Due to the excellent specific capacity and high working voltage, manganese oxide (MnO 2 ) has attracted considerable attention for aqueous zinc-ion batteries (AZIBs). However, the irreversible structural collapse and sluggish ionic diffusion lead to poor rate capability and inferior lifespan. Herein, we proposed a novel organic/inorganic hybrid cathode of carbon-based poly(4,4'-oxybisbenzenamine)/MnO 2 (denoted as C@PODA/MnO 2 ) for AZIBs. Various in/ex situ analyses and theoretical calculations prove that PODA chains with C=N groups can provide a more active surface/ interface for ion/electron mobility and zinc ion storage in the hybrid cathode. More importantly, newly formed MnÀ N interfacial bonds can effectively promote ion diffusion and prevent Mn atoms dissolution, enhancing redox kinetics and structural integrity of MnO 2 . Accordingly, C@PODA/MnO 2 cathode exhibits high capacity (321 mAh g À 1 or 1.7 mAh cm À 2 at 0.1 A g À 1 ), superior rate performance (88 mAh g À 1 at 10 A g À 1 ) and excellent cycling stability over 2000 cycles. Hence, rational interfacial designs shed light on the development of organic/ inorganic cathodes for advanced AZIBs.

Dendrite formation severely compromises further development of zinc ion batteries. Increasing the nucleation overpotential plays a crucial role in achieving uniform deposition of metal ions. However, this strategy has not yet attracted enough attention from researchers to our knowledge. Here, we propose that thermodynamic nucleation overpotential of Zn deposition can be boosted through complexing agent and select sodium L-tartrate (Na-L) as example. Theoretical and experimental characterization reveals L-tartrate anion can partially replace H2O in the solvation sheath of Zn2+, increasing de-solvation energy. Concurrently, the Na+ could absorb on the surface of Zn anode preferentially to inhibit the deposition of Zn2+ aggregation. In consequence, the overpotential of Zn deposition could increase from 32.2 to 45.1 mV with the help of Na-L. The Zn-Zn cell could achieve a Zn utilization rate of 80% at areal capacity of 20 mAh cm−2. Zn-LiMn2O4 full cell with Na-L additive delivers improved stability than that with blank electrolyte. This study also provides insight into the regulation of nucleation overpotential to achieve homogeneous Zn deposition.

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Dendrite growth and electrode/electrolyte interface side reactions in aqueous zinc-ion batteries (AZIBs) not only impair the battery lifetime but also pose serious safety concerns for the battery system, hindering its application in large-scale energy storage systems. Herein, by introducing positively charged chlorinated graphene quantum dot (Cl-GQD) additives into the electrolyte, a bifunctional dynamic adaptive interphase is proposed to achieve Zn deposition regulation and side reaction suppression in AZIBs. During the charging process, the positively charged Cl-GQDs are adsorbed onto the Zn surface, acting as an electrostatic shield layer that facilitates smooth Zn deposition. In addition, the relative hydrophobic properties of chlorinated groups also build a hydrophobic protective interface for the Zn anode, mitigating the corrosion of the Zn anode by water molecules. More importantly, the Cl-GQDs are not consumed throughout the cell operation and exhibit a dynamic reconfiguration behavior, which ensures the stability and sustainability of this dynamic adaptive interphase. Consequently, the cells mediated by the dynamic adaptive interphase enable dendrite-free Zn plating/stripping for more than 2000 h. Particularly, even at 45.5% depth of discharge, the modified Zn//LiMn 2 O 4 hybrid cells still retain 86% capacity retention after 100 cycles, confirming the feasibility of this simple approach for application with limited Zn sources.

Dual‐ion batteries (DIBs) is a promising technology for large‐scale energy storage. However, it is still questionable how material structures affect the anion storage behavior. In this paper, we synthesis graphite with an ultra‐large interlayer distance and heteroatomic doping to systematically investigate the combined effects on DIBs. The large interlayer distance of 0.51 nm provides more space for anion storage, while the doping of the heteroatoms reduces the energy barriers for anion intercalation and migration and enhances rapid ionic storage at interfaces simultaneously. Based on the synergistic effects, the DIBs composed of carbon cathode and lithium anode afford ultra‐high capacity of 240 mAh g−1 at current density of 100 mA g−1. Dual‐carbon batteries (DCBs) using the graphite as both of cathode and anode steadily cycle 2400 times at current density of 1 A g−1. Hence, this work provides a reference to the strategy of material designs of DIBs and DCBs.

Lithium-oxygen batteries (LOBs) are well known for their high energy density. However, their reversibility and rate performance are challenged due to the sluggish oxygen reduction/evolution reactions (ORR/OER) kinetics, serious side reactions and uncontrollable Li dendrite growth. The electrolyte plays a key role in transport of Li + and reactive oxygen species in LOBs. Here, we tailored a dilute electrolyte by screening suitable crown ether additives to promote lithium salt dissociation and Li + solvation through electrostatic interaction. The electrolyte containing 100 mM 18crown-6 ether (100-18C6) exhibits enhanced electrochemical stability and triggers a solution-mediated Li 2 O 2 growth pathway in LOBs, showing high discharge capacity of 10 828.8 mAh g carbon À 1 . Moreover, optimized electrode/electrolyte interfaces promote ORR/OER kinetics on cathode and achieve dendrite-free Li anode, which enhances the cycle life. This work casts new lights on the design of low-cost dilute electrolytes for high performance LOBs.

Heterostructures with interfacial effects have exhibited great potential for improving the electrochemical kinetics of electrode materials. However, the application of heterostructures is hampered by complicated synthesis parameters and numerous single components. Herein, a multiple‐templating synthesis strategy is proposed to improve the interfacial effect of heterojunction composites, mitigate volume variation upon lithiation/de‐lithiation, and increase interfacial compatibility with poly‐oxyethylene‐based (PEO‐based) electrolytes. Benefiting from the structural and compositional superiorities, the novel NiS/SnO2/MOF (NSM) electrode achieves superior electrochemical performance with exceptional specific capacity, outstanding rate capability and ultralong cyclability. As a result of the compatibility between organic components and the porous properties of metal organic frameworks (MOFs), the NSM electrode exhibits greater interfacial compatibility with PEO‐based solid‐state electrolytes. This work not only describes a meticulous protocol for heterostructured high‐performance electrode materials, but also provides a new insight to enhance the connectivity between the interfaces of solid‐state batteries.