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Vol. 18 (2026)

Self-Assembled Ordered Nanostructure of Zwitterionic Co-Solutes Induces Localized High-Concentration Electrolytes for Ultrastable and Efficient Zinc Metal Anodes

https://doi.org/10.1007/s40820-025-02040-4
Shengyang Huang
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑Ro, Jangan‑Gu, Suwon 16419, Republic of Korea
Zuyang Hu
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑Ro, Jangan‑Gu, Suwon 16419, Republic of Korea
Xin Wang Mo
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑Ro, Jangan‑Gu, Suwon 16419, Republic of Korea
Yeonju Park
Department of Chemistry, Institute for Molecular Science and Fusion Technology, Kangwon National University, Chuncheon 24341, Republic of Korea
Jun Su Kim
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑Ro, Jangan‑Gu, Suwon 16419, Republic of Korea
Gun Jang
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑Ro, Jangan‑Gu, Suwon 16419, Republic of Korea
Dong Hyun Min
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑Ro, Jangan‑Gu, Suwon 16419, Republic of Korea
Hao Fu
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑Ro, Jangan‑Gu, Suwon 16419, Republic of Korea
Peixun Xiong
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑Ro, Jangan‑Gu, Suwon 16419, Republic of Korea
Zhipeng Wen
Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, People’s Republic of China
Young Mee Jung
Department of Chemistry, Institute for Molecular Science and Fusion Technology, Kangwon National University, Chuncheon 24341, Republic of Korea
Jaeyun Kim
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑Ro, Jangan‑Gu, Suwon 16419, Republic of Korea
Hyunjoo Lee
Clean Energy Center, Institute of Science and Technology (KIST), 5, Hwarang‑Ro 14‑Gil, Seongbuk‑Gu, Seoul 02792, Republic of Korea
Chihyun Hwang
Advanced Batteries Research Center, Korea Electronics Technology Institute (KETI), 25, Saenari‑Ro, Seongnam 13509, Republic of Korea
Youngkwon Kim
Advanced Batteries Research Center, Korea Electronics Technology Institute (KETI), 25, Saenari‑Ro, Seongnam 13509, Republic of Korea
Cheng Chao Li
Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, People’s Republic of China
Qingyun Dou
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑Ro, Jangan‑Gu, Suwon 16419, Republic of Korea
Ho Seok Park
School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu‑Ro, Jangan‑Gu, Suwon 16419, Republic of Korea

Corresponding Author: Qingyun Dou

douqy3@mail.sysu.edu.cn

Nano-Micro Letters, Vol. 18 (2026), Article Number: 194

Abstract

Localized high-concentration electrolytes (LHCEs) are considered as promising electrolyte candidates to resolve technical issues of metal batteries owing to their unique interfacial properties and solvation structures. Herein, we propose a self-assembly chemical strategy into the LCHEs induced by ordered nanostructure of zwitterionic co-solutes for highly efficient and ultrastable zinc (Zn) metal batteries. Through the systematic screening of six zwitterionic compounds, 3-(decyldimethylammonio)propanesulfonate salt (C10) with the decyl chain and zwitterions was determined as an optimum to construct quasi-spherical aggregates with a periodic length of 3.77 nm, as confirmed by comprehensive synchronous small-angle X-ray scattering, Guinier, pair distance distribution function, Porod, and other spectroscopic characterizations and molecular dynamic simulation. In particularly, this self-assembled structure in electrolyte environments was attributed to increasing the proportion of both contact and aggregated ion pairs for the formation of LHCEs as well as to providing fast and selective Zn2+ conducting channels and uniform solid electrolyte interfaces for facilitated charge transfer kinetics. Moreover, the preferential adsorption of the self-assembled C10 on the Zn(002) surface modulated the electrical double layer to suppress hydrogen evolution and corrosion reactions. Consequently, the Zn||Zn symmetric cells in Zn(OTf)2/C10 electrolytes showed long-term plating/stripping behaviors over 2800 h at 1 mA cm−2 and 1 mAh cm−2 as well as over 1200 h even at 5 mA cm−2 and 5 mAh cm−2 with a very high depth of discharge of 42.7%. Furthermore, the Zn||VO2/CNT full cells in Zn(OTf)2/C10 electrolytes delivered a record-high capacity of 8.10 mAh cm−2 at an ultrahigh cathode mass loading of 50 mg cm−2 after 150 cycles.


Highlights:
1 Self-assembled zwitterion (C10) induces localized high-concentration electrolytes, regulating Zn2+ solvation, guiding selective ion transport, and enabling uniform solid electrolyte interface formation.
2 A comprehensive set of advanced analyses (Guinier, PDDF, Porod) combined with spectroscopy and simulations reveals that C10 self-assembles into ~3.8 nm quasi-spherical aggregates and bilayer-like interfacial structures.
3 C10 enables ultrastable cycling (>2800 h) in symmetric cells and record areal capacity (8.1 mAh cm−2 at 50 mg cm−2) in Zn||VO2/CNT full cells, highlighting its practical potential for high-energy Zn batteries.

Keywords

Localized high-concentration electrolytes Self-assembled Multifunctional additives Zwitterions Zn metals
Huang, Shengyang, Zuyang Hu, Xin Wang Mo, Yeonju Park, Jun Su Kim, Gun Jang, Dong Hyun Min, Hao Fu, Peixun Xiong, Zhipeng Wen, Young Mee Jung, Jaeyun Kim, Hyunjoo Lee, Chihyun Hwang, Youngkwon Kim, Cheng Chao Li, Qingyun Dou, and Ho Seok Park. 2026. “Self-Assembled Ordered Nanostructure of Zwitterionic Co-Solutes Induces Localized High-Concentration Electrolytes for Ultrastable and Efficient Zinc Metal Anodes”. Nano-Micro Letters 18 (January):194. https://doi.org/10.1007/s40820-025-02040-4.
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