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连接链长度对交联聚苯乙烯固定N-羟基邻苯二甲酰亚胺催化环己基苯氧化的影响
引用本文:孙婷婷,单玉华,王继元,陈韶辉,黄超. 连接链长度对交联聚苯乙烯固定N-羟基邻苯二甲酰亚胺催化环己基苯氧化的影响[J]. 石油学报(石油加工), 2020, 36(2): 244-252. DOI: 10.3969/j.issn.1001-8719.2020.02.004
作者姓名:孙婷婷  单玉华  王继元  陈韶辉  黄超
作者单位:1. 常州大学 江苏省先进催化与绿色制造协同创新中心,江苏 常州 213164; 2. 中国石化 扬子石化有限公司南京研究院,江苏 南京 210048
基金项目:江苏省绿色催化材料与技术重点实验室项目(BM2012110)和江苏省科技厅前瞻性研究项目(BY2014037-12)资助
摘    要:为解决N-羟基邻苯二甲酰亚胺(NHPI)催化剂难以回收利用的问题,采用不同链长的卤代烃,通过烷基化反应,将NHPI化学固定于交联聚苯乙烯(CPS)微球,制得了具有不同长度连接链的CPS-NHPI-Cn非均相催化剂。采用X射线光电子能谱(XPS)、红外光谱(FT-IR)、N2吸附-脱附(BET)、扫描电子显微镜(SEM)等分析手段进行表征。将所制备的CPS-NHPI-Cn用于催化环己基苯(CHB)氧化过程,考察了连接链长度(C1~C9)及反应条件对催化性能的影响。结果表明:连接链长度明显影响CPS-NHPI-Cn的催化性能,连接链长从度C1增至C6,CPS-NHPI-Cn催化剂的活性增加。以CPS-NHP-C6为催化剂,在95 ℃、1 MPaO2分压下反应8h,环己基苯的转化率为28.4%,环己酮和苯酚的选择性分别为90.7%和87.6%。CPS-NHP-C6循环使用10次,其催化性能没有明显下降。

关 键 词:交联聚苯乙烯微球(CPS)  固定N-羟基邻苯二甲酰亚胺(NHPI)  连接链长度;环己基苯;催化氧化  
收稿时间:2019-01-28

Effects of Link Chain Length on Oxidation of Cyclohexylbenzene Catalyzed by immobilized N-Hydroxyphthalimide on Cross-linked Polystyrene
SUN Tingting,SHAN Yuhua,WANG Jiyuan,CHEN Shaohui,HUANG Chao. Effects of Link Chain Length on Oxidation of Cyclohexylbenzene Catalyzed by immobilized N-Hydroxyphthalimide on Cross-linked Polystyrene[J]. Acta Petrolei Sinica (Petroleum Processing Section), 2020, 36(2): 244-252. DOI: 10.3969/j.issn.1001-8719.2020.02.004
Authors:SUN Tingting  SHAN Yuhua  WANG Jiyuan  CHEN Shaohui  HUANG Chao
Affiliation:1. Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, Changzhou University, Changzhou 213164, China; 2. Nanjing Research Institute, SINOPEC Yangzi Petrochemical Co. Ltd., Nanjing 210048, China
Abstract:To solve the drawbacks of difficult recovery and reuse of N-hydroxyphthalmide (NHPI), the cross-linked polystyrene (CPS) immobilized NHPI (CPS-NHPI-Cn) catalysts with different link chain lengths were prepared by chemical immobilization of NHPI on the surface of CPS microsphere using different chain lengths of halogenated hydrocarbons as alkylation agents. The synthesized CPS-NHPI-Cn catalysts were characterized by XPS, FT-IR, BET and SEM, and evaluated by cyclohexylbenzene oxidation. The effects of link chain length (C1-C9) in CPS-NHPI-Cn and reaction conditions on the catalytic performance were investigated. Results indicate that the link chain length affects the catalytic performance of CPS-NHPI-Cn obviously, and the catalytic activity increases with the link chain number from 1 to 6. Using CPS-NHPI-C6 as catalyst, at 95 ℃ and 1 MPaO2 partial pressure for 8 h, the cyclohexylbenzene conversion is 28.4%, with the selectivity of cyclohexanone and phenol is 90.7% and 87.6%, respectively. After the CPS-NHPI-C6 catalyst has been reused for 10 times, the catalytic performance is still as high as that of fresh one.
Keywords:cross-linked polystyrene microsphere(CPS)  immobilization N-hydroxyphthalimide(NHPI)  link chain length  cyclohexylbenzene  catalytic oxidation  
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