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V-Ce复合氧化物催化间二甲苯气相氨氧化制间苯二甲腈
1. 华东理工大学化工学院,上海 200237; 2. 中国石油化工股份有限公司上海石油化工研究院,绿色化工与工业催化国家重点实验室,上海 201208
Gas Phase Ammoxidation of meta-Xylene to Isophthalonitrile over V-Ce Composite Oxides
1. School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China; 2. State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Shanghai Research Institute of Petrochemical Technology, SINOPEC, Shanghai 201208, China
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摘要 采用喷雾干燥成型的方法,制备了不同Ce/V比的无Cr环境友好型V-Ce复合氧化物催化剂,在流化床反应器中考察了Ce/V比及Mo助剂对催化剂反应性能的影响,并通过X射线衍射(XRD)、拉曼光谱、氢气程序升温还原(H2-TPR)、NH3程序升温脱附(NH3-TPD)和X射线光电子能谱(XPS)等方法对催化剂进行了表征。结果表明,CeVO4晶相对于提高间苯二甲腈(IPN)收率具有关键作用,随着Ce/V比的提高,逐渐出现CeO2晶相,主产物IPN选择性下降。V-Ce复合氧化物催化剂表面以弱酸为主。V1Ce0.8/SiO2表现出较优的催化性能,其IPN收率为60.0%。进一步添加助剂Mo,可显著降低深度氧化产物COx选择性,当Mo/V比为0.10时,催化剂的IPN收率可提高至62.5%。
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习鹏博1
2
冯 冰2
顾龙勤2
杨为民1
2
关键词 流化床气相氨氧化V-Ce催化剂间苯二甲腈    
Abstract:Environmental friendly and Cr-free composite oxide catalysts with different Ce/V ratios were prepared through spray drying method. The effect of Ce/V ratio and the addition of Mo on the ammoxidation performance of the catalysts were investigated in a fluid bed reactor. The structure of the catalysts was characterized by X-ray diffraction (XRD), Raman spectra, H2 temperature programmed reduction (H2-TPR), NH3 temperature programmed desorption (NH3-TPD) and X-ray photoelectron spectroscopy (XPS). The characterization results showed that the catalysts consisting of CeVO4 crystal phase played a key role in improving the yield of isophtalonitrile (IPN). With the increase of Ce/V ratio, the CeO2 crystal phase appeared gradually, and the selectivity of the main product IPN decreased. The surface acid site of the V-Ce composite oxide catalysts was mainly weak site. The V1Ce0.8/SiO2 sample exhibited the best catalytic performance among the four catalysts with different Ce/V ratios, with IPN yield of 60.0%. Moreover, the addition of Mo promoter into the V1Ce0.8/SiO2 sample could suppress the COx formation and further improve the gas-phase ammoxidation performance. The IPN yield could reach 62.5% when the Mo/V ratio was 0.10.
Key words fluidized bed    gas phase ammoxidation    V-Ce catalyst    isophthalonitrile   
收稿日期: 2020-04-28     
作者简介: 习鹏博(1996—),男,硕士研究生;杨为民(1966—),男,教授级高级工程师,通讯联系人。E-mail: yangwm.sshy@sinopec.com。
引用本文:   
习鹏博1,2,冯 冰2等. V-Ce复合氧化物催化间二甲苯气相氨氧化制间苯二甲腈[J]. 化学反应工程与工艺, 2020, 36(3): 222-229.
XI Pengbo1,2,FENG Bing2 et al. Gas Phase Ammoxidation of meta-Xylene to Isophthalonitrile over V-Ce Composite Oxides[J]. 化学反应工程与工艺, 2020, 36(3): 222-229.
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