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Construction of polymer‐based artificial solid‐electrolyte interphase films on Zn metal anode holds great potential in the suppression of both dendrite growth and side reaction in rechargeable aqueous Zn‐ion batteries. However, the traditional polymer films suffer from the critical issues of sluggish Zn2+ transport kinetics and rigid interface. Herein, zinc alginate (ZA) hydrogel is designed and prepared as a dynamic interface and Zn2+ redistributor on Zn anode via in situ cross‐linking reaction. The zincophilic and negatively charged carboxyl groups of ZA promote the transport of Zn2+ ions along a "Z‐type" pathway, the repulsion of free SO42‐ anions, and the desolvation of Zn2+ ions, consequently leading to the homogeneous deposition of Zn and the effective suppression of side reaction. Additionally, the dynamic flexibility of ZA hydrogel endows the Zn anode with self‐adapting interface to accommodate the volume variation and repair the possible ruptures, thereby guaranteeing the long‐term cycling stability. Assisted by the ZA layer, the Zn anode achieves a prolonged lifespan over 2200 h without the formation of Zn dendrites and by‐products. Outstanding cycling stability is also demonstrated for the Zn anode when coupled with MnO2 cathode, further demonstrating its prospects for practical application. [ABSTRACT FROM AUTHOR]

Lithium/thionyl chloride (Li/SOCl2) primary batteries are appealing power solutions because of their remarkable electrochemical performances. However, their mass applications are hindered by the challenges in sustainability, cost and safety concerns owing to the employed Li chemistry. Here, magnesium (Mg) chemistry is shown as a promising alternative through synergistic optimization of electrolyte solvation and electrode reaction kinetics. The first Mg/SOCl2 primary battery yields surprisingly high specific capacities up to ≈14 000 mAh g−1 at a decent discharge voltage of ≈1.67 V, which outperforms the state‐of‐the‐art Mg‐based primary batteries. In addition, it retains almost 100% of the original capacity after 20‐day reservation. The impressive battery performances are originated from the stabilized MgCl2 formation on high‐surface‐area carbon cathode and suppressed Mg anode corrosion via the Mg‐induced solvation effect. Mg/SOCl2 primary batteries are promising candidates for low‐cost and recyclable power supplies, and they thus open new avenues for the development of sustainable battery chemistries. [ABSTRACT FROM AUTHOR]