Jun Huang

Aqueous batteries feature intrinsic safety, but how to achieve regular and planar electrodeposits at liquid‐solid interfaces has emerged as a fundamental barrier to energy‐dense aqueous batteries that use metal anodes. Based on classical crystal growth theory, sluggish metal ion transport during the deposition process will lead to rapid interfacial metal ion depletion, resulting in a sharp increase in interfacial supersaturation and subsequently inducing dendrite growth. Herein, micropore high‐entropy single‐atoms carbon nanoparticles (CuNiMnCoIr/CNs) were synthesized as a unique electrolyte additive to suppress interfacial Zn ²⁺ concentration polarization and strengthen Zn chemistry at the atomic level. The micropore CuNiMnCoIr/CNs not only provide abundant Zn ²⁺ transport channels but significantly reduce the migration energy barrier of Zn ²⁺ from the bulk electrolyte to electrode interface to promote rapid desolvation kinetics and homogenize Zn ²⁺ flux, thereby effectively alleviating interfacial Zn ²⁺ supersaturation and guiding layer‐by‐layer Zn deposition. Consequently, trace CuNiMnCoIr/CNs additive delivers a high Zn ²⁺ transference number of 0.89 and enables Zn//Zn cells to cycle stably for over 4000 h at 5 mA cm ⁻² , and 800 h even at 50 mA cm ⁻² , with an outstanding cumulative deposition capacity up to 20 Ah cm ⁻² . Such knowledge may provide new insights to challenge interface chemistry for advanced aqueous metal‐ion batteries.

Gel electrolyte has emerged as a desirable candidate for high‐safety Zn ion batteries (ZIBs), but it is enormously restricted by the sluggish Zn ²⁺ ion transport and severe electric field distortion at the electrode/electrolyte interface, leading to Zn anode failure. Herein, a unique gel electrolyte with precise atomic‐level regulation of Zn ²⁺ migration is developed through incorporating Sn single‐atoms (SAs)‐loaded carbon fibers (CFs) into the polyacrylamide (PAM) matrix (PAM/CFs@Sn) for building stable Zn anodes. The CFs fillers are introduced into the PAM gel electrolyte, which can promote more uniform Zn ²⁺ flux and charge distribution, thereby alleviating electric‐field heterogeneity. Meanwhile, the atomic‐level zincophilic Sn SAs sites offer abundant and uniform active centers to lower the Zn ²⁺ migration energy barrier, thereby promoting regular and planar Zn deposition. These combined advantages of the PAM/CFs@Sn gel electrolyte enable Zn anodes to achieve stable cycling up to 3740 h at 0.5 mA cm ⁻² , a high Zn ²⁺ transference number of 0.89 and an average coulombic efficiency of 99.5% over 1480 h, etc. Overall, this work provides a reliable atomic‐level zinc chemistry regulating strategy of gel electrolytes toward durable Zn anodes and beyond.

Zinc‐ion batteries (ZIBs) are promising for large‐scale energy storage, but their practical applications are still greatly limited by the thermodynamic and kinetic mismatch resulting from uneven interfacial electric fields and sluggish Zn ²⁺ transport kinetics. Herein, electron‐delocalized Co‐doped ZnO nanocrystals were synthesized as an electrolyte additive to synergistically regulate the local electric field and Zn ²⁺ transport kinetics of the electrode–electrolyte interface for building efficient ZIBs. Specifically, Co doping induces lattice distortion and facilitates the formation of oxygen vacancies, thereby promoting electron delocalization and redistributing the interface electric field. Meanwhile, combining the electron delocalization strategy with nanocrystals helps to achieve numerous zincophilic sites, thereby accelerating the Zn ²⁺ transport, resulting in regular and planar Zn deposition. Encouragingly, the Zn//Zn symmetric cell achieves exceptional cycling stability of 2700 h at 10 mA cm ⁻² and 1 mAh cm ⁻² with a high cumulative plated capacity of 13 700 mAh cm ⁻² ; the Zn//Cu asymmetric cell exhibits high reversibility with an average coulombic efficiency of 99.73% for over 3300 h. The strategy of synergistically regulating the interfacial electric field and the Zn ²⁺ transport kinetics provides a universal route to challenge Zn interface chemistry for advanced ZIBs and could be extended to other aqueous metal‐ion batteries.

