Tracking Mechanistic Pathway of Photocatalytic CO2 Reaction at Ni Sites Using Operando, Time-Resolved Spectroscopy

化学 催化作用 人工光合作用 光催化 光谱学 超快激光光谱学 吸收光谱法 均相催化 催化循环 光化学 纳米技术 材料科学 有机化学 物理 量子力学
作者
Yangguang Hu,Fei Zhan,Qian Wang,Yujian Sun,Can Yu,Xuan Zhao,Hao Wang,Ran Long,Guozhen Zhang,Chao Gao,Wenkai Zhang,Jun Jiang,Ye Tao,Yujie Xiong
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:142 (12): 5618-5626 被引量:154
标识
DOI:10.1021/jacs.9b12443
摘要

Harvesting solar energy for catalytic conversion of CO2 into valuable chemical fuels/feedstocks is an attractive yet challenging strategy to realize a sustainable carbon-cycle utilization. Homogeneous catalysts typically exhibit higher activity and selectivity as compared with heterogeneous counterparts, benefiting from their atomically dispersed catalytic sites and versatile coordination structures. However, it is still a "black box" how the coordination and electronic structures of catalysts dynamically evolve during the reaction, forming the bottleneck for understanding their reaction pathways. Herein, we demonstrate to track the mechanistic pathway of photocatalytic CO2 reduction using a terpyridine nickel(II) complex as a catalyst model. Integrated with a typical homogeneous photosensitizer, the catalytic system offers a high selectivity of 99% for CO2-to-CO conversion with turnover number and turnover frequency as high as 2.36 × 107 and 385.6 s-1, respectively. We employ operando and time-resolved X-ray absorption spectroscopy, in combination with other in situ spectroscopic techniques and theoretical computations, to track the intermediate species of Ni catalyst in the photocatalytic CO2 reduction reaction for the first time. Taken together with the charge dynamics resolved by optical transient absorption spectroscopy, the investigation elucidates the full mechanistic reaction pathway including some key factors that have been often overlooked. This work opens the "black box" for CO2 reduction in the system of homogeneous catalysts and provides key information for developing efficient catalysts toward artificial photosynthesis.
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