Nanoengineered Functional Cellulose Ionic Conductor Toward High‐ Performance All‐Solid‐State Zinc‐Ion Battery

Abstract

The rechargeable zinc‐ion battery is regarded as a promising candidate for the next‐generation energy storage system, however, zinc dendrite growth and hydrogen evolution reaction (HER) have greatly hindered the practical application of the battery. Herein, a functionalized, nano‐engineering Zn2+ coordinated carboxylate cellulose solid‐state electrolyte (denoted as Zn‐CCNF@XG) for zinc‐ion battery is constructed through a straightforward approach. According to the experimental and density functional theory (DFT) results of dissociation energy, the notably decreased dissociation energy by −COOH is favorable to Zn2+ de‐coordinating and rapid ion‐hopping in Zn‐CCNF@XG to achieve high ionic conductivity and transference number. More importantly, the engineered molecular channels are beneficial to enlarging the distance between the nanofibril chains, providing a larger space for the movement of Zn2+. Benefiting from the coordination of Zn2+ with −OH in carboxylate cellulose nanofibrils, Zn‐CCNF@XG as a good ionic conductor displays a high ionic conductivity of 1.17 × 10−4 S cm−1 and transference number of 0.78. The Zn||NaV3O8·1.5H2O full cell with Zn‐CCNF@XG maintains a capacity retention of 83.46% with a coulombic efficiency of 99.99% after 3000 cycles (1 A g−1). The proposed strategy by introducing a functional group to cellulose nanofibrils effectively avoids the dendrite and HER, providing valuable guidelines for the practical application of zinc‐ion batteries.

Advances of Nanomaterials for High-Efficiency Zn Metal Anodes in Aqueous Zinc-Ion Batteries

“…Additionally, the unstable electrode/electrolyte interface remains a major obstacle affecting the electrochemical performance of SPEs. It is worth noting that the rapid development of nanomaterials provides effective pathways for solving the interfacial compatibility problems between SPEs and ZMAs. , Among them, 2D MXene materials benefit from their high conductivity and plentiful active groups, which can be well combined with the polymer matrices to expedite ion migration and improve the anode/electrolyte interface. Feng et al employed hydrogen interaction to bond MXene nanosheets onto the PVDF-HFP (PH) substrate .…”