Positively Charged Amino Acid-Modulated Interfacial Chemistry and Deposition Textures for Highly Reversible Zinc Anodes.

Abstract

Interfacial active water molecule-induced parasitic reactions and stochastic Zn2+ transport-caused dendrite issue significantly impede the implementation of aqueous Zn-ion batteries. Herein, three positively charged amino acids, namely arginine, histidine, and lysine, were utilized as adsorption-type electrolyte additives to enhance the stability and reversibility of Zn anodes. Combined theoretical and experimental analyses verified that these amino acid cations can synergistically modulate the interfacial microenvironment and promote orientational Zn deposition. The adsorbed amino acid cations reconfigured the interfacial electric double layer structure, forming SO42-- and H2O-poor interfaces, thereby retarding hydrogen evolution and corrosion side reactions. Simultaneously, the preferential adsorption of the amino acid cations at specific facets induced crystallographic orientational Zn deposition along unterminated facets. Three deposition architectures, namely planar texture, subvertical alignment, and vertical erection, were obtained, all effectively inhibiting dendrite formation. Consequently, symmetric cells with the three amino acid cations exhibited high stripping/plating reversibility of over 2000 cycles at 5 mA cm-2. Moreover, MnO2-based full cells exhibited markedly improved stabilities compared with their additive-free counterparts.