Plasma-assisted aerogel interface engineering enables uniform Zn2+ flux and fast desolvation kinetics toward zinc metal batteries

Abstract

The poor reversibility of Zn anodes induced by dendrite growth, surface passivation, and corrosion, severely hinders the practical applicability of Zn metal batteries. To address these issues, a plasma-assisted aerogel (PAG) interface engineering was proposed as efficient ion transport modulator that can simultaneously regulate uniform Zn2+ flux and desolvation behavior during battery operation. The PAG with ordered mesopores acted as an ion sieve to homogenize Zn deposition and accelerate Zn2+ flux, which is favorable for corrosion resistance and dendrite suppression. Importantly, the plasma-assisted aerogel with abundant hydrophilic groups can facilitate the desolvation kinetics of Zn2+ due to the multiple hydrogen-bonding interaction with the activated water molecules, thus accelerating the Zn2+ migration kinetics. Consequently, the Zn/Zn cell assembled with PAG-modified separator demonstrates stable plating and stripping behavior (over 1400 h at 1 mA cm−2) and high Coulombic efficiency (99.8% at 1 mA cm−2 after 1100 cycles), and the Zn||MnO2 full cell shows excellent long-term cycling stability and maintains a high capacity of 154.9 mA h g−1 after 1000 cycles at 1 A g−1. This study provides a feasible approach for the large-scale fabrication of aerogel functionalized separators to realize ultra-stable Zn metal batteries.