- Research Article
- 10.1002/adfm.75778
Desolvation and Self‐Assembled Molecular Engineering Synergistically Reshape the Electric Double Layer toward Highly Stable Zinc Metal Anodes
- May 11, 2026
- Advanced Functional Materials
- Qiyu Fan + 10 more +10
ABSTRACT Aqueous zinc‐ion batteries (AZIBs) offer significant advantages and wide applications. However, Zn dendrite growth and water‐induced side reactions still hinder their commercialization. Here, bis ( 2 ‐carboxyethyl) disulfide (BD), a centrosymmetric molecule featuring a dynamic covalent disulfide bond and highly electronegative carboxyl groups, serves as a multifunctional electrolyte additive. It is discovered that BD optimizes the Zn 2+ solvation structure and restructures the hydrogen‐bond network. In particular, the adsorbed layer of BD molecules at the electrode/electrolyte interface undergoes S─S bond cleavage, forming a self‐assembled molecular layer of β ‐mercaptopropionic acid. This unique self‐assembled molecular layer not only provides numerous uniform and stable deposition sites for Zn 2+ , but also constructs an H 2 O‐poor and SO 4 2− ‐repellent electric double layer (EDL), effectively suppressing H 2 O‐induced side reactions and corrosion while guiding uniform and orderly Zn 2+ deposition on the (002) plane. Consequently, Zn||Zn symmetric cells based on BD‐containing electrolyte exhibit stable stripping/plating behavior for over 4700 h at 1 mA cm −2 and 3000 h at 5 mA cm −2 . Furthermore, Zn||VO 2 full cells maintain a capacity retention of 79.5% after 5000 cycles at 5 A g −1 . This self‐assembled molecular engineering of reshaping the EDL offers a novel strategy for constructing stable and reversible Zn anodes in AZIBs.
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