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吉林化工学院学报, 2023, 40(7): 11-18     https://doi.org/10.16039/j.cnki.cn22-1249.2023.07.003
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催化剂ZrO2/Na-β和ZrO2/H-β的制备及其催化环己酮和异丙醇MPV反应的性能 #br#
董林辉1**,孟凡飞2,宋鹏3,邱俊1*
1.吉林化工学院 化学与制药工程学院, 吉林 吉林 132022; 2.长春理工大学 化学与环境工程学院, 吉林 长春  130012; 3.中国石油抚顺石化石油一厂, 辽宁 抚顺, 113004
Preparation of ZrO2/Na-β and ZrO2/H-β Catalysts and Their Catalytic Performance for the MPV Reaction of Cyclohexanone and Isopropanol
DONG Linhui1 **, MENG Fanfei2, SONG Peng3, QIU Jun1*
1 School of Chemical & Pharmaceutical Engineering, Jilin Institute of Chemical Technology, Jilin City132022, China; 2 School of Materials Science and Engineering, Changchun University of Science and Technology, Changchun 130012, China; 3 PetroChina Fushun Petrochemical Oil Plant, Fushun 113004,China
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摘要 

采用浸渍法制备了具有Na-β和H-β分子筛担载ZrO2的催化剂ZrO2/Na-β和ZrO2/H-β,将其应用于环己酮和异丙醇的MPV还原反应,考察了它们的催化性能。采用XRD、SEM-EDS、NH3-TPD、BET比表面积及孔结构、ICP-MS对催化剂进行了表征,通过气相色谱-质谱联用和气相色谱对产物进行鉴别和含量分析。实验结果表明,对于环己酮和异丙醇的MPV还原反应,与H-β、Na-β、ZrO2/Na-β相比,ZrO2/H-β表现出更高的催化活性。Zr酸中心对环己酮和异丙醇的MPV反应更重要。6%ZrO2/H-β为催化剂,环己酮与异丙醇的摩尔比为1:20,催化剂用量为反应物总质量的6%, 80 ℃下,反应5 h,以环己酮为基准,采用面积归一化计算,环己酮的转化率为91.2%。催化剂经焙烧可以再生,焙烧后的催化剂在使用5次后,环己酮的转化率明显下降为79.4%,而干燥后的催化剂使用1次后就失去部分活性,催化剂的使用寿命有待于进一步深入研究提高。

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董林辉
孟凡飞
宋鹏
邱俊
关键词:  改性β分子筛  催化剂  MPV还原反应  性能     
Abstract: 

ZrO2/Na-β and ZrO2/H-β catalysts which ZrO2 supported on Na-β and H-β molecular sieves were prepared by impregnation method, and applied to the MPV reduction reaction of cyclohexanone and isopropanol to examine their catalytic properties. The catalysts were also characterized by XRD, SEM-EDS, NH3-TPD, BET specific surface area and pore structure, and ICP-MS. The products were identified by gas chromatography-mass spectrometer and analyzed and gas chromatography. The experimental results showed that ZrO2/H-β exhibited higher catalytic activity compared with H-β, Na-β, ZrO2/Na-β for the MPV reduction reaction of cyclohexanone and isopropanol. Due to ZrO2/H-β possesses both Zr and Al acid centers, these promote that the catalytic efficiency of MPV reaction of cyclohexanone and isopropanol was further improved. 6%ZrO2/H-β was used as the catalyst, the molar ratio of cyclohexanone to isopropanol was 1:20, and the dosage of catalyst was 6% of the total mass of the reactants. The reaction was carried out at 80 ℃ for 5 h. Based on cyclohexanone, the Area-normalized calculation, the conversion rate of cyclohexanone was 91.2%. The catalyst can be regenerated by calcination. The conversion rate of cyclohexanone decreases to 79.4% after 5 times of recycle, while the dried catalyst loses part of its activity after 1 time of recycle. The service life of the catalyst needs further study to improve.

Key words:  modified molecular sieve β    catalyst    MPV reduction reaction    catalytic performance
               出版日期:  2023-07-25      发布日期:  2023-07-25      整期出版日期:  2023-07-25
ZTFLH:  O 643.36  
引用本文:    
董林辉, 孟凡飞, 宋鹏, 邱俊.
催化剂ZrO2/Na-β和ZrO2/H-β的制备及其催化环己酮和异丙醇MPV反应的性能 #br#
[J]. 吉林化工学院学报, 2023, 40(7): 11-18.
DONG Linhui , MENG Fanfei, SONG Peng, QIU Jun. Preparation of ZrO2/Na-β and ZrO2/H-β Catalysts and Their Catalytic Performance for the MPV Reaction of Cyclohexanone and Isopropanol . Journal of Jilin Institute of Chemical Technology, 2023, 40(7): 11-18.
链接本文:  
http://xuebao.jlict.edu.cn/CN/10.16039/j.cnki.cn22-1249.2023.07.003  或          http://xuebao.jlict.edu.cn/CN/Y2023/V40/I7/11
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