Solid solvation structure design improves all-solid-state organic batteries

doi:10.1038/s41557-025-01866-0

. 2025 Aug 4.

doi: 10.1038/s41557-025-01866-0. Online ahead of print.

Solid solvation structure design improves all-solid-state organic batteries

Yang Hu^#¹, Han Su^#^{1

2}, Jiamin Fu^#¹, Jing Luo¹, Qihang Yu³, Feipeng Zhao¹, Weihan Li^{1

4

5}, Sixu Deng^{1

3}, Yu Liu^{1

2}, Yi Yuan¹, Yi Gan¹, Yijia Wang¹, Jung Tae Kim¹, Ning Chen⁶, Mohsen Shakouri⁶, Xiaoge Hao¹, Yingjie Gao¹, Tianlu Pang⁷, Nian Zhang⁷, Ming Jiang⁸, Xia Li³, Yang Zhao¹, Jiangping Tu², Changhong Wang^{9

10

11}, Xueliang Sun^{12

13

14}

Affiliations

¹ Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, Canada.
² School of Materials Science and Engineering, Zhejiang University, Hangzhou, People's Republic of China.
³ Department of Chemical and Materials Engineering, Concordia University, Montreal, Quebec, Canada.
⁴ Eastern Institute for Advanced Study, Eastern Institute of Technology, Nngbo, People's Republic of China.
⁵ Zhejiang Key Laboratory of All-Solid-State Battery, Ningbo Key Laboratory of All-Solid-State Battery, Ningbo, People's Republic of China.
⁶ Canadian Light Source Inc., University of Saskatchewan, Saskatoon, Saskatchewan, Canada.
⁷ Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, People's Republic of China.
⁸ Institute of Physical Science and Information Technology, Anhui University, Hefei, People's Republic of China.
⁹ Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, Canada. cwang@eitech.edu.cn.
¹⁰ Eastern Institute for Advanced Study, Eastern Institute of Technology, Nngbo, People's Republic of China. cwang@eitech.edu.cn.
¹¹ Zhejiang Key Laboratory of All-Solid-State Battery, Ningbo Key Laboratory of All-Solid-State Battery, Ningbo, People's Republic of China. cwang@eitech.edu.cn.
¹² Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, Canada. xsun@eitech.edu.cn.
¹³ Eastern Institute for Advanced Study, Eastern Institute of Technology, Nngbo, People's Republic of China. xsun@eitech.edu.cn.
¹⁴ Zhejiang Key Laboratory of All-Solid-State Battery, Ningbo Key Laboratory of All-Solid-State Battery, Ningbo, People's Republic of China. xsun@eitech.edu.cn.

^# Contributed equally.

PMID: 40759737
DOI: 10.1038/s41557-025-01866-0

Solid solvation structure design improves all-solid-state organic batteries

Yang Hu et al. Nat Chem. 2025.

. 2025 Aug 4.

doi: 10.1038/s41557-025-01866-0. Online ahead of print.

Authors

Affiliations

¹ Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, Canada.
² School of Materials Science and Engineering, Zhejiang University, Hangzhou, People's Republic of China.
³ Department of Chemical and Materials Engineering, Concordia University, Montreal, Quebec, Canada.
⁴ Eastern Institute for Advanced Study, Eastern Institute of Technology, Nngbo, People's Republic of China.
⁵ Zhejiang Key Laboratory of All-Solid-State Battery, Ningbo Key Laboratory of All-Solid-State Battery, Ningbo, People's Republic of China.
⁶ Canadian Light Source Inc., University of Saskatchewan, Saskatoon, Saskatchewan, Canada.
⁷ Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, People's Republic of China.
⁸ Institute of Physical Science and Information Technology, Anhui University, Hefei, People's Republic of China.
⁹ Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, Canada. cwang@eitech.edu.cn.
¹⁰ Eastern Institute for Advanced Study, Eastern Institute of Technology, Nngbo, People's Republic of China. cwang@eitech.edu.cn.
¹¹ Zhejiang Key Laboratory of All-Solid-State Battery, Ningbo Key Laboratory of All-Solid-State Battery, Ningbo, People's Republic of China. cwang@eitech.edu.cn.
¹² Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, Canada. xsun@eitech.edu.cn.
¹³ Eastern Institute for Advanced Study, Eastern Institute of Technology, Nngbo, People's Republic of China. xsun@eitech.edu.cn.
¹⁴ Zhejiang Key Laboratory of All-Solid-State Battery, Ningbo Key Laboratory of All-Solid-State Battery, Ningbo, People's Republic of China. xsun@eitech.edu.cn.

