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However, the inferior cycling life due to water\u2010induced parasitic reactions and uncontrollable dendrites growth impede their application. Electrolyte optimization via the use of additives is a promising strategy to enhance the stability of AZIBs. Nevertheless, the mechanism of optimal multifunctional additive strategy requires further exploration. Herein, sodium dodecyl benzene sulfonate (SDBS) is proposed as a dual\u2010functional additive in ZnSO<jats:sub>4<\/jats:sub> electrolyte. Benefiting from the additive, both side reactions and zinc dendrites growth are significantly inhibited. Further, a synchrotron radiational spectroscopic study is employed to investigate SDB<jats:sup>\u2212<\/jats:sup> adjusted electric double layer (EDL) near the Zn surface and the optimized solvation sheath of Zn<jats:sup>2+<\/jats:sup>. First\u2010principles calculations verify the firm adsorption of SDB<jats:sup>\u2212<\/jats:sup>, and restriction of random diffusion of Zn<jats:sup>2+<\/jats:sup> on the Zn surface. In particular, the SDBS additive endows Zn||Zn symmetric cells with a 1035\u00a0h ultra\u2010stable plating\/stripping at 0.2\u00a0mA\u00a0cm<jats:sup>\u22122<\/jats:sup>. This work not only provides a promising design strategy by dual\u2010functional electrolyte additives for high stable AZIBs, but also exhibits the prospect of synchrotron radiation spectroscopy analysis on surface EDL and Zn<jats:sup>2+<\/jats:sup> solvation shell optimization.<\/jats:p>","DOI":"10.1002\/smtd.202301115","type":"journal-article","created":{"date-parts":[[2023,12,25]],"date-time":"2023-12-25T11:39:55Z","timestamp":1703504395000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":74,"title":["Anion Additive Integrated Electric Double Layer and Solvation Shell for Aqueous Zinc Ion Battery"],"prefix":"10.1002","volume":"8","author":[{"given":"Xiya","family":"Yang","sequence":"first","affiliation":[{"name":"National Synchrotron Radiation Laboratory CAS Center for Excellence in Nanoscience University of Science and Technology of China  Hefei Anhui 230029 P. R. 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