Shahadat Ali, Mujahid Hussain, Muhammad Faizan, Chia-Chin Chang, Syed Irfan
Developed a coordination-centered, failure-aware framework connecting ligand exchange, ion pairing, and coordination-derived interphases to Zn inventory loss and full-cell failure. Reconciled conflicting reports on Zn(002), Zn(100), and Zn(101) textures as interface- and flux-dependent stability-kinetics trade-offs. Emphasized the importance of limited-Zn and anode-free configurations, cathode-derived cross-talk, proton activity, and the mismatch between symmetric and practical full cells.
Aqueous zinc batteries combine nonflammable electrolytes and abundant Zn with attractive cost and safety, yet practical cells remain limited by chemistry that spans the Zn 2+ solvation shell, the electric double layer, and both electrode interfaces. This review develops a coordination-centered, failure-aware framework that connects ligand exchange, ion pairing, hydrogen-bond organization, adsorption, desolvation, nucleation, crystallographic growth, and coordination-derived interphases to Zn inventory loss and full-cell failure. We distinguish true coordination effects from correlated physical phenomena such as wetting, electrostatic screening, and surface-tension changes, and evaluate mechanistic claims using spectroscopy, operando imaging, gas analysis, electrochemical mass balance, molecular simulation, and data-driven models. Conflicting reports on Zn(002), Zn(100), and Zn(101) textures are reconciled as interface- and flux-dependent stability–kinetics trade-offs rather than a universal facet ranking. Particular emphasis is placed on limited-Zn and anode-free configurations, cathode-derived cross-talk, proton activity and local pH, and the mismatch between long-lived symmetric cells and practical full cells. Quantitative descriptors are compared against current/areal-capacity pairs, cumulative plated capacity, Zn depth of discharge, cathode loading, N/P and E/C ratios, calendar stability, pouch-cell scale, cost, and sustainability. The resulting coordination-to-device map defines the evidence needed to translate molecular regulation into durable, inventory-efficient aqueous Zn batteries.