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通过钾促进的沸石封装铂催化剂调节非氧化烷烃脱氢反应的选择性

Tuning the Selectivity in the Nonoxidative Alkane Dehydrogenation Reaction by Potassium-Promoted Zeolite-Encapsulated Pt Catalysts.

作者信息

Gong Nengfeng, Zhou Runhui, Wan Hongliu, Hou Huaming, Dou Xiaomeng, Gong Jianhong, He Peng, Liu Lichen

机构信息

State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, P. R. China.

National Energy Center for Coal to Clean Fuels, Synfuels China Technology Co., Ltd., Beijing 101407, P. R. China.

出版信息

JACS Au. 2024 Dec 1;4(12):4934-4947. doi: 10.1021/jacsau.4c00949. eCollection 2024 Dec 23.

Abstract

The significance of the nonoxidative dehydrogenation of middle-chain alkanes into corresponding alkenes is increasing in the context of the world's declining demands on transportation fuels and the growing demand for chemicals and materials. The middle-chain alkenes derived from the dehydrogenation reaction can be transformed into value-added chemicals in downstream processes. Due to the presence of multiple potential reaction sites, the reaction mechanism of the dehydrogenation of middle-chain alkanes is more complicated than that in the dehydrogenation of light alkanes, and there are few prior studies on elucidating their detailed structure-reactivity relationship. In this work, we have employed Pt catalysts encapsulated in pure-silica MFI zeolite crystallites as model catalysts and studied how the catalytic performances for dehydrogenation of -pentane can be modulated by the K promotor in the Pt-MFI catalyst. A combination of comprehensive structural characterizations by aberration-corrected electron microscopy, X-ray absorption spectroscopy, in situ CO-IR, X-ray photoelectron spectroscopy, and kinetic studies shows that K promoter can not only influence the particle size but also modify the electronic properties of Pt species, which further affect the activity and selectivity in the dehydrogenation of -pentane.

摘要

在全球对运输燃料需求下降以及对化学品和材料需求不断增长的背景下,中链烷烃非氧化脱氢生成相应烯烃的重要性日益凸显。由脱氢反应得到的中链烯烃可在下游工艺中转化为高附加值化学品。由于存在多个潜在反应位点,中链烷烃脱氢的反应机理比轻烷烃脱氢更为复杂,且此前鲜有关于阐明其详细结构-反应活性关系的研究。在这项工作中,我们采用封装在纯硅MFI沸石微晶中的Pt催化剂作为模型催化剂,研究了Pt-MFI催化剂中的K助剂如何调节对戊烷脱氢的催化性能。通过校正像差电子显微镜、X射线吸收光谱、原位CO-IR、X射线光电子能谱等综合结构表征以及动力学研究表明,K助剂不仅能影响粒径,还能改变Pt物种的电子性质,进而影响戊烷脱氢的活性和选择性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b7d0/11672148/0022ae8fa97e/au4c00949_0001.jpg

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