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氮掺杂碳负载催化剂上环烷烃的脱氢反应：活性组分和底物分子结构的影响

Dehydrogenation of Cycloalkanes over N-Doped Carbon-Supported Catalysts: The Effects of Active Component and Molecular Structure of the Substrate.

作者信息

Wang Jian, Liu He, Fan Shiguang, Wang Shuai, Xu Guanjun, Guo Aijun, Wang Zongxian

机构信息

State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao 266580, China.

出版信息

Nanomaterials (Basel). 2021 Oct 26;11(11):2846. doi: 10.3390/nano11112846.

DOI:10.3390/nano11112846
PMID:34835611
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8617684/
Abstract

Efficient dehydrogenation of cycloalkanes under mild conditions is the key to large-scale application of cycloalkanes as a hydrogen storage medium. In this paper, a series of active metals loaded on nitrogen-doped carbon (M/CN, M = Pt, Pd, Ir, Rh, Au, Ru, Ag, Ni, Cu) were prepared to learn the role of active metals in cycloalkane dehydrogenation with cyclohexane as the model reactant. Only Pt/CN, Pd/CN, Rh/CN and Ir/CN can catalyze the dehydrogenation of cyclohexane under the set conditions. Among them, Pt/CN exhibited the best catalytic activity with the TOF value of 269.32 h at 180 °C, followed by Pd/CN, Rh/CN and Ir/CN successively. More importantly, the difference of catalytic activity between these active metals diminishes with the increase in temperature. This implies that there is a thermodynamic effect of cyclohexane dehydrogenation with the synthetic catalysts, which was evidenced by the study on the activation energy. In addition, the effects of molecular structure on cycloalkane dehydrogenation catalyzed by Pt/CN were studied. The results reveal that cycloalkane dehydrogenation activity and hydrogen production rate can be enhanced by optimizing the type, quantity and position of alkyl substituents on cyclohexane.

摘要

在温和条件下实现环烷烃的高效脱氢是环烷烃作为储氢介质大规模应用的关键。本文制备了一系列负载在氮掺杂碳上的活性金属（M/CN，M = Pt、Pd、Ir、Rh、Au、Ru、Ag、Ni、Cu），以环己烷为模型反应物研究活性金属在环烷烃脱氢反应中的作用。在设定条件下，只有Pt/CN、Pd/CN、Rh/CN和Ir/CN能催化环己烷脱氢。其中，Pt/CN表现出最佳催化活性，在180℃时的TOF值为269.32 h，其次依次为Pd/CN、Rh/CN和Ir/CN。更重要的是，随着温度升高，这些活性金属之间的催化活性差异减小。这意味着合成催化剂对环己烷脱氢存在热力学效应，这一点通过活化能研究得到了证实。此外，研究了分子结构对Pt/CN催化环烷烃脱氢的影响。结果表明，通过优化环己烷上烷基取代基的类型、数量和位置，可以提高环烷烃脱氢活性和产氢速率。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/78f0e4d41d14/nanomaterials-11-02846-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/a6bf80396108/nanomaterials-11-02846-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/7d448d3eaea5/nanomaterials-11-02846-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/f798b193f601/nanomaterials-11-02846-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/5698855e064b/nanomaterials-11-02846-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/1fd0310a0f8e/nanomaterials-11-02846-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/7a4c294bb97d/nanomaterials-11-02846-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/f96a4f564429/nanomaterials-11-02846-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/7f21ff7d7dc7/nanomaterials-11-02846-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/928e9bf1774d/nanomaterials-11-02846-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/78f0e4d41d14/nanomaterials-11-02846-g010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/a6bf80396108/nanomaterials-11-02846-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/7d448d3eaea5/nanomaterials-11-02846-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/f798b193f601/nanomaterials-11-02846-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/5698855e064b/nanomaterials-11-02846-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/1fd0310a0f8e/nanomaterials-11-02846-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/7a4c294bb97d/nanomaterials-11-02846-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/f96a4f564429/nanomaterials-11-02846-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/7f21ff7d7dc7/nanomaterials-11-02846-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/928e9bf1774d/nanomaterials-11-02846-g009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8282/8617684/78f0e4d41d14/nanomaterials-11-02846-g010.jpg

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