Transesterification of ethylacetoacetate catalysed by metal free mesoporous carbon nitride

被引:24
作者
Anand, Chokkalingam [1 ]
Priya, Subramaniam Vishnu [1 ]
Lawrence, Geoffrey [1 ]
Mane, Gurudas P. [3 ]
Dhawale, Dattatray S. [1 ]
Prasad, Kumaresapillai S. [1 ]
Balasubramanian, Veerappan V. [2 ]
Wahab, Mohammad A. [1 ]
Vinu, Ajayan [1 ]
机构
[1] Univ Queensland, Australian Inst Bioengn & Nanotechnol, Brisbane, Qld 4072, Australia
[2] Rensselaer Polytech Inst, Howard P Isermann Dept Chem & Biol Engn, Troy, NY 12180 USA
[3] Natl Inst Mat Sci, MANA, Tsukuba, Ibaraki 3050044, Japan
关键词
Mesoporous; Carbon nitride; beta-Keto esters; Ethylenediamine; SBA-15; BETA-KETO-ESTERS; MECHANICAL STABILITY; ORGANIC-SOLVENTS; MOLECULAR-SIEVES; NITROGEN-CONTENT; PORE-SIZE; NANOPARTICLES;
D O I
10.1016/j.cattod.2012.07.025
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The basic catalytic performance of the mesoporous carbon nitride (MCN) for the transesterification of ethylacetoacetate with various alcohols such as 1-butanol, 1-octanol, cyclohexanol, benzyl alcohol and furfuryl alcohol under heterogeneous reaction conditions without using any solvents was demonstrated. The catalyst was prepared by using a nano-hard templating approach through a simple polymerisation reaction between ethylenediamine (EDA) and carbon tetrachloride (CTC) in the mesochannels of the SBA-15 followed by the carbonisation and the silica removal by HF. The material was thoroughly analysed by sophisticated characterisation techniques such as X-ray diffraction (XRD), N-2 adsorption studies, high resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy and CHN analysis. Structural investigation of the MCN by XRD, HRTEM and N-2 adsorption revealed that the prepared catalyst exhibits highly ordered two-dimensional (2D) porous arrays with a high surface area and a large pore volume. The catalytic results revealed that the MCN was found to be an efficient catalyst in transesterifying long and short chain primary alcohols, and cyclic and aromatic alcohols to afford their corresponding beta-keto esters in high yields. More importantly, the catalyst was highly active when 1-butanol was used. The influence of various parameters such as temperature, reactant feed ratio, catalyst weight, and time-on-stream on the yield of the final product was studied in detail. In addition, the activity of the catalyst was also compared with pure mesoporous carbon and the results were discussed. The recyclability studies revealed that the MCN catalyst was highly stable under the rigorous reaction conditions and can be reused several times without any significant loss of catalytic activity. Crown Copyright (C) 2012 Published by Elsevier B. V. All rights reserved.
引用
收藏
页码:164 / 169
页数:6
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