Chaotropic Anion‐Regulated Interfacial Desolvation Enables Ultrafast Aqueous Zn‐Ion Storage in TiN‐Integrated δ‐MnO 2 /MXene Heterostructure Anodes

ABSTRACT Aqueous zinc‐ion hybrid supercapacitors (AZI‐HSCs) offer a compelling sustainable energy storage platform, yet their development is constrained by incompatible electrode‐electrolyte dynamics. Sluggish anode kinetics and narrow electrolyte voltage windows fundamentally limit their performance. While δ‐MnO 2 offers high theoretical capacity as an anode, its practical deployment is hindered by poor conductivity, slow ion diffusion, and structural instability. Herein, an atomic‐scale charge‐modulated δ‐MnO 2 /MXene–TiN heterostructure anode synergized with a chaotropic ClO 4 − ‐modified electrolyte holistically overcomes these limitations. Nitrogen functionalization engineers conductive Ti–N scaffolds…

• NN
  National Natural Science Foundation of China

  Awards: 12327804, 52231007, 22405050, T2321003, 22088101, 22005046
• SA
  Science and Technology Commission of Shanghai Municipality

  Award: 24ZR1406400
• AS
  Aeronautical Science Foundation of China

  Awards: 2024M0730P9001, 202400180P9001
• FR
  Fundamental Research Funds for the Central Universities

  Awards: 2232024D‐31, 2232024A‐01
• SA
  Science and Technology on Surface Physics and Chemistry Laboratory

  Award: JCKYS2023120201