Maximizing Electrostatic Polarity of Non‐Sacrificial Electrolyte Additives Enables Stable Zinc‐Metal Anodes for Aqueous Batteries

Abstract

Although additives are widely used in aqueous electrolytes to inhibit the formation of dendrites and hydrogen evolution reactions on Zn anodes, there is a lack of rational design principles and systematic mechanistic studies on how to select a suitable additive to regulate reversible Zn plating/stripping chemistry. Here, using saccharides as the representatives, we reveal that the electrostatic polarity of non‐sacrificial additives is a critical descriptor for their ability to stabilize Zn anodes. Non‐sacrificial additives are found to continuously modulate the solvation structure of Zn ions and form a molecular adsorption layer (MAL) for uniform Zn deposition, avoiding the thick solid electrolyte interphase layer due to the decomposition of sacrificial additives. A high electrostatic polarity renders sucrose the best hydrated Zn2+ desolvation ability and facilitates the MAL formation, resulting in the best cycling stability with a long‐term reversible plating/stripping cycle life of thousands of hours. This study provides theoretical guidance for the screening of optimal additives for high‐performance ZIBs.

Rational Design of High‐Loading Electrodes with Superior Performances Toward Practical Application for Energy Storage Devices

“…kinetics, structural breakdown of the electrode during use, limited active material utilization, and the complexities of fabricating thick electrodes. The proposed strategies to counteract these performance degradations encompass micro-nano structural designs, heteroatom doping, additive enhancements, [31] and refining the electrode fabrication process (Figure 1). In light of recent research advancements, we further suggest potential pathways for the development of high-loading electrodes suitable for industrial manufacturing and commercial deployment.…”

An effective descriptor for the screening of electrolyte additives toward the stabilization of Zn metal anodes

“…4g and Table S2, ESI †). 38,[43][44][45][46][47][48][49][50][51] The interfacial kinetics of the Zn anode was evaluated by the rate performance of symmetric cells (Fig. 4e).…”

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

“…The primary contributing factor to this predicament lies in the limited single‐role function and barren optimization capabilities of the current electrolyte additives [20,25] . Meanwhile, the majority of these additives are inappropriate for environmentally sustainable or commercially viable large‐scale applications due to their toxicity, flammability, instability, and readily sacrificable [20,24a,26] . The development of a multifunctional electrolyte additive that encompasses multiple mechanisms of action and exhibits superior optimization performance is crucial for the realization of high‐rate and long‐life Zn anodes for AZIBs [1a,20,27] .…”