Nov 2025
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Committee Members Information
Abstract
The photothermal hydrogenation of CO2 offers a promising route for the sustainable synthesis of fuels and chemicals by utilizing solar energy. By combining thermal and photon-induced effects, this approach enhances catalytic activity under relatively mild conditions, thereby reducing overall energy input and bridging the gap between renewable energy utilization and carbon-neutral fuel production. This dissertation presents a systematic investigation into catalyst design, mechanistic understanding, and performance optimization of photothermal catalysis for CO2 hydrogenation, covering from reverse water gas shift (RWGS) to produce CO to more complex Fischer-Tropsch (FTS) like catalysts to produce C2+ hydrocarbons.
Firstly, indium-based catalysts are developed for RWGS. The introduction of surface defects on indium-based catalysts markedly improves light-harvesting capability and catalytic activity, enabling efficient CO formation at lower reaction temperatures. Later on, a potassium-promoted CuFe catalyst is engineered to couple the reverse water-gas shift (RWGS) reaction with Fischer-Tropsch synthesis (FTS), where plasmon-induced hot carrier generation promotes the formation of active iron carbide species under lower temperatures. Additionally, potassium-promoted FeMn catalysts are explored, revealing that controlled Mn incorporation optimizes active phase composition and chain-growth probability. These systems demonstrate efficient hydrocarbon formation under both mild and industrially relevant conditions.