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AICHE JOURNAL · 2023 ·Vol. 69 ·期 12 ·e18249 · IF 3.7

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

Ying Zhang,Xiaofang Wang,Huihui Deng,Qin Sun,Baozhen Li,Wenchun Zheng,Zhuangzhuang Ren,Xiangqing Fang,Li Tan,Yu Tang,Lizhi Wu

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.

研究领域: 催化化学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Heteroatom doping-induced Pt dispersion and electronic effect for boosting the catalytic performance in the hydrogenation of nitrobenzene to p-aminophenol

Chong Yao,Jiwei Wu,Limei Pan,Lu Yu,Jie Luo,Jinjin Shan,Jie Liu,Chunshan Lu,Feng Feng,Xiaoliang Xu,Lili Lin,Yuxue Yue,Qingtao Wang,Jia Zhao,Qunfeng Zhang,Xiaonian Li

N-doped carbon materials were synthesized using a straightforward salt template method for Pt metal modification, resulting in a reduction in particle size from 4.8 nm to 2.1 nm due to the interaction between Pt and the carrier. The hydrogenation activity of nitrobenzene increased by 4.5 times compared to undoped catalysts. Additionally, the electronic effects of N and Pt enhanced the selectivity of p-aminophenol by up to 20.4 %. The anchoring of Pt by N improved the stability of active metal centers in a strong acidic system, thereby retarding Pt loss. Theoretical calculations and characterization revealed that the enhancement of activity relied on the high dispersion of Pt, while the improvement in product selectivity was associated with changes in the adsorption strength of the phenylhydroxylamine intermediate. N anchoring of Pt, inducing an electron effect, disentangled the activity and selectivity of nitrobenzene hydrogenation for the preparation of p-aminophenol.

研究领域: 催化 · 材料科学 · 化学工程
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