UNDERSTANDING AND DESIGNING INTERPHASE IN ZINC AND LITHIUM ANODES
Interphase instability has long been recognized as a significant challenge for rechargeable battery electrodes, encompassing metal-ion anodes, metal anodes, layered cathodes, and other components. Unraveling the fundamental failure mechanisms underlying interphase instability necessitates interdisciplinary collaboration, drawing from fields such as chemistry, chemical engineering, materials science, and leveraging various technologies such as advanced electron microscopy and in-situ visualization, etc. In this thesis, our focus lies in analyzing the chemical structure, reaction kinetics, and diffusion kinetics from the perspectives of chemistry and chemical engineering to elucidate the root causes of interphase instability in Zinc (Zn) and Lithium (Li) anodes. Despite the promising attributes of cost-effective and safe aqueous Zn batteries for next-generation battery systems, they face challenges such as rampant dendrite growth, severe corrosion reactions, and low energy density, among others. Similarly, while Li metal anodes offer high energy density and voltage, their unstable interphase limits capacity and cycle life during reversible cycling processes. To address these issues, we designed a range of artificial interphases tailored to mitigate different forms of interphase instabilities, including polymer adsorption interphases, iCVD polymer deposition interphases, and metal ion replacement interphases, among others. Our investigations revealed that these interphases can modulate the chemical composition of Zn/Li anodes and influence the deposition morphology of Zn/Li metal. Compared to interphases formed by side reactions, artificial interphases offer enhanced stability and controllability. Furthermore, they regulate the reaction and diffusion rates of ions at the interphase, enabling the attainment of reversible high-capacity metallic Zn and Li anode.