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磷改性Cu/USY催化剂的制备及其乙炔氢氯化催化性能
1.新疆大学化学化工学院,石油天然气精细化工教育部和新疆维吾尔自治区重点实验室,新疆 乌鲁木齐 830046; 2.新疆德安环保科技股份有限公司,新疆 乌鲁木齐 830026
Preparation of P-Modified Cu/USY Catalyst and Its Catalytic Performance for Acetylene Hydrochlorination
1. Key Laboratory of Oil and Gas Fine Chemicals of Education and Xinjiang Uyghur Autonomous Region, College of Chemistry and Chemical Engineering, Xinjiang University, Urumqi 830046, China; 2. Xinjiang De’an Environmental Protection Technology Co Ltd, Urumqi 830026, China
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摘要 以USY分子筛为载体,CuCl2为活性组分,采用超声辅助-浸渍法制备了一系列磷(以H3PO4为磷源)改性的Cu/USY催化剂,在固定床反应器上考察了其乙炔氢氯化催化性能。结果表明:在总空速为119 h-1、HCl和C2H2体积比为1.29和反应温度为160 ℃的条件下,P-Cu/USY具有较高的催化活性,当P的质量分数为2 %时,催化剂初始活性可达98.68%,反应9 h后,仍可保持57.86%。基于催化剂的扫描电子显微镜(SEM)、比表面积测试(BET)、热重分析(TG)、X射线衍射(XRD)、表面元素分析(EDS)和X射线光电子能谱(XPS)表征,可以推断适宜的P改性可有效抑制催化剂表面积炭的生成,减少Cu活性组分的流失和还原,从而改善Cu/USY催化剂的初始活性,为用于乙炔氢氯化反应的分子筛无汞催化剂的研究提供了一种新思路。
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王 璐1
闫海军1
廉立臻1
王 丰1
王吉德1
马莉达2
张琳琳2
关键词 磷改性分子筛催化剂乙炔氢氯化    
Abstract:A series of P (H3PO4 as phosphate source) modified Cu/USY catalysts were prepared by ultrasonic-assisted impregnation method using USY molecular sieve as catalyst support and CuCl2 as active component precursor, respectively. The catalytic performances for acetylene hydrochlorination were investigated in a fixed-bed reactor. The results suggested that P-Cu/USY catalyst had a better catalytic performance at a total gas hourly space of 119 h-1, volume ratio of HCl to C2H2 of 1.29 and temperature 160 ℃. When the mass fraction of phosphate was 2 %, the initial activity of the catalyst could reach above 98.68 % and it could still maintain 57.86% even after 9 h reaction. The catalysts were characterized by the techniques of scanning electron microscopy (SEM), specific surface area test (BET), thermogravimetric analysis (TG), X-ray diffraction (XRD), surface elemental analysis (EDS) and X-ray photoelectron spectroscopy (XPS). It was speculated that the presence of phosphate species was favorable to the inhibition of the carbon deposition, the Cu loss and the reduction of Cu2+ active component on the catalyst surface, hence enhancing the initial activity of Cu/USY catalysts. All the findings provided a new idea for the study of mercury-free zeolites catalysts for acetylene hydrochlorination.
Key wordsP modification    Cu    molecular sieve    catalyst    acetylene hydrochlorination   
收稿日期: 2018-04-02     
基金资助:新疆自治区自然科学基金面上项目(2017D01C034)。
作者简介: 王 璐(1989—),女,博士,副教授。E-mail: wanglu_4951@163.com。
引用本文:   
王 璐1,闫海军1,廉立臻1等. 磷改性Cu/USY催化剂的制备及其乙炔氢氯化催化性能[J]. 化学反应工程与工艺, 2018, 34(3): 254-260.
Wang Lu1,Yan Haijun1,Lian Lizhen1 et al. Preparation of P-Modified Cu/USY Catalyst and Its Catalytic Performance for Acetylene Hydrochlorination[J]. 化学反应工程与工艺, 2018, 34(3): 254-260.
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