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用于环己烯一步转化为己二酸的AgWCN纳米复合材料的合成及其机理研究。

Synthesis of AgWCN Nanocomposites for the One-Step Conversion of Cyclohexene to Adipic Acid and Its Mechanistic Studies.

作者信息

Goyal Reena, Sameer Siddharth, Sarkar Bipul, Bag Arijit, Singhal Nikita, Bordoloi Ankur

机构信息

Nano Catalysis area, Refinery Technology Division, CSIR-Indian Institute of Petroleum, Dehradun, 248005, India.

Chemical Science Division, CSIR-Indian Institute of Petroleum, Dehradun, 248005, India.

出版信息

Chemistry. 2017 Nov 21;23(65):16555-16565. doi: 10.1002/chem.201703111. Epub 2017 Nov 2.

DOI:10.1002/chem.201703111
PMID:28891230
Abstract

A novel catalyst composed of silver nanoparticles grafted on WCN has been prepared by using a facile pH-adjusted method. The material reported in this study presents a non-mineral acid route for the synthesis of the industrially significant monomer adipic acid through the selective oxidation of cyclohexene. Ag has been stabilized in the hydrophobic matrix during the formation of the mesoporous silica material by using aniline as stabilizing agent. A cyclohexene conversion of 92.2 % with 96.2 % selectivity for adipic acid was observed with the AgWCN -2 catalyst, therefore, the AgWCN catalyst was found to be efficient for the direct conversion to adipic acid with respect to their monometallic counterparts. The energy profile diagrams for each reaction path by using the AgWCN catalyst were studied along with their monometallic counterparts by using the Gaussian 09 package. The reported material can avoid the use of harmful phase-transfer catalysts (PTC) and/or chlorinated additives, which are two among other benefits of the reported work.

摘要

通过一种简便的pH调节方法制备了一种由接枝在WCN上的银纳米颗粒组成的新型催化剂。本研究报道的材料提供了一种非无机酸途径,通过环己烯的选择性氧化来合成具有工业重要性的单体己二酸。在介孔二氧化硅材料形成过程中,通过使用苯胺作为稳定剂,银已稳定在疏水基质中。使用AgWCN -2催化剂时,观察到环己烯转化率为92.2%,己二酸选择性为96.2%,因此,相对于其单金属对应物,发现AgWCN催化剂对于直接转化为己二酸是有效的。使用高斯09软件包,研究了使用AgWCN催化剂的每个反应路径的能量分布图及其单金属对应物的能量分布图。所报道的材料可以避免使用有害的相转移催化剂(PTC)和/或氯化添加剂,这是所报道工作的其他好处之一。

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