Freestanding and Flexible Interfacial Layer Enables Bottom-Up Zn Deposition Toward Dendrite-Free Aqueous Zn-Ion Batteries

Aqueous rechargeable zinc ion batteries are regarded as a competitive alternative to lithium-ion batteries because of their distinct advantages of high security, high energy density, low cost, and environmental friendliness. However, deep-seated problems including Zn dendrite and adverse side reactions severely impede the practical application. In this work, we proposed a freestanding Zn-electrolyte interfacial layer composed of multicapsular carbon fibers (MCFs) to regulate the plating/stripping behavior of Zn anodes. The versatile MCFs protective layer can uniformize the electric field and Zn(2+) flux, meanwhile, reduce the deposition overpotentials, leading to high-quality and rapid Zn deposition kinetics. Furthermore, the bottom-up and uniform deposition of Zn on the Zn-MCFs interface endows long-term and high-capacity plating. Accordingly, the Zn@MCFs symmetric batteries can keep working up to 1500 h with 5 mAh cm(−2). The feasibility of the MCFs interfacial layer is also convinced in Zn@MCFs||MnO(2) batteries. Remarkably, the Zn@MCFs||α-MnO(2) batteries deliver a high specific capacity of 236.1 mAh g(−1) at 1 A g(−1) with excellent stability, and maintain an exhilarating energy density of 154.3 Wh kg(−1) at 33% depth of discharge in pouch batteries. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-022-00921-6.