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十元环沸石上催化己烷裂解过程的选择性描述符。

Selectivity descriptors of the catalytic -hexane cracking process over 10-membered ring zeolites.

作者信息

Ma Pandong, Zhou Hexun, Li Yubing, Wang Mengheng, Nastase Stefan Adrian F, Zhu Mengsi, Cui Jiale, Cavallo Luigi, Cheng Kang, Dutta Chowdhury Abhishek

机构信息

College of Chemistry and Molecular Sciences, Wuhan University Wuhan 430072 Hubei PR China

State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University Xiamen 361005 PR China

出版信息

Chem Sci. 2024 Jun 24;15(30):11937-11945. doi: 10.1039/d4sc00603h. eCollection 2024 Jul 31.

DOI:10.1039/d4sc00603h
PMID:39092105
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11290429/
Abstract

Zeolite-mediated catalytic cracking of alkanes is pivotal in the petrochemical and refining industry, breaking down heavier hydrocarbon feedstocks into fuels and chemicals. Its relevance also extends to emerging technologies such as biomass and plastic valorization. Zeolite catalysts, with shape selectivity and selective adsorption capabilities, enhance efficiency and sustainability due to their well-defined network of pores, dimensionality, cages/cavities, and channels. This study focuses on the alkane cracking over 10-membered ring (10-MR) zeolites under industrially relevant conditions. Through a series of characterizations, including UV-vis spectroscopy and solid-state NMR spectroscopy, we intend to address mechanistic debates about the alkane cracking mechanism, aiming to understand the dependence of product selectivity on zeolite topologies. The findings highlight topology-dependent mechanisms, particularly the role of intersectional void spaces in zeolite ZSM-5, influencing aromatic-based product selectivity. This work provides a unique understanding of zeolite-catalyzed hydrocarbon conversion, linking alkane activation steps to the traditional hydrocarbon pool mechanism, contributing to the fundamental knowledge of this crucial industrial process.

摘要

沸石介导的烷烃催化裂化在石油化工和炼油工业中至关重要,它能将较重的烃类原料分解为燃料和化学品。其相关性还延伸到生物质和塑料增值等新兴技术领域。沸石催化剂具有形状选择性和选择性吸附能力,由于其明确的孔网络、维度、笼/腔和通道,可提高效率和可持续性。本研究聚焦于在工业相关条件下10元环(10-MR)沸石上的烷烃裂化。通过一系列表征,包括紫外可见光谱和固态核磁共振光谱,我们旨在解决有关烷烃裂化机理的机制争论,旨在了解产物选择性对沸石拓扑结构的依赖性。研究结果突出了拓扑结构依赖性机制,特别是ZSM-5沸石中交叉空隙空间的作用,影响基于芳烃的产物选择性。这项工作为沸石催化的烃类转化提供了独特的理解,将烷烃活化步骤与传统的烃池机理联系起来,有助于深入了解这一关键工业过程的基础知识。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d50/11290429/bb90523b1375/d4sc00603h-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d50/11290429/253da4570c5d/d4sc00603h-f1.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d50/11290429/95608a625980/d4sc00603h-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d50/11290429/bb90523b1375/d4sc00603h-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d50/11290429/253da4570c5d/d4sc00603h-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d50/11290429/0e3d6938afef/d4sc00603h-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d50/11290429/35db35aebe8f/d4sc00603h-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d50/11290429/95608a625980/d4sc00603h-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6d50/11290429/bb90523b1375/d4sc00603h-s1.jpg

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本文引用的文献

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Molecular Views on Mechanisms of Brønsted Acid-Catalyzed Reactions in Zeolites.沸石中布朗斯特酸催化反应机理的分子观点
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Low-temperature upcycling of polyolefins into liquid alkanes via tandem cracking-alkylation.通过串联裂化-烷基化将聚烯烃低温升级为液体烷烃。
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Selectivity descriptors for the direct hydrogenation of CO to hydrocarbons during zeolite-mediated bifunctional catalysis.沸石介导双功能催化过程中CO直接加氢制烃的选择性描述符。
Nat Commun. 2021 Oct 8;12(1):5914. doi: 10.1038/s41467-021-26090-5.
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