Boron-Induced Redispersion of Pt Species during Propane Dehydrogenation

脱氢 丙烷 催化作用 化学 环境科学 化学工程 有机化学 工程类
作者
Mengyang Liu,Shaobo Han,Wenna Zhang,Bin Gu,Jingmei Li,Chengyu Jin,Xin Rong,Chenglin Sun
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:15 (5): 4251-4258 被引量:13
标识
DOI:10.1021/acscatal.4c07243
摘要

In a propane dehydrogenation (PDH) reaction system, low-Pt catalysts generally suffer from rapid deactivation and poor durability due to easy sintering at high temperatures and in a reductive atmosphere. Herein, we develop a catalyst (PtSnK-B/Al2O3, named as PtSnK-B0.32) with both low Pt loading (0.15 wt %) and high durability by facile doping of trace boron into a conventional Pt-based catalyst. Density functional theory (DFT) calculations show that pure Pt clusters have weak binding energy with support, leading to a further undesired Pt sintering process. In contrast, when boron (B) is added to the Pt-based catalyst, the undesired Pt sintering process is significantly inhibited. Moreover, being initiated by propane molecules, the pure Pt clusters are readily to dissociate into Pt atoms due to their longer Pt-Pt bond lengths, then the dissociated Pt atoms are captured by B or BOx species to form stable Pt–B clusters under PDH conditions. The formation of highly dispersed Pt–B clusters allows the catalyst to achieve high intrinsic activity; compared with the catalyst without B (PtSnK, 0.14 wt % Pt), the Ea value of the B-doped catalyst is obviously reduced. Significantly, the durability of PtSnK-B0.32 is three times that of PtSnK and even twice that of 0.26PtSnK with a Pt loading of 0.26 wt %. The facile synthesis method, lower Pt content, and higher durability provide a promising application perspective.
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