance of such antielectronegativity reversibility, it has not yet been demonstrated in inorganic selenides. We report an unexpected example showing that oxy-substituted sites in metal selenides can be restored to selenized forms reversibly by mild electrochemical manipulation in a copper aqueous solution. Synchrotron measurements of the localized lattice and bond structure suggest that copper as an electron donor can transfer extra electrons to oxidized metal centers via the O-V-Se-Cu-bonded bridge path in the deep-intertwined interface to confer rare reversibility. We demonstrate that such reversibility is generalized in vanadium diselenide and manganese diselenides/selenides, offering the possibility of applying promising selenides in widespread aqueous systems. {\textcopyright} 2025 American Chemical Society",

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Electron Donors in the Intertwined Interface Restore Oxy-Substituted Selenides. / Sun, Yuanhe (Co-first Author); Yang, Junwei (Co-first Author); Zhang, Wei (Co-first Author) et al.
In: Journal of the American Chemical Society, Vol. 147, No. 31, 06.08.2025, p. 28151-28160.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Electron Donors in the Intertwined Interface Restore Oxy-Substituted Selenides

AU - Sun, Yuanhe

AU - Yang, Junwei

AU - Zhang, Wei

AU - Li, Haitao

AU - Lin, Mengru

AU - Shi, Hao

AU - Gao, Yi

AU - Wen, Wen

AU - Zhi, Chunyi

AU - Li, Xiaolong

AU - Zhu, Daming

PY - 2025/8/6

Y1 - 2025/8/6

N2 - Nature chose selenium as the antioxidant element center in proteins, permitting the reversible conversion of organic bioenzymes between oxidized and selenized forms. Despite the importance of such antielectronegativity reversibility, it has not yet been demonstrated in inorganic selenides. We report an unexpected example showing that oxy-substituted sites in metal selenides can be restored to selenized forms reversibly by mild electrochemical manipulation in a copper aqueous solution. Synchrotron measurements of the localized lattice and bond structure suggest that copper as an electron donor can transfer extra electrons to oxidized metal centers via the O-V-Se-Cu-bonded bridge path in the deep-intertwined interface to confer rare reversibility. We demonstrate that such reversibility is generalized in vanadium diselenide and manganese diselenides/selenides, offering the possibility of applying promising selenides in widespread aqueous systems. © 2025 American Chemical Society

AB - Nature chose selenium as the antioxidant element center in proteins, permitting the reversible conversion of organic bioenzymes between oxidized and selenized forms. Despite the importance of such antielectronegativity reversibility, it has not yet been demonstrated in inorganic selenides. We report an unexpected example showing that oxy-substituted sites in metal selenides can be restored to selenized forms reversibly by mild electrochemical manipulation in a copper aqueous solution. Synchrotron measurements of the localized lattice and bond structure suggest that copper as an electron donor can transfer extra electrons to oxidized metal centers via the O-V-Se-Cu-bonded bridge path in the deep-intertwined interface to confer rare reversibility. We demonstrate that such reversibility is generalized in vanadium diselenide and manganese diselenides/selenides, offering the possibility of applying promising selenides in widespread aqueous systems. © 2025 American Chemical Society

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Electron Donors in the Intertwined Interface Restore Oxy-Substituted Selenides

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