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Aqueous zinc ion batteries (AZIBs) with high safety, low cost, and eco‐friendliness advantages show great potential in large‐scale energy storage systems. However, their practical application is hindered by low Columbic efficiency and unstable zinc anode resulting from the side reactions and deterioration of zinc dendrites. Herein, tripropylene glycol (TG) is chosen as a dual‐functional organic electrolyte additive to improve the reversibility of AZIBs significantly. Importantly, ab initio molecular dynamics theoretical simulations and experiments such as in situ electrochemical impedance spectroscopy, and synchrotron radiation‐based in situ Fourier transform infrared spectroscopy confirm that TG participates in the solvation sheath of Zn2+, regulating overpotential and inhibiting side reactions; meanwhile, TG inhibits the deterioration of dendrites and modifies the direction of zinc deposition by constructing an adsorbed layer on the zinc anode. Consequently, a Zn‐MnO2 full cell with TG electrolyte exhibited a specific capacity of 124.48 mAh g‐1 after 1000 cycles at a current density of 4 A g‐1. This quantitative regulation for suitable solvation sheath and adsorbed layer on zinc anode, and its easy scalability of the process can be of immediate benefit for the dendrite‐free, high‐performance, and low‐cost energy storage systems. [ABSTRACT FROM AUTHOR]

The practicality of aqueous zinc ion batteries (AZIBs) for large‐scale energy storage is hindered by challenges associated with zinc anodes. In this study, a low‐cost and multi‐function electrolyte additive, cetyltrimethyl ammonium bromide (CTAB), is presented to address these issues. CTAB adsorbs onto the zinc anode surface, regulating Zn2+ deposition orientation and inhibiting dendrite formation. It also modifies the solvation structure of Zn2+ to reduce water reactivity and minimize side reactions. Additionally, CTAB optimizes key physicochemical parameters of the electrolyte, enhancing the stability of the electrode/electrolyte interface and promoting reversibility in AZIBs. Theoretical simulations combined with operando synchrotron radiation‐based in situ Fourier transform infrared spectra and in situ electrochemical impedance spectra further confirm the modified Zn2+ coordination environment and the adsorption effect of CTAB cations at the anode/electrolyte interface. As a result, the assembled Zn‐MnO2 battery demonstrates a remarkable specific capacity of 126.56 mAh g−1 at a high current density of 4 A g−1 after 1000 cycles. This work highlights the potential of CTAB as a promising solution for improving the performance and practicality of AZIBs for large‐scale energy storage applications. [ABSTRACT FROM AUTHOR]

Rechargeable aqueous zinc‐ion batteries are considered as ideal candidates for large‐scale energy storage due to their high safety, eco‐friendliness, and low cost. However, Zn anode invites dendrite growth and parasitic reactions at anode‐electrolyte interface, impeding the practical realization of the battery. In this study, the electrochemical performance of the Zn‐metal anode is proposed to improve by using a 3D ZnTe semiconductor substrate. The substrate features high zincophilicity, high electronic conductivity and electron affinity, and a low Zn nucleation energy barrier to promote dendrite‐proof Zn deposition along the (002) crystal plane, while it also maintains high chemical stability against parasitic metal corrosion and hydrogen evolution reactions at surface, and a stable skeleton structure against the volume variation of anode. A Zn‐metal anode based on the telluride substrate shows a long cycle life of over 3300 h with a small voltage hysteresis of 48 and 320 mV at 1 and 30 mA cm−2, respectively. A zinc telluride@Zn//MnO2 full cell can operate for over 500 cycles under practical conditions in terms of lean electrolyte (18 µL mAh−1) and limited Zn metal (negative/positive capacity ratio of 3:1, and a high mass loading of the cathode. [ABSTRACT FROM AUTHOR]