Multifunctional Cellulose Nanocrystals Electrolyte Additive Enable Ultrahigh‐Rate and Dendrite‐Free Zn Anodes for Rechargeable Aqueous Zinc Batteries

Abstract

The design of aqueous zinc (Zn) chemistry energy storage with high rate‐capability and long serving life is a great challenge due to its inhospitable coordination environment and dismal interfacial chemistry. To bridge this big gap, herein, we build a highly reversible aqueous Zn battery by taking advantages of the biomass‐derived cellulose nanocrystals (CNCs) electrolyte additive with unique physical and chemical characteristics simultaneously. The CNCs additive not only serves as fast ion carriers for enhancing Zn2+ transport kinetics but regulates the coordination environment and interface chemistry to form dynamic and self‐repairing protective interphase, resulting in building ultra‐stable Zn anodes under extreme conditions. As a result, the engineered electrolyte system achieves a superior average coulombic efficiency of 97.27% under 140 mA cm‐2, and steady charge‐discharge for 982 h under 50 mA cm‐2, 50 mAh cm‐2, which proposes a universal pathway to challenge aqueous Zn chemistry in green, sustainable, and large‐scale applications.

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

“…Besides, nano-organic additives play a positive role in enhancing the performance of the ZMAs. As illustrated in Figure g, a green nanoscale electrolyte additive (approximately 400 nm in length) was prepared through a simple oxidation technique of cellulose nanocrystals (CNCs) . Ascribing to the nanosize effect of CNCs, they can provide a large number of reactive sites, which greatly facilitates ion migration and optimizes the coordination environment, enabling the uniform deposition of Zn 2+ and boosting the cyclability of the ZMAs (Figure h).…”

“…As illustrated in Figure 10g, a green nanoscale electrolyte additive (approximately 400 nm in length) was prepared through a simple oxidation technique of cellulose nanocrystals (CNCs). 188 Ascribing to the nanosize effect of CNCs, they can provide a large number of reactive sites, which greatly facilitates ion migration and optimizes the coordination environment, enabling the uniform deposition of Zn 2+ and boosting the cyclability of the ZMAs (Figure 10h). Surprisingly, Zn||Zn symmetric cells containing CNCs show reversible plating/stripping for 982 h at 50 mA cm −2 , demonstrating excellent transfer kinetics and high-rate stability.…”

“…(g) Schematic illustration of the fabrication of CNCs and (h) Zn plating/stripping process with CNCs electrolyte additive. Reprinted with permission from ref (). Copyright 2024, Wiley-VCH.…”

Bio-inspired hydroxyl-rich electrolyte additive for highly reversible aqueous Zn-ion batteries with strong coordination chemistry

“…17 To address the above issues, the central principle is to enhance the deposition kinetics and restrain H 2 O reactivity. Accordingly, different strategies, such as the structural design of Zn metal anodes, 18–20 interphase engineering, 21–24 water-in-salt electrolytes 25–27 and electrolyte additives, 28–30 have been reported with great achievements in improving the performance of ZIBs. Among these strategies, electrolyte additives feature low cost and high operability and have drawn much attention in recent years, 31–33 which have a crucial effect on regulating the zinc coordination chemistry and are deemed as an effective pathway to attain superior performance ZIBs.…”