Regulating the Inner Helmholtz Plane with a High Donor Additive for Efficient Anode Reversibility in Aqueous Zn‐Ion Batteries

Abstract The performance of aqueous Zn ion batteries (AZIBs) is highly dependent on inner Helmholtz plane (IHP) chemistry. Notorious parasitic reactions containing hydrogen evolution reactions (HER) and Zn dendrites both originate from abundant free H 2 O and random Zn deposition inside active IHP. Here, we report a universal high donor number (DN) additive pyridine (Py) with only 1 vol. % addition (Py‐to‐H 2 O volume ratio), for regulating molecule distribution inside IHP. Density functional theory (DFT) calculations and molecular dynamics (MD) simulation verify that incorporated Py additive could tailor Zn 2+ solvation sheath and exclude H 2 O molecules from IHP effectively, which is in favor of preventing H…

• NN
  National Natural Science Foundation of China

  Award: No. 52003188, T2188101, 22173066
• NS
  Natural Science Foundation of Jiangsu Province

  Award: No. BK20200871
• SK
  State Key Laboratory for Modification of Chemical Fibers and Polymer Materials

  Award: No. KF2104
• NK
  National Key Research and Development Program of China

  Award: No. 2022YFB2502200