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Synergistic mechanism of isolated Fe3+ and highly dispersed Ptδ+ over zeolite for boosting propane dehydrogenation

Journal 2023 · IF 3.7 · 69(12): e18249 · 发表于 2023 年 9 月 21 日
作者: Ying Zhang,Xiaofang Wang,Huihui Deng,Qin Sun,Baozhen Li,Wenchun Zheng,Zhuangzhuang Ren,Xiangqing Fang,Li Tan,Yu Tang,Lizhi Wu
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摘要

Pt-based catalysts have been widely investigated in propane dehydrogenation (PDH) owing to their high activity in C  H activation, while it suffers from Pt sintering and coke deposition. We develop a transition metal Fe and zeolite support synergistic-modified method to realize the highly dispersed and stable Pt species inside zeolite over Pt/Fe-silicate-1. And it shows the excellent PDH performance with propylene generation rate of 51.6 mol C 3 H 6 g Pt −1 h −1 and low deactivation rate constant k d of 0.017 h −1 as well as a high TOF Pt of 37.6 s −1 at 550°C. The systematic characterizations reveal the isolated Fe 3+ species could significantly improve Pt dispersity and regulate Pt electronic density to realize a more positive Pt δ+ species inside Silicalite-1 pore. And the further in situ DRIFTS experiments demonstrate that the synergistic effect between the appropriate acidic Fe sites and the highly dispersed Pt δ+ species around Fe species are responsible for the superior PDH performance.