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Finned Zn-MFI zeolite encapsulated noble metal nanoparticle catalysts for the oxidative dehydrogenation of propane with carbon dioxide

Journal 2023 · IF 13.1 · 发表于 2023 年 2 月 13 日
作者: En-Hui Yuan,Yiming Niu,Xing Huang,Meng Li,Jun Bao,Yong-Hong Song,Bingsen Zhang,Zhao-Tie Liu,Marc-Georg Willinger,Zhong-Wen Liu
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摘要

Oxidative dehydrogenation of propane with carbon dioxide (CO 2 -ODP) characterizes the tandem dehydrogenation of propane to propylene with the reduction of the greenhouse gas of CO 2 to valuable CO. However, the existing catalyst is limited due to the poor activity and stability, which hinders its industrialization. Herein, we design the finned Zn-MFI zeolite encapsulated noble metal nanoparticles (NPs) as bifunctional catalysts (NPs@Zn-MFI) for CO 2 -ODP. Characterization results reveal that the Zn 2+ species are coordinated with the MFI zeolite matrix as isolated cations and the NPs of Pt, Rh, or RhPt are highly dispersed in the zeolite crystals. The isolated Zn 2+ cations are very effective for activating the propane and the small NPs are favorable for activating the CO 2 , which synergistically promote the selective transformation of propane and CO 2 to propylene and CO. As a result, the optimal 0.25%Rh0.50%Pt@Zn-MFI catalyst shows the best propylene yield, satisfactory CO 2 conversion, and long-term stability. Moreover, considering the tunable synergetic effects between the isolated cations and NPs, the developed approach offers a general guideline to design more efficient CO 2 -ODP catalysts, which is validated by the improved performance of the bifunctional catalysts via simply substituting Sn 4+ cations for Zn 2+ cations in the MFI zeolite matrix.

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