Bimetallic Ni-Zn site anchored in siliceous zeolite framework for synergistically boosting propane dehydrogenation

双金属片 脱氢 催化作用 丙烷 烧结 焦炭 化学工程 选择性 材料科学 沸石 解吸 无机化学 吸附 化学 有机化学 冶金 工程类
作者
Chengming Huang,Dingmei Han,Linjie Guan,Linhua Zhu,Yi Mei,Dedong He,Yun Zu
出处
期刊:Fuel [Elsevier]
卷期号:307: 121790-121790 被引量:61
标识
DOI:10.1016/j.fuel.2021.121790
摘要

Propane dehydrogenation (PDH) is a prospective benign process for the production of propylene, but generally depends on high-price Pt and toxic Cr(VI) catalysts that often suffer from the rapid deactivation derived from metal sintering and severe coke deposition. To overcome these problems, the breakthroughs in an alternative catalyst design with efficient, low-cost and eco-friendly play a crucial role in successfully developing this process. Here, we facilely fabricate the bimetallic-site catalyst of Ni-Zn anchored in the zeolitic framework of silicalite-1 (depicted as NiZn-S-1) by employing ligand-protected strategy, which performs high temperature stability. Under comparable conditions, the NiZn-S-1 catalyst with high Ni/Zn molar ratio of 3:1 (named 0.2Ni0.06Zn-S-1) exhibits superior catalytic activity (initial propane conversion of 32.5 % and actual TOFpropane of 28.5 min−1) with low deactivation rate (0.0778 h−1) and great propylene selectivity (>90%) after 30 h on stream. In particular, the catalytic performance on this catalyst almost keeps same as that of fresh catalyst after 4 successive oxidation–reduction cycles. Multiple characterizations further demonstrate that the enhancement of PDH performance ought to be attributed to the synergistic effect between bimetallic Ni-Zn sites, which favors the selective activation of C–H bond and propylene desorption to reduce the formation of coke species with high graphitization degree, boosting the improvement of catalyst stability. The design of novel bimetallic-sites catalyst can give a new idea on the development of alternative PDH catalysts with economical- and environment-friendly in the future.
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