Pt-Sn clusters anchored at Al_(penta)~(3+) sites as a sinter-resistant and regenerable catalyst for propane dehydrogenation

Pt-Sn clusters anchored at Al_(penta)~(3+) sites as a sinter-resistant and regenerable catalyst for propane dehydrogenation
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锚定在 Al_(penta)~(3 ) 位点上的 Pt-Sn 簇作为丙烷脱氢的抗烧结和可再生催化剂

DOI:
10.1016/j.jechem.2021.06.002
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发表时间:
2022
影响因子:
13.1
通讯作者:
Zhu Haibo
Zhu Haibo
中科院分区:
化学1区
文献类型:
--
作者:
Zhu Xinyue;Wang Tinghai;Xu Zhikang;Yue Yuanyuan;Lin Minggui;Zhu Haibo

文献摘要

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Pt-based catalysts are widely used in propane dehydrogenation reaction for the production of propylene.Suppressing irreversible deactivation caused by the sintering of Pt particles under harsh conditions and regeneration process is a significant challenge in this catalyst.Herein,a series of highly ordered mesoporous Al_2O_3 supports with different levels of Al_(penta)~(3+) sites,are fabricated and used as the support to disperse Pt-Sn_2 clusters.Characterizations of Pt-Sn_2/meso-Al_2O_3 with XRD,NMR,CO-IR,STEM,TG,and Raman techniques along with propane dehydrogenation-regeneration cycles test reveal the structure-stability-re generability relationship.The coordinatively unsaturated pentacoordinate Al~(3+) (Al_(penta)~(3+)) can strongly anchor Pt atoms via a formation of Al-O-Pt bond,and thus stabilize the Pt-based particles at the surface of Al_2O_3.The stability and regenerability of Pt-Sn_2/meso-Al_2O_3 are strongly dependent on the content of Al_(penta)~(3+) sites in the Al_2O_3 structure,and a high level of Al_(penta)~(3+) sites can effectively prevent the agglomeration of Pt-Sn_2 clusters into large Pt nanoparticles in the consecutive dehydrogenation-regeneration cycles.The Pt-Sn_2/meso-Al_2O_3-600 with the highest level of Al_(penta)~(3+) (50.8%) delivers the best performance in propane dehydrogenation,which exhibits propane conversion of 40% and propylene selectivity above 98% at 570 ℃ with 10 vol% C_3H_8 and 10 vol% H_2 feed.A slow deactivation in this catalyst is ascribed to the formation of coke,and the catalytic performance can be fully restored in the consecutive dehydrogenation-regeneration cycles via a simple calcination treatment.