水煤气变换反应
纳米棒
沮丧的刘易斯对
催化作用
化学
吸附
产量(工程)
铂金
化学工程
路易斯酸
物理化学
纳米技术
材料科学
有机化学
工程类
冶金
作者
Wenbin Li,Jie Gan,Yuxuan Liu,Yong Zou,Sai Zhang,Yongquan Qu
标识
DOI:10.1002/anie.202305661
摘要
The low-temperature reverse water-gas shift (RWGS) reaction faces the following obstacles: low activity and unsatisfactory selectivity. Herein, the dual-active sites of platinum (Pt) clusters and frustrated Lewis pair (FLP) on porous CeO2 nanorods (Ptcluster /PN-CeO2 ) provide an interface-independent pathway to boost high performance RWGS reaction at low temperatures. Mechanistic investigations illustrate that Pt clusters can effectively activate and dissociate H2 . The FLP sites, instead of the metal and support interfaces, not only enhance the strong adsorption and activation of CO2 , but also significantly weaken CO adsorption on FLP to facilitate CO release and suppress the CH4 formation. With the help of hydrogen spillover from Pt to PN-CeO2 , the Ptcluster /PN-CeO2 catalysts achieved a CO yield of 29.6 %, which is very close to the thermodynamic equilibrium yield of CO (29.8 %) at 350 °C. Meanwhile, the Ptcluster /PN-CeO2 catalysts delivered a large turnover frequency of 8720 h-1 . Moreover, Ptcluster /PN-CeO2 operated stably and continuously for at least 840 h. This finding provides a promising path toward optimizing the RWGS reaction.
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