Author ORCID Identifier

https://orcid.org/0000-0001-8274-6882

Semester

Summer

Date of Graduation

2026

Document Type

Dissertation

Degree Type

PhD

College

Statler College of Engineering and Mineral Resources

Department

Mechanical and Aerospace Engineering

Committee Chair

Xingbo Liu

Committee Co-Chair

Shanshan Hu

Committee Member

Wenyuan Li

Committee Member

Wei Li

Committee Member

Konstantinos A. Sierros

Committee Member

Xiaolin Li

Abstract

Aqueous zinc-ion batteries (AZIBs) have become increasingly attractive as grid-scale energy storage solutions due to their safety, low cost, and environmental friendliness. However, the anode-electrolyte interface in AZIBs is prone to instability due to severe dendrite growth, self-corrosion, parasitic water-induced side reactions, and hydrogen evolution reactions (HER), which collectively lead to poor cyclability. To date, various interfacial engineering strategies have been investigated to address these challenges and improve the stability of Zn metal anodes. This dissertation presents a unified strategy for regulating Zn deposition through synergistic electrode and electrolyte design in laboratory-scale coin cells and then applies these concepts to practical pouch-cell configurations.

For the typical laboratory-scale coin cell, high-stability Zn anodes and high-performance AZIBs are developed through synergistic strategies that combine a molybdenum dioxide coating layer on Zn (MoO2@Zn) with Tween 80 as an electrolyte additive in the first study, and, in the second work, a hybrid metallic cation-anionic surfactant additive (La3+ and sodium dodecyl sulfate) is introduced. To better understand the reasons for the improved battery performance, the regulatory mechanisms of these systems in AZIBs have been thoroughly examined using material and electrochemical characterization and stimulation methods. Building on these coin-cell studies, the final study focuses on scaling up to practical pouch-type cells and explores how electrolyte additives mitigate electrochemical heterogeneity caused by realistic cell geometries. Through systematic investigations of different additives in ZnSO4 electrolyte, such as β-cyclodextrin and Tween 80, distinct roles in regulating bulk ion transport and interfacial adsorption are identified, revealing how these additives mitigate non-uniform electric-field and Zn2+ flux distributions in practical cell architectures.

Overall, this research establishes a comprehensive framework for stabilizing Zn metal anodes through interfacial engineering, including surface coatings and electrolyte additives, and for practical, scaled-up pouch-type cells. The findings provide fundamental insights into Zn deposition behavior and offer design principles for developing durable, scalable aqueous ZIBs.

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