Engineering dual active metal sites on metal-organic frameworks for photocatalytic CO2 reduction

Photocatalytic CO2 reduction (CO2RR) presents a promising strategy for addressing the global challenges of CO2 emissions and renewable energy utilization.Metal-organic frameworks (MOFs) have received extensive research attention for their applications in CO2RR due to their superior CO2 capture capabilities, photochemical properties, and structural tunability.In this thesis, we investigated the atomic-level engineering of the dual metal active sites on metal-organic frameworks to optimize photocatalytic CO2RR performance.We systemically evaluated how dual-atom catalysts (DACs), metal loading density, and bimetallic combinations (electronic structure tuning) influence the selectivity and efficiency of CO2 conversion, particularly towards high-value multicarbon (C2+) products.Combining experimental results with theoretical modeling, we established structure-activity relationships and developed rational design principles for optimizing MOF-based photocatalysts with tailored dual metal site.Advanced characterization techniques, including transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), X-ray absorption fine structure (XAFS) analysis, and photoluminescence (PL) were employed to probe the coordination environment and photoinduced charge transfer capability of catalysts.