Light-Field Orchestrated Tandem Photothermal Catalysis for Highly Selective CO <sub>2</sub> -To-C <sub>2+</sub> Olefin Conversion
Shangbo Ning, Xiuting Wu, Hui Song, Xinyu Ma, Shengying Yue, Senlin Zhang, Linjun Tang, R. J. LIU, Xingyu Yin, Shuxin Ouyang, Jinhua Ye
Abstract
The direct photothermal conversion of CO 2 into multicarbon olefins with high selectivity presents a promising route for sustainable carbon utilization. However, achieving high activity and selectivity simultaneously remains a formidable challenge due to intrinsic trade-offs in catalytic efficiency. Here, we introduce a spatially modulated light-field that orchestrates tandem active sites, enabling one-pot CO 2 -to-olefin conversion. Light-field-driven reduction rapidly transforms bimetallic ferrite into alloyed carbide in situ, forming synergistic CoFe oxide/carbide interfaces. At a CO 2 conversion of 39.6%, the optimized system in a batch reactor delivers a C 2–4 olefin productivity of 2.05 mmol g –1 h –1, of which 78.5% corresponds to C 2 H 4 and C 3 H 6, while under flow conditions it achieves a C 2+ olefin selectivity of 72% among the hydrocarbon products, thereby establishing a benchmark for photothermal CO 2 -to-olefin conversion. Mechanistic investigations demonstrate that light-modulated interfacial coupling between oxide and alloy carbide phases dynamically reconfigures the electronic structure of unsaturated CoFe active sites, thereby mitigating mass-transfer limitations during C 1 -intermediate hydrogenation and directing selectivity toward C 2+ olefins. Furthermore, scalability tests confirm the feasibility of this approach, as an integrated reactor system produces 66.1 L m –2 of C 2–4 olefins per day under ambient sunlight. This work paves the way for advanced light-driven catalytic systems for industrial CO 2 high value-added conversion.