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水杨醛席夫碱金属配合物对模型硫化物的催化氧化性能研究
作者姓名:Jia Chaoyang  Liang Shuyuan  Liu Lei  Shao Xue  Zhang Longli  Wang Fangzhu  Jiang Cuiyu
作者单位:1. 中国石油大学(华东)化工学院 2. 中国石油大学(华东)理学院
基金项目:This work was supported by the National Natural Science Foundation of China(No.21576292).
摘    要:Seven kinds of Schiff base metal complexes(C1-C7)were synthesized by the reaction of substituted salicylaldehyde Schiff base with cobalt nitrate,nickel nitrate,and copper nitrate,respectively.The oxygen carrying performance,and the catalytic property of complexes for the oxidation of model sulfides 1-hexanethiol,dibutyl sulfide,and 2-methylthiophene along with their influencing factors were explored,while the oxidized products of the model sulfides were also analyzed and characterized.The results show that the catalytic oxidation property of the complexes is determined by their oxygen carrying performance and solubility in n-octane.The oxygen carrying performance of the complexes is mainly affected by the central ion species,the electronic effects,and the spatial effects of the substituents as well as the degree of conjugation.More specifically,the oxygen carrying performance can be improved by enhancing the oxygenation capacity of the central metal ions,increasing the electron donating ability of the ligand substituent,and diminishing the steric hindrance as well as extending the conjugated chain.Complexes C7 were found to be with high oxygen carrying capacity and high solubility in n-octane,which shows the best catalytic oxidation property,and the oxidation conversion rates for 1-hexylthiol,dibutyl sulfide,and 2-methylthiophene are 74.2%,65.1%,and 22.7%,respectively.Upon using the oxidation catalyst of Schiff base metal complexes,three sulfides can be oxidized by oxygen to form sulfones and sulfoxides.1-Hexanethiol and dibutyl sulfide will continue to be oxidized to form sulfates and sulfites.

关 键 词:Schiff  base  metal  complexes  1-hexanethiol  dibutyl  sulfide  2-methylthiophene  catalytic  oxidation  structureactivity  relationship
收稿时间:2020-05-27
修稿时间:2020-07-13

Study of the Property of Salicylaldehyde Schif Base Metal Complexes for Catalytic Oxidation of Model Sulfdes
Jia Chaoyang,Liang Shuyuan,Liu Lei,Shao Xue,Zhang Longli,Wang Fangzhu,Jiang Cuiyu.Study of the Property of Salicylaldehyde Schif Base Metal Complexes for Catalytic Oxidation of Model Sulfdes[J].China Petroleum Processing and Petrochemical Technology,2021,23(1):58-66.
Affiliation:1. College of Chemical Engineering, China University of Petroleum, Qingdao 266580; 2. College of Science, China University of Petroleum, Qingdao 266580;
Abstract:Seven kinds of Schiff base metal complexes (C1—C7) were synthesized by the reaction of substituted salicylaldehyde Schiff base with cobalt nitrate, nickel nitrate, and copper nitrate, respectively. The oxygen carrying performance, and the catalytic property of complexes for the oxidation of model sulfdes 1-hexanethiol, dibutyl sulfde, and 2-methylthiophene along with their infuencing factors were explored, while the oxidized products of the model sulfdes were also analyzed and characterized. The results show that the catalytic oxidation property of the complexes is determined by their oxygen carrying performance and solubility in n-octane. The oxygen carrying performance of the complexes is mainly afected by the central ion species, the electronic efects, and the spatial efects of the substituents as well as the degree of conjugation. More specifcally, the oxygen carrying performance can be improved by enhancing the oxygenation capacity of the central metal ions, increasing the electron donating ability of the ligand substituent, and diminishing the steric hindrance as well as extending the conjugated chain. Complexes C7 were found to be with high oxygen carrying capacity and high solubility in n-octane, which shows the best catalytic oxidation property, and the oxidation conversion rates for 1-hexylthiol, dibutyl sulfde, and 2-methylthiophene are 74.2%, 65.1%, and 22.7%, respectively. Upon using the oxidation catalyst of Schif base metal complexes, three sulfdes can be oxidized by oxygen to form sulfones and sulfoxides. 1-Hexanethiol and dibutyl sulfde will continue to be oxidized to form sulfates and sulftes.
Keywords:Schiff base metal complexes  1-hexanethiol  dibutyl sulfide  2-methylthiophene  catalytic oxidation  structure-activity relationship  
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