Deciphering multi-dimensional interfacial mechanisms via organic cosolvent engineering for sustainable zinc metal batteries
Abstract Introducing organic cosolvent is a common and cost-effective electrolyte engineering for aqueous Zn-battery, reshaping the solvation environment of electrolyte and modulating the interfacial electrochemistry on Zn-metal electrode. Clarifying the mechanisms governing interfacial dynamic evol...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-04-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-59069-7 |
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| author | Xiaoyu Yu Ming Chen Junhao Wang Shiqi Li Haitang Zhang Qingao Zhao Haiyan Luo Yaping Deng Hanfeng Liang Jiang Zhou Fei Wang Dongliang Chao Yeguo Zou Guang Feng Yu Qiao Shi-Gang Sun |
| author_facet | Xiaoyu Yu Ming Chen Junhao Wang Shiqi Li Haitang Zhang Qingao Zhao Haiyan Luo Yaping Deng Hanfeng Liang Jiang Zhou Fei Wang Dongliang Chao Yeguo Zou Guang Feng Yu Qiao Shi-Gang Sun |
| author_sort | Xiaoyu Yu |
| collection | DOAJ |
| description | Abstract Introducing organic cosolvent is a common and cost-effective electrolyte engineering for aqueous Zn-battery, reshaping the solvation environment of electrolyte and modulating the interfacial electrochemistry on Zn-metal electrode. Clarifying the mechanisms governing interfacial dynamic evolution and electrochemical performance is essential for guiding cosolvent selection. However, the absence of direct visualization for dynamic interfacial evolution during Zn plating/stripping has impeded mechanistic understanding of cosolvent-mediated effects in electrolyte engineering. Here, we combine advanced in-situ spectroscopy with theoretical calculation to decouple the interfacial evolution at the molecular level. We find that cosolvents not only weaken the connectivity of the interfacial hydrogen-bond network between water molecules, thereby hindering the H+ transfer, but also accelerate the interfacial dynamic transition of Zn2+-(de)solvation from transient to steady state. Additionally, we observe a dynamic adsorption substitution between cosolvent and water, which weakens the electric field intensity exerted on interfacial water. Furthermore, we demonstrate that cosolvents can modify the components content and distribution of the passivation-layer via indirect regulation pathway, rather than a typical self-decomposition mechanism. These multidimensional insights bridge the knowledge gap in cosolvent functionality, offering rational principles for tailoring solvation structures and interfacial dynamics in next-generation aqueous batteries. |
| format | Article |
| id | doaj-art-c771f4e42d5b4c42a262cf02170b5842 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-c771f4e42d5b4c42a262cf02170b58422025-08-20T03:53:32ZengNature PortfolioNature Communications2041-17232025-04-0116111410.1038/s41467-025-59069-7Deciphering multi-dimensional interfacial mechanisms via organic cosolvent engineering for sustainable zinc metal batteriesXiaoyu Yu0Ming Chen1Junhao Wang2Shiqi Li3Haitang Zhang4Qingao Zhao5Haiyan Luo6Yaping Deng7Hanfeng Liang8Jiang Zhou9Fei Wang10Dongliang Chao11Yeguo Zou12Guang Feng13Yu Qiao14Shi-Gang Sun15State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology (HUST)State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology (HUST)State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversitySchool of Materials Science and Engineering, Hunan Provincial Key Laboratory of Electronic Packaging and Advanced Functional Materials, Central South UniversityDepartment of Chemistry, Department of Materials Science, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan UniversityLaboratory of Advanced Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, School of Chemistry and Materials, Fudan UniversityState Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology (HUST)State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityState Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen UniversityAbstract Introducing organic cosolvent is a common and cost-effective electrolyte engineering for aqueous Zn-battery, reshaping the solvation environment of electrolyte and modulating the interfacial electrochemistry on Zn-metal electrode. Clarifying the mechanisms governing interfacial dynamic evolution and electrochemical performance is essential for guiding cosolvent selection. However, the absence of direct visualization for dynamic interfacial evolution during Zn plating/stripping has impeded mechanistic understanding of cosolvent-mediated effects in electrolyte engineering. Here, we combine advanced in-situ spectroscopy with theoretical calculation to decouple the interfacial evolution at the molecular level. We find that cosolvents not only weaken the connectivity of the interfacial hydrogen-bond network between water molecules, thereby hindering the H+ transfer, but also accelerate the interfacial dynamic transition of Zn2+-(de)solvation from transient to steady state. Additionally, we observe a dynamic adsorption substitution between cosolvent and water, which weakens the electric field intensity exerted on interfacial water. Furthermore, we demonstrate that cosolvents can modify the components content and distribution of the passivation-layer via indirect regulation pathway, rather than a typical self-decomposition mechanism. These multidimensional insights bridge the knowledge gap in cosolvent functionality, offering rational principles for tailoring solvation structures and interfacial dynamics in next-generation aqueous batteries.https://doi.org/10.1038/s41467-025-59069-7 |
| spellingShingle | Xiaoyu Yu Ming Chen Junhao Wang Shiqi Li Haitang Zhang Qingao Zhao Haiyan Luo Yaping Deng Hanfeng Liang Jiang Zhou Fei Wang Dongliang Chao Yeguo Zou Guang Feng Yu Qiao Shi-Gang Sun Deciphering multi-dimensional interfacial mechanisms via organic cosolvent engineering for sustainable zinc metal batteries Nature Communications |
| title | Deciphering multi-dimensional interfacial mechanisms via organic cosolvent engineering for sustainable zinc metal batteries |
| title_full | Deciphering multi-dimensional interfacial mechanisms via organic cosolvent engineering for sustainable zinc metal batteries |
| title_fullStr | Deciphering multi-dimensional interfacial mechanisms via organic cosolvent engineering for sustainable zinc metal batteries |
| title_full_unstemmed | Deciphering multi-dimensional interfacial mechanisms via organic cosolvent engineering for sustainable zinc metal batteries |
| title_short | Deciphering multi-dimensional interfacial mechanisms via organic cosolvent engineering for sustainable zinc metal batteries |
| title_sort | deciphering multi dimensional interfacial mechanisms via organic cosolvent engineering for sustainable zinc metal batteries |
| url | https://doi.org/10.1038/s41467-025-59069-7 |
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