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用于乙炔氢氯化反应的高效碳载金离子液体催化剂。

Highly effective carbon-supported gold-ionic liquid catalyst for acetylene hydrochlorination.

作者信息

Qi Xueyan, Chen Weifeng, Zhang Jinli

机构信息

College of Materials Science and Engineering, Hebei University of Engineering Handan 056038 Hebei PR China

School of Chemical Engineering and Technology, Tianjin University Tianjin 300072 PR China

出版信息

RSC Adv. 2019 Jul 15;9(38):21931-21938. doi: 10.1039/c9ra04082j. eCollection 2019 Jul 11.

DOI:10.1039/c9ra04082j
PMID:35518844
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9066470/
Abstract

The sulfur-containing ionic liquid (IL) trimethylsulfonium iodide (CHSI) was used to synthesize an efficient non-mercuric catalyst with HAuCl·4HO as a precursor and spherical active carbon (SAC) as a support. Various Au-IL/SAC catalysts were synthesized using the incipient wetness impregnation technique and applied to acetylene hydrochlorination. The 0.3% Au-IL/SAC catalyst showed the best catalytic performance, with an acetylene conversion of 90% at a temperature of 170 °C and gas hourly space velocity (GHSV) of 360 h using water as the solvent. The catalyst also displayed excellent long-term stability: CH conversion was maintained at 97% for up to 200 h ( = 170 °C, GHSV = 90 h). Brunauer-Emmett-Teller surface area, thermogravimetric analysis, temperature programmed desorption, X-ray diffraction, transmission electron microscopy, and X-ray photoelectron spectroscopy results together showed that the CHSI additive significantly improved the dispersion of Au species and inhibited coke deposition on the catalyst surface during the acetylene hydrochlorination reaction. The superior activity and stability of the Au-IL/SAC catalyst make it a green catalyst for the industrial application of acetylene hydrochlorination.

摘要

以含硫离子液体(IL)碘化三甲基锍(CHSI)为原料,以HAuCl·4HO为前驱体、球形活性炭(SAC)为载体,合成了一种高效的无汞催化剂。采用初湿浸渍法合成了各种Au-IL/SAC催化剂,并将其应用于乙炔氢氯化反应。0.3%Au-IL/SAC催化剂表现出最佳的催化性能,在170℃、气时空速(GHSV)为360 h、以水为溶剂的条件下,乙炔转化率为90%。该催化剂还表现出优异的长期稳定性:在170℃、GHSV = 90 h的条件下,CH转化率在长达200 h内保持在97%。布鲁诺尔-埃米特-泰勒比表面积、热重分析、程序升温脱附、X射线衍射、透射电子显微镜和X射线光电子能谱结果共同表明,CHSI添加剂显著改善了Au物种的分散性,并在乙炔氢氯化反应过程中抑制了催化剂表面的积炭。Au-IL/SAC催化剂优异的活性和稳定性使其成为乙炔氢氯化工业应用的绿色催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6313/9066470/dd918b25fbff/c9ra04082j-f8.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6313/9066470/dd918b25fbff/c9ra04082j-f8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6313/9066470/fa35c16959b6/c9ra04082j-f1.jpg
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本文引用的文献

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Chem Commun (Camb). 2017 Aug 22;53(86):11733-11746. doi: 10.1039/c7cc05986h.
2
Discovery, Development, and Commercialization of Gold Catalysts for Acetylene Hydrochlorination.乙炔氯化用金催化剂的发现、开发和商业化。
J Am Chem Soc. 2015 Nov 25;137(46):14548-57. doi: 10.1021/jacs.5b07752. Epub 2015 Nov 12.
3
Silicon carbide-derived carbon nanocomposite as a substitute for mercury in the catalytic hydrochlorination of acetylene.
碳化硅衍生碳纳米复合材料在乙炔催化氯化反应中替代汞。
Nat Commun. 2014 Apr 22;5:3688. doi: 10.1038/ncomms4688.
4
The catalytic pathways of hydrohalogenation over metal-free nitrogen-doped carbon nanotubes.金属自由氮掺杂碳纳米管上的卤化氢催化途径。
ChemSusChem. 2014 Mar;7(3):723-8. doi: 10.1002/cssc.201300793. Epub 2014 Jan 23.