Toward Cost-Effective Stable Zn Battery Anodes: Design Concepts for Scalable Electrochemical Energy Storage

ConspectusZinc (Zn) metal batteries are among the most extensively studied and practically deployed electrochemical energy storage systems, owing to their low cost, intrinsic safety, environmental benignity, and natural compatibility with aqueous electrolytes. These attributes render Zn-based batteries attractive for large-scale stationary storage, wearable and flexible electronics, and emerging applications that require high operational safety and mechanical robustness. Despite these advantages, the widespread adoption of Zn metal batteries is limited by their relatively low energy density and poor cycling stability, which originate primarily from the complex, dynamic, and typically unstable electrochemical behavior of the Zn metal anode during repeated plating and stripping. Addressing these challenges requires a mechanistic understanding of Zn electrodeposition and interfacial processes across multiple length and time scales, spanning atomistic ion transport and interfacial reactions, mesoscale morphology evolution, and macroscopic nno-planar growth of the deposits to ultimately compromise cell performance. In this Account, we summarize our recent efforts to elucidate and engineer Zn metal anodes for reversible and stable operation under both conventional and extreme electrochemical conditions, with the goal of bridging fundamental insights into Zn deposition dynamics with practical strategies for enhancing battery durability and performance. We begin by establishing the fundamental principles governing Zn electrodeposition, with a particular focus on the crystallographic control of Zn growth. By inducing preferentially textured (002) Zn anodes, we demonstrate that dendritic and mossy Zn growth can be effectively suppressed in mildly acidic or neutral electrolytes, enabling smoother and more reversible Zn plating/stripping. These results provide a framework that links microscopic deposition dynamics to macroscopic electrochemical performance metrics, including Coulombic efficiency, cycling stability, and rate capability. Building on this foundation, we investigate the formation and functional roles of salt-induced solid–electrolyte interphases (SEIs) and artificially engineered interphases on Zn metal substrates. Through electrolyte engineering and interfacial design strategies, including initiated chemical vapor deposition (iCVD), we show that tailored interphases can regulate Zn2+ transport, homogenize interfacial ion flux, suppress parasitic side reactions, and stabilize the Zn/electrolyte interface over prolonged cycling. These interphases function not merely as passive protective layers, but as active regulators of interfacial electrochemistry that enable sustained Zn metal reversibility under demanding conditions. Importantly, we further explore Zn metal cycling under extreme environments, including highly alkaline electrolytes and electrochemical regimes characterized by hydrodynamic instability. Although such conditions are conventionally regarded as detrimental to Zn stability, they offer valuable opportunities to interrogate Zn deposition behavior beyond diffusion-limited assumptions. By examining Zn electrodeposition under these nonideal regimes, we uncover new pathways for achieving reversible Zn cycling and identify underexplored mechanisms governing interfacial stability. Beyond fundamental studies, we discuss the integration of Zn metal batteries into functional systems, including soft robotic platforms, where electrochemical stability must be preserved under dynamic mechanical deformation and unconventional operating environments. Finally, we outline remaining challenges and open questions for Zn metal batteries, including cathode selection and the identification of application spaces in which Zn-based systems offer distinct advantages over competing chemistries. Collectively, this Account distills design principles for stabilizing Zn metal anodes and provides guidance for the future development of durable, high-performance Zn metal batteries.