Tough MXene-Cellulose Nanofibril Ionotronic Dual-Network Hydrogel Films for Stable Zinc Anodes

Developing ionotronic interface layers for zinc anodes with superior mechanical integrity is one of the efficient strategies to suppress the growth of zinc dendrites in favor of the cycling stability of aqueous zinc-ion batteries (AZIBs). Herein, we assembled robust 2D MXene-based hydrogel films cross-linked by 1D cellulose nanofibril (CNF) dual networks, acting as interface layers to stabilize Zn anodes. The MXene-CNF hydrogel films integrated multifunctionalities, including a high in-plane toughness of 18.39 MJ m-3, high in-plane/out-of-plane elastic modulus of 0.85 and 3.65 GPa, mixed electronic/ionic (ionotronic) conductivity of 1.53 S cm-1 and 0.52 mS cm-1, and high zincophilicity with a high binding energy (1.33 eV) and low migration energy barrier (0.24 eV) for Zn2+. These integrated multifunctionalities, endowed with coupled multifield effects, including strong stress confinement and uniform ionic/electronic field distributions on Zn anodes, effectively suppressed dendrite growth, as proven by experiments and simulations. An example of the MXene-CNF|Zn showed a reduced nucleation overpotential of 19 mV, an extended cycling life of over 2700 h in Zn||Zn cells, and a high capacity of 323 mAh g-1 in Zn||MnO2 cells, compared with bare Zn. This work offers an approach for exploring mechanically robust 1D/2D ionotronic hydrogel interface layers to stabilize the Zn anodes of AZIBs.