A conventional single-phase solid electrolyte interphase (SEI) lacks the multifunctionality to endure repeated Zn plating/stripping, making it difficult to achieve high-performance zinc-ion batteries (ZIBs). Herein, a synergistic ion-solvent modulation using 1-vinyl-3-ethylimidazolium tetrafluoroborate (VElmBF₄) constructs a multiphase SEI with enhanced mechanical and electrochemical stability, enabling reversible Zn²⁺ plating/stripping for a high Zn utilization rate (ZUR). Consequently, the multiphase SEI enables a Zn||Zn cell to have an ultralong rate capability at periodically changing current densities from 1 to 20 mA cm^-2 for over 2500 h, an ultralong plating/stripping lifespan exceeding 4000 h at 1 mA cm^-2, and superior stability for over 2000 h even under a high ZUR of 28.5%. Moreover, the Zn||Cu asymmetric cell demonstrates a high average Coulombic efficiency of 99.86% in over 900 cycles at 5 mA cm^-2, 2.5 mAh cm^-2, which offers a promising avenue for high-performance ZIBs.

A unique face-to-face electronic channel regulation strategy was proposed for building highly reversible Zn anodes through integrating polyacrylamide gel electrolytes with commercial carbon cloth by a simple and mass-producible hot-pressing process.

Zinc (Zn) metal anodes have garnered significant attentions for their applications in aqueous Zn‐ions batteries (AZIBs), but the electrochemical plating/stripping chemistry and failure mechanism under multifactorial conditions remain ambiguous, and the reversibility is overestimated under the single condition. Herein, a reversibility indicator ( R _i ) based on the characteristic crystallization peaks is proposed to evaluate the plating/stripping chemistry and understand the reversibility, particularly in Zn//Cu asymmetric cells. Moreover, a nanomicellar electrolyte composing sodium dodecyl sulfate and curcumin has been designed, which encapsulates Zn ²⁺ within the nanodomain structure via the strong coordination interaction between β ‐diketone moiety of curcumin molecules and Zn ²⁺ , leading to the controlled Zn ²⁺ release and enhancing Zn ²⁺ transfer kinetics for the dense Zn deposition. Additionally, the initial consecutive hydrogen bonding network is disrupted, thereby suppressing the hopping transport of protons for interfacial side reactions. As a result, the Zn//Zn cell delivers a stable cycling up to 3800 h, a high discharge of depth with 28.5% for over 1200 h, and the Zn//Cu cell with low R _i value (0.87) exhibits highly reversible cycling for 1418 h at 5 mA cm ⁻² . This study provides an innovative insight into promoting the symmetric Zn plating/stripping chemistry for highly reversible AZIBs.

RNA and DNA as eco-friendly electrolyte additives form stable nucleic acid recognition interfaces, protecting Zn anodes and promoting uniform interfacial reactions for high-performance ZIBs.

Dendrite growth and irreversible side reactions caused by inhomogeneous ionic/electric field distributions at Zn anodes in conventional gel electrolytes, combined with their inherent ion transport constraints, seriously limit the electrochemical performance and cycling stability of aqueous Zn ion batteries (ZIBs). Herein, a synergistic ion rectification/charge redistribution strategy is established by incorporating phytic acid (PA)‐phosphorylated MIL‐88A metal–organic frameworks into the polyacrylamide (PAM) gel electrolyte for building highly reversible Zn anodes. This unique strategy leverages the phosphate groups on PA as zincophilic sites within the gel electrolyte for promoting rapid ion migration, while the porous MIL‐88A dissipates charge accumulation caused by ion concentration differences and adjust the micro‐space charge distribution for ensuring uniform electric field distribution and effectively suppressing Zn dendrite formation, thereby enabling highly reversible ZIBs. As a result, this synergistic ion rectification/charge redistribution strategy achieves the high Zn ²⁺ ions transference number of 0.66, the excellent coulombic efficiency of Zn//Cu cell of 99.7%, the outstanding cycle life of Zn//Zn cell exceeding 3600 h and a high cumulative capacity of 2200 mAh cm ⁻² , providing a promising solution for the design of highly reversible Zn‐based energy storage devices.

Chlorogenic acid (CGA) is investigated as an electrolyte additive to achieve superior stability for zinc anodes.