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取代水杨醛席夫碱金属配合物结构对硫化物催化氧化性能的影响

Effect of Substituted Salicylaldehyde Schiff Base Metal Complex Structure on Catalytic Oxidation Property of Sulfide
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摘要 将取代水杨醛席夫碱分别与Co(NO3)2、Ni(NO3)2反应合成了7种席夫碱金属配合物(C1~C7),并考察了其载氧性能,对模型硫化物1-己硫醇、二丁基硫醚、2-甲基噻吩的催化氧化性能及其影响因素。结果表明:配合物的载氧性能主要受其中心离子种类、配体取代基电子效应和空间效应及共轭程度的影响;中心离子与O2的配位能力越强、配体取代基推电子能力越大且空间位阻越小、共轭链越长越有利于配合物载氧,其中每摩尔C7配合物的载氧量为0.523 mol;配合物的催化氧化性能由其载氧性能和在正辛烷中的溶解度共同决定,载氧量越高、溶解度越大,则对硫化物的催化氧化性能越好;配合物C6的催化氧化性能最佳,且对1-己硫醇和二丁基硫醚的催化氧化性能优于对2-甲基噻吩。 The oxygen carrying properties of seven Schiff base metal complexes(C1-C7)synthesized by the reaction of substituted salicylaldehyde Schiff base with cobalt nitrate and nickel nitrate,and the catalytic oxidation properties of the model sulfides 1-hexanethiol,dibutyl sulfide and 2-methylthiophene were studied.Results show that the oxygen carrying properties of the complexes are mainly affected by many factors,such as the central ion species,the electronic effects of the substituents,the spatial effects and the degree of conjugation.The stronger coordination ability between the central ion and the oxygen molecule,the greater the electron-donating ability of the ligand substituent,the smaller the steric hindrance,and the longer the conjugated chain,the more favorable the oxygen carring property becomes.Among seven complexes,the molar oxygen carrying property of C7 is 0.523 mol.The catalytic oxidation performance is determined by the oxygen carrying properties of the complexes and the solubility in n-octane.In terms of complexes,the higher the oxygen carrying properties and the higher the solubility,the better the desulfurization performance.C6 has the highest catalytic oxidation performance,and the catalytic oxidation properties of complexes in 1-hexanethiol and dibutyl sulfide are better than 2-methylthiophene.
作者 姜翠玉 梁书源 贾超洋 刘蕾 邵雪 张龙力 JIANG Cuiyu;LIANG Shuyuan;JIA Chaoyang;LIU Lei;SHAO Xue;ZHANG Longli(College of Science, China University of Petroleum, Qingdao 266580, China;College of Chemical Engineering, China University of Petroleum, Qingdao 266580, China)
出处 《石油学报(石油加工)》 EI CAS CSCD 北大核心 2020年第3期476-483,共8页 Acta Petrolei Sinica(Petroleum Processing Section)
基金 国家自然科学基金项目(21576292)资助。
关键词 席夫碱金属配合物 取代水杨醛 载氧性能 催化氧化性能 构效关系 Schiff base metal complexes substituted salicylaldehyde oxygen carrying property catalytic oxidation property structure-activity relationship
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