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A self-assembly strategy uses ordered nanostructures from zwitterionic co-solutes to build highly efficient, ultrastable aqueous zinc (Zn) metal batteries. Screening six zwitterionic compounds identifies C10 (3-(decyldimethylammonio)propanesulfonate) as optimal, forming quasi-spherical aggregates (periodic length 3.77 nm) supported by SAXS analyses, spectroscopy, and molecular dynamics. The structure increases contact/aggregated ion pairs to generate LHCEs with selective Zn2+ channels, uniform solid electrolyte interfaces, and suppressed hydrogen evolution and corrosion via preferential adsorption on Zn(002), yielding >2800 h symmetric cycling and record areal capacity in Zn||VO2/CNT 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31-2103/TB  \nARTICLE [https://doi.org/10.1007/s40820-025-02040-4](https://doi.org/10.1007/s40820-025-02040-4)  \nCite as  \nNano-Micro Lett.(2026) 18:194  \nReceived: 23 October 2025  \nAccepted: 25 November 2025  \nPublished online: 4 January 2026 © The Author(s) 2026, modified publication 2026  \nSelf‑Assembled Ordered Nanostructure of Zwitterionic Co‑Solutes Induces Localized High‑Concentration Electrolytes for Ultrastable and Efficient Zinc Metal Anodes  \nShengyang Huang 1, Zuyang Hu 1,2, Xin Wang Mo 1, Yeonju Park3,4, Jun Su Kim 1, Gun Jang 1, Dong Hyun Min 1, Hao Fu 1, Peixun Xiong 1, Zhipeng Wen2,  \nYoung Mee Jung3,4, Jaeyun Kim 1, Hyunjoo Lee5, Chihyun Hwang6, Youngkwon Kim6 *  \n,  \nCheng Chao Li2 *, Qingyun Dou 1,7 *, Ho Seok Park1,8 *  \nHIGHLIGHTS  \n• Self-assembled zwitterion (C10) induces localized high-concentration electrolytes, regulating Zn2+ solvation, guiding selective ion transport, and enabling uniform solid electrolyte interface formation.  \n• A comprehensive set of advanced analyses (Guinier, PDDF, Porod) combined with spectroscopy and simulations reveals that C 10 self-assembles into ~3.8 nm quasi-spherical aggregates and bilayer-like interfacial structures.  \n• 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.  \nABSTRACT 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 selfassembled 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.  \nKEYWORDS Localized high-concentration electrolytes; Self-assembled; Multifunctional additives; Zwitterions; Zn metals  \n* Youngkwon Kim, [ykkim96@keti.re.kr](ykkim96@keti.re.kr); Cheng Chao Li, [licc@gdut.edu.cn](licc@gdut.edu.cn); Qingyun Dou, [douqy3@mail.sysu.edu.cn](douqy3@mail.sysu.edu.cn); Ho Seok Park, [phs0727@skku.edu](phs0727@skku.edu)  \n1 School of Chemical Engineering, Sungkyunkwan University (SKKU), 2066 Seobu-Ro, Jangan-Gu, Suwon 16419, Republic of Korea  \n1 Introduction  \nIn recent years, the ever-increasing demand for safe and cost-effective energy storage systems has motivated the development of advanced rechargeable batteries [1–3] . Among various battery technologies, aqueous zinc metal batteries","cbCaicHXrTE5oIY8","https://ap.wps.com/l/cbCaicHXrTE5oIY8","pdf",7564944,"English","# Introduction\n# Highlights\n# Abstract\n# Keywords","[{\"question\":\"What problem do localized high-concentration electrolytes (LHCEs) aim to solve for metal batteries?\",\"answer\":\"LHCEs target technical issues arising from unfavorable interfacial properties and solvation structures, improving interfacial behavior for metal batteries.\"},{\"question\":\"How does the zwitterionic co-solute C10 contribute to LHCE formation and Zn2+ transport?\",\"answer\":\"C10 self-assembles into quasi-spherical aggregates and bilayer-like interfacial structures that increase contact and aggregated ion pairs, providing fast and selective Zn2+ conducting channels and more uniform solid electrolyte interfaces.\"},{\"question\":\"What cycling and capacity performance are reported for zinc metal cells using Zn(OTf)2/C10 electrolytes?\",\"answer\":\"Zn||Zn symmetric cells show long-term plating/stripping over 2800 h at 1 mA cm−2 and 1 mAh cm−2, and Zn||VO2/CNT full cells deliver a record areal capacity of 8.10 mAh cm−2 at a cathode mass loading of 50 mg cm−2 after 150 cycles.\"}]","Self-Assembled Ordered Nanostructure of Zwitterionic Co-Solutes Induces Localized High-Concentration Electrolytes for Ultrastable and Efficient Zinc Metal Anodes | PDF",1790686251]