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Abstract
Addressing global energy and environmental challenges requires integrated solutions that enable both sustainable energy storage and carbon dioxide utilization. This dissertation investigates interfacial and nanoconfined metal architectures for two key aqueous electrochemical systems: Sn metal-based batteries and electrochemical CO2 reduction toward high multi-carbon products. These two systems are unified by a common strategy, molecular-level control of interfacial chemistry and microenvironment to overcome efficiency, selectivity, and stability limitations.
In aqueous Sn metal batteries, challenges such as poor reversibility caused by dead Sn formation and hydrogen evolution are mitigated through interfacial engineering (Chapter 2) and co-cation regulation (Chapter 3). The inertness of Sn toward hydrogen evolution and its isotropic growth behavior makes it particularly well-suited for aqueous environments, especially under acidic conditions where traditional Zn-based batteries struggle. Through surface modification and electrolyte optimization, these works achieve high Coulombic efficiency, extended cycling life, and competitive energy densities, establishing Sn as a viable alternative anode for aqueous battery technologies.
In parallel, this dissertation explores the role of nanoconfinement and microenvironment modulation in steering eCO2RR selectivity. Cu single atom-based catalysts supported on microporous carbon frameworks are developed to enhance *CO intermediate stabilization and promote C–C and C2–C1 coupling (Chapter 4). These catalysts exhibit high Faradaic efficiency toward C2+ alcohol products, including glycerol and ethanol. Structure–function relationships reveal that micropore size and adsorption enthalpy play key roles in controlling reaction pathways, intermediate coverage, and product branching.
Together, these studies establish a coherent design framework in which interfacial chemistry, ion transport, and nanoconfinement are leveraged to enhance the performance of aqueous electrochemical systems. By connecting insights from energy storage and CO2 conversion, these works contribute fundamental understanding and practical strategies toward multifunctional electrochemical platforms that support carbon neutrality and sustainable energy integration.