The booming of aqueous zinc-ion batteries (AZIBs) draws the researchers' attention to issues of zinc metal anodes, such as uncontrollable dendrite growth, corrosion, and volume effects. Zinc powder anode is more suitable for the industrial application of AZIBs than the widely used zinc foil anode due to its low cost, tunability and processability. However, the related solutions are rarely studied because the above issues of zinc metal anode are more serious in zinc powder anode. Herein, for the first time, we design a semi-solid zinc slurry anode consisting of zinc powder and zincophilic tin additive dispersed in a conductive elastic rheological network. Zinc can be deposited homogeneously on the dispersed tin particles, which avoids agglomerative zinc deposition and alleviates volume change during repeated zinc stripping/plating. Moreover, the practical application of the full cell with slurry is very promising since its operating life can be easily extended by facile slurry renewal.

Aqueous zinc‐ion battery is regarded as one of the promising devices for large‐scale energy storage systems owing to its high safety, cost‐effectiveness, and competitive electrochemical properties. However, the dendrite growth on zinc metal anodes dramatically hinders its further practical applications, and the internal mechanism of dendrite evolution is still unclear. The introduction of a protective layer on the anode interface is an effective method to avoid zinc dendrite growth. Herein, a two‐dimensional (2D) atomic surface diffusion mechanism is proposed to reveal the evolution of zinc deposition from tiny protrusion to dendrite under uneven electric and ionic fields. Further, the conductive copper nitride (CN) protective layer is constructed on the zinc metal anode by a facile and scalable magnetron sputtering approach. Their protective layer possesses a high zinc affinity and high diffusion barrier for zinc atom migration, leading to spacious nucleation, and uniform zinc deposition, thus significantly boosting the electrochemical stability. For the first time, the role of the restricted 2D atomic surface diffusion mechanism in inhibiting the formation of zinc tiny protrusion that induces uneven electric and ionic fields is revealed. This work can provide a novel insight for future research on dendrite‐free zinc metal anodes by interfacial modification.

Aqueous Zn‐ion batteries (AZIBs) are regarded as a promising alternative to the widely used lithium‐ion batteries in large‐scale energy storage systems. The researches on the development of novel aqueous electrolyte to improve battery performance have also attracted great interest since the electrolyte is a key component for Zn2+ migration between cathode and anode. Herein, we briefly summarized and illuminated the recent development tendency of aqueous electrolyte for AZIBs, then deeply analyzed its existing issues (water decomposition, cathode dissolution, corrosion and passivation, and dendrite growth) and discussed the corresponding optimization strategies (pH regulation, concentrated salt solution, electrolyte composition design, and functional additives). The internal mechanisms of these strategies were further revealed and the relationships between issues and solutions were clarified, which could guide the future development of aqueous electrolytes for AZIBs.

Developing a highly stable and dendrite-free zinc anode is essential to the commercial application of zinc metal batteries. However, the understanding of zinc dendrites formation mechanism is still insufficient. Herein, for the first time, we discover that the interfacial heterogeneous deposition induced by lattice defects and epitaxial growth limited by residual stress are intrinsic and critical causes for zinc dendrite formation. Therefore, an annealing reconstruction strategy was proposed to eliminate lattice defects and stresses in zinc crystals, which achieve dense epitaxial electrodeposition of zinc anode. The as-prepared annealed zinc anodes exhibit dendrite-free morphology and enhanced electrochemical cycling stability. This work first proves that lattice defects and residual stresses are also very important factors for epitaxial electrodeposition of zinc in addition to crystal orientation, which can provide a new mechanism for future researches on zinc anode modification.

No abstract