The notorious dendrites and corrosion reactions mainly derive from the instability of interface kinetics in aqueous environments, prominently impeding the Zn anode in commercial applications. To circumvent this issue, we employed sodium methylenedinaphthalene disulphonate (SMD) to modulate interfacial deposition kinetics by forming heterogeneous interfaces containing the electrical double layer (EDL) and solid electrolyte interface (SEI) in different stages for achieving crystallographic optimization of Zn deposition and inhibiting parasitic reactions. Benefitting from the vital interplay between -S = O of SMD and Zn2+, as well as the adsorption privilege of SMD to water on the Zn anode, the EDL can assume functions of promoting the initial desolvation of Zn(H2O)62+ and uniformizing nucleation sites of Zn electroplating at the early stage, dedicated to the subsequent formation of compact SEI and Zn (002) preferential nucleation. Subsequently, the SMD-induced SEI interphase further steers the stratiform growth of the Zn (002) plane following the as-formed zinc seed nucleation template, realizing late-stage regulation of interfaces to deposition dynamics. As anticipated, utilizing SMD-contained electrolyte results in the Zn anode exhibiting remarkable stability for 1400 h under harsh conditions of 5 mA cm−2 and 3 mA h cm−2, facilitating the improvement of lifespan in Zn-MnO2 full cells during 1400 cycles. This work highlights the significance of interface regulation in reversible deposition dynamics and provides promising insights into stabilizing Zn anodes.
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