^# Contributed equally.

PMID: 40759737
DOI: 10.1038/s41557-025-01866-0

Abstract

Organic electrode materials offer a versatile, sustainable approach for next-generation lithium-ion batteries but are limited by low working voltages and poor cycling stability. Here we report a solid-solvation-structure design strategy to improve both the voltage and stability of organic electrode materials in all-solid-state batteries. As a proof of concept, we incorporate halide electrolytes as solid solutes and tetrachloro-o-benzoquinone as a solid solvent to form homogeneous solid cathode solutions. Systematic optimization of the inner solvation configuration enables tetrachloro-o-benzoquinone to achieve a high working voltage (3.6 V vs. Li⁺/Li) at room temperature within an asymmetric solid solvation sheath. Moreover, the equilibrium redox pathway and electrostatically driven self-healing interfaces revealed rapid redox kinetics and stable performance over 7,500 cycles in all-solid-state batteries under low stack pressures. This work demonstrates that organic electrode materials can serve as viable, durable and cost-effective alternatives to transition metal oxides in all-solid-state batteries.

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Conflict of interest statement

Competing interests: The authors declare no competing interests.

References

1. Williams, D., Byrne, J. & Driscoll, J. A high energy density lithium/dichloroisocyanuric acid battery system. J. Electrochem. Soc. 116, 2 (1969).
1. Lu, Y. & Chen, J. Prospects of organic electrode materials for practical lithium batteries. Nat. Rev. Chem. 4, 127–142 (2020).
1. Lu, Y., Zhang, Q., Li, L., Niu, Z. Q. & Chen, J. Design strategies toward enhancing the performance of organic electrode materials in metal-ion batteries. Chem 4, 2786–2813 (2018).
1. Armand, M. et al. Conjugated dicarboxylate anodes for Li-ion batteries. Nat. Mater. 8, 120–125 (2009).
1. Hu, J. et al. Emerging organic electrodes for Na-ion and K-ion batteries. Energy Storage Mater. 56, 267–299 (2023).

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[1] Williams, D., Byrne, J. & Driscoll, J. A high energy density lithium/dichloroisocyanuric acid battery system. J. Electrochem. Soc. 116, 2 (1969).

[2] Williams, D., Byrne, J. & Driscoll, J. A high energy density lithium/dichloroisocyanuric acid battery system. J. Electrochem. Soc. 116, 2 (1969).

[3] Lu, Y. & Chen, J. Prospects of organic electrode materials for practical lithium batteries. Nat. Rev. Chem. 4, 127–142 (2020).

[4] Lu, Y. & Chen, J. Prospects of organic electrode materials for practical lithium batteries. Nat. Rev. Chem. 4, 127–142 (2020).

[5] Lu, Y., Zhang, Q., Li, L., Niu, Z. Q. & Chen, J. Design strategies toward enhancing the performance of organic electrode materials in metal-ion batteries. Chem 4, 2786–2813 (2018).

[6] Lu, Y., Zhang, Q., Li, L., Niu, Z. Q. & Chen, J. Design strategies toward enhancing the performance of organic electrode materials in metal-ion batteries. Chem 4, 2786–2813 (2018).

[7] Armand, M. et al. Conjugated dicarboxylate anodes for Li-ion batteries. Nat. Mater. 8, 120–125 (2009).

[8] Armand, M. et al. Conjugated dicarboxylate anodes for Li-ion batteries. Nat. Mater. 8, 120–125 (2009).

[9] Hu, J. et al. Emerging organic electrodes for Na-ion and K-ion batteries. Energy Storage Mater. 56, 267–299 (2023).

[10] Hu, J. et al. Emerging organic electrodes for Na-ion and K-ion batteries. Energy Storage Mater. 56, 267–299 (2023).

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Solid solvation structure design improves all-solid-state organic batteries

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Solid solvation structure design improves all-solid-state organic batteries

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Abstract

Conflict of interest statement

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Abstract

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