Cu/HY催化剂在乙炔氢氯化反应中的性能及其失活原因  

Catalytic Performance and Deactivation of Cu/HY Catalysts for Acetylene Hydrochlorination

作　　者：相博文 王璐[1] 王丰[1] 王吉德[1] XIANG Bowen;WANG Lu;WANG Feng;WANG Jide(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)

机构地区：[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,乌鲁木齐830046

出　　处：《应用化学》2018年第12期1449-1456,共8页Chinese Journal of Applied Chemistry

基　　金：国家自然科学基金(U1403293,21263025);新疆大学博士启动基金(BS160222)项目资助

摘　　要：采用等体积浸渍法制备了以分子筛为载体的铜基无汞催化剂(Cu/HY),在固定床反应器中,考察了Cu/HY催化剂用于乙炔氢氯化反应制取氯乙烯的催化性能,并采用扫描电子显微镜(SEM)、能量散射光谱(EDS)、电感耦合等离子光谱(ICP-AES)、氮气吸脱附(BET)、热重分析(TG)、透射电子显微镜(TEM)、X射线粉末衍射(XRD)和X射线光电子能谱(XPS)表征手段对反应前后的催化剂进行了表征和分析。结果表明,反应温度为160℃,常压,空速为120 h^(-1),V(HCl)/V(C_2H_2)=1.25,Cu的负载质量分数为15%时,Cu/HY催化剂的乙炔氢氯化性能最佳,乙炔转化率可达84%,氯乙烯选择性始终大于95%,且具有较好的稳定性;通过表征分析,认为催化剂表面形成积碳,铜活性物种的还原、团聚和流失是导致Cu/HY催化剂活性下降的主要原因。Zeolite supported Cu-based mercury-free catalysts （Cu/HY） were prepared by incipient-wetness impregnation, and their catalytic performance for acetylene hydrochlorination was evaluated in a fixed reactor. The structure parameters and theory properties of the fresh and used catalysts were characterized by scanning electron microscopy （SEM） , energy dispersive spectroscopy （EDS） , inductively coupled plasma-atomic emission spectroscopy（ICP-AES）, N 2 adsorption and desorption isotherms（BET）, thermogravimetry （TG） , transmission electron microscopy（TEM）, X-ray powder diffraction （XRD） and X-ray photoelectron spectroscopy （XPS）. The acetylene conversion reached 84%, the selectivity for vinyl chloride was more than 95% and a better stability was observed on Cu/HY mercury-free catalysts with 15% （mass fraction） Cu loading , under the reaction conditions of 160 ℃, 101.325 kPa, a total gas hourly space of 120 h^-1 , V （HCl）/ V （C2H2 ）= 1.25. Besides, the characterization results show that the generation of carbon deposition , the reduction, agglomeration and loss of Cu active components are the main reasons for the decrease of the catalyst activity.

关 键 词：催化剂 分子筛 乙炔氢氯化 催化 氯乙烯 

分 类 号：O643[理学—物理化学]