Aqueous zinc ion batteries (AZIBs) are receiving increasing attention for large-scale energy storage systems owing to their appealing features with intrinsic safety, low cost, and scalability. Unfortunately, the water-induced parasitic reactions and dendrite growth on the Zn anode severely impede the further development of AZIBs. Herein, a thiourea additive is introduced into ZnSO 4 electrolyte to construct unique metal-molecule interface for simultaneously regulating the Zn anode interface chemistry and the bulk electrolyte environment. Experimental results and theoretical calculations reveal that the formed metal-molecule interface can not only serve as a corrosion inhibitor for alleviating the water-induced side reactions, but also act as a Zn 2+ ion regulator for promoting the homogenous Zn deposition, thus achieving a corrosion-free and dendrite-free Zn anode. Consequently, the Zn|Zn symmetric cell exhibits an extended lifespan of 1200 h at 1 mA cm -2 , 1mAh cm -2 , and a high cumulative capacity of 3000 mAh cm -2 at 10 mA cm -2 . When paired with V 2 O 5 cathode, the Zn|V 2 O 5 full cell delivers a high capacity retention of 76.0% after 1000 cycles at 1 A g -1 . This study paves a new way to modulate Zn electrode interface chemistry by the novel design of metal-molecule interface for advanced rechargeable Zn metal batteries and beyond.

Metallic‐phase selenide molybdenum (1T‐MoSe2) has become a rising star for sodium storage in comparison with its semiconductor phase (2H‐MoSe2) owing to the intrinsic metallic electronic conductivity and unimpeded Na+ diffusion structure. However, the thermodynamically unstable nature of 1T phase renders it an unprecedented challenge to realize its phase control and stabilization. Herein, a plasma‐assisted P‐doping‐triggered phase‐transition engineering is proposed to synthesize stabilized P‐doped 1T phase MoSe2 nanoflower composites (P‐1T‐MoSe2 NFs). Mechanism analysis reveals significantly decreased phase‐transition energy barriers of the plasma‐induced Se‐vacancy‐rich MoSe2 from 2H to 1T owing to its low crystallinity and reduced structure stability. The vacancy‐rich structure promotes highly concentrated P doping, which manipulates the electronic structure of the MoSe2 and urges its phase transition, acquiring a high transition efficiency of 91% accompanied with ultrahigh phase stability. As a result, the P‐1T‐MoSe2 NFs deliver an exceptional high reversible capacity of 510.8 mAh g−1 at 50 mA g−1 with no capacity fading over 1000 cycles at 5000 mA g−1 for sodium storage. The underlying mechanism of this phase‐transition engineering verified by profound analysis provides informative guide for designing advanced materials for next‐generation energy‐storage systems.

Uncontrollable dendrite growth and sluggish ion‐transport kinetics are considered as the main obstacles for the further development of high‐performance aqueous zinc ion batteries (AZIBs). Here, a nature‐inspired separator (ZnHAP/BC) is developed to tackle these issues via the hybridization of the biomass‐derived bacterial cellulose (BC) network and nano‐hydroxyapatite particles (HAP). The as‐prepared ZnHAP/BC separator not only regulates the desolvation process of the hydrated Zn2+ ions (Zn(H2O)62+) by suppressing the water reactivity through the surface functional groups, alleviating the water‐induced side‐reactions, but also boosts the ion‐transport kinetics and homogenize the Zn2+ flux, resulting in a fast and uniform Zn deposition. Remarkably, the Zn|Zn symmetric cell with ZnHAP/BC separator harvests a long‐term stability over 1600 h at 1 mA cm−2, 1 mAh cm−2 and endures stable cycling over 1025 and 611 h even at a high depth of discharge (DOD) of 50% and 80%, respectively. The Zn|V2O5 full cell with a low negative/positive (N/P) capacity ratio of 2.7 achieves a superior capacity retention of 82% after 2500 cycles at 10 A g−1. Furthermore, the Zn/HAP separator can be totally degraded within 2 weeks. This work develops a novel nature‐derived separator and provides insights in constructing functional separators toward sustainable and advanced AZIBs.

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Melamine-based porous organic polymers (POPs) are promising for gas uptake and water treatment because of their unique and tunable porosity, high nitrogen (N) content, and high Brunauer−Emmett−Teller (BET) surface area (S BET ). However, it is difficult to construct ketone-based POPs by the Friedel−Crafts acylation reaction. Herein, the ketone-based POPs were postfunctionalized with melamine (MA) by the Schiff-based reaction and the rigid triazine rings of MA were embedded in the polymer chains as rigid cross-linkers, resulting in the polymers with high S BET (555 m 2 •g −1 ) and total pore volume (0.72 cm 3 •g −1 ). Moreover, plentiful imine, amino, and triazine functionalities were inserted in the polymers, providing the polymers with high N content of 41.83 wt %. The resulting polymers were promising for CO 2 capture (145 mg• g −1 ; 273 K, 1.0 bar) and Hg 2+ removal (372 mg•g −1 ). This study offers a universal strategy to construct melamine-based POPs from various ketone-functionalized HCPs via a simple postfunctionalization.