Lunar‐Based Photothermal CO 2 Reduction Strategy: Self‐Evolving Transient Active Interface and Band Engineering

ABSTRACT Inspired by lunar soil composition, we constructed a dynamically adaptive Pd/Ov‐FeTiO 3 photothermal catalyst for in situ resource utilization. Under photothermal conditions, the catalyst undergoes significant self‐evolution, forming a transient active interface rich in oxygen vacancies (Ov) and palladium. This unique structure effectively enhances the adsorption of CO 2 and key intermediates by shifting the d‐band center upward, while reconstructing the interfacial electron transport pathway, enabling rapid transfer of photogenerated electrons to the reactants. Furthermore, Ov‐induced d‐d transitions successfully release the energy of infrared photons, extending the photoresponse range to the near‐infrared region and significantly improving the full‐spectrum utilization efficiency of sunlight. In the photothermal CO 2 hydrogenation reaction at 300°C, the optimized catalyst exhibits a CO generation rate of 33.23 mol g Pd − 1 h − 1 , maintaining excellent performance in the visible‐infrared region. By combining femtosecond transient absorption spectroscopy, in situ XPS, in situ EPR, and DFT calculations, this study reveals the core role of transient active interfaces in promoting charge separation, lowering reaction energy barriers, and guiding reaction pathways. It not only proposes a highly efficient photothermal catalytic material design strategy based on a “self‐evolution” mechanism but also provides a practical pathway for extraterrestrial artificial photosynthesis, marking a crucial step toward practical application.