双胺基双酚铜配合物催化甲苯氧化合成苯甲酸  

Catalytic Oxidation of Toluene to Benzoic Acid over Diamino-Bis(phenolate)Copper Complex

作　　者：胡炜杰 刘泽 黄佳莹 周贤太 陈亚举 陈嘉贤 HU Weijie;LIU Ze;ZHOU Xiantai;HUANG Jiaying;CHEN Yaju;CHEN Jiaxian(School of Chemistry,Guangdong University of Petrochemical Technology,Maoming 525000,China;School of Chemical Engineering and Technology,Sun Yat-sen University,Zhuhai 519082,China;Maoming Green Chemical Research Institute,Maoming 525011,China)

机构地区：[1]广东石油化工学院化学学院,广东茂名525000 [2]中山大学化学工程与技术学院,广东珠海519082 [3]茂名绿色化工研究院,广东茂名525011

出　　处：《广东石油化工学院学报》2023年第4期38-42,共5页Journal of Guangdong University of Petrochemical Technology

基　　金：广东省科技创新战略专项(2021S0007,2021S0008);茂名市科技计划项目(2021014);广东省普通高校青年创新人才类项目(2021KQNCX056);茂名市哲学社会科学规划项目(2022YB01);广东石油化工学院人才引进项目(2019rc047,2019rc049);大学生创新创业训练计划项目(73322080)。

摘　　要：通过将四齿双胺基双酚配体与铜盐发生配位反应制备得到一种结构新颖的双胺基双酚铜配合物。将所得配合物作为均相催化剂应用于氧气存在条件下、以N-羟基邻苯二甲酰亚胺为助催化剂的甲苯氧化合成苯甲酸反应中。结果表明,该催化剂在温和的条件下实现了甲苯分子中C─H键的活化和氧化,且高选择性得到了产物苯甲酸。系统考察了催化剂用量、助催化剂用量、反应温度、氧气压力和反应时间等因素对催化性能的影响。在最佳反应条件下,甲苯转化率为51.8%,苯甲酸选择性可达91.4%。A novel structure of diamino-bis(phenolate)copper complex was prepared based on coordination reaction of a quadridentate diamino-bis(phenolate)ligand with copper salt.The obtained complex compound was then employed as homogeneous catalyst for the synthesis of benzoic acid from toluene in the presence of molecular oxygen by using N-hydroxyphthalimide as a co-catalyst.The results showed that this catalyst achieved the activation and oxidation of C-H bonds in toluene molecules under mild conditions,and the product benzoic acid was obtained with high selectivity.The effects of reaction parameters including catalyst loading,co-catalyst dosage,reaction temperature,O 2 pressure and reaction time on catalytic performance were investigated systematically.Under the optimal reaction conditions,good conversion of toluene(51.8%)and selectivity to benzoic acid(91.4%)were obtained.

关 键 词：C—H键 甲苯氧化 金属配合物 氧气 苯甲酸 

分 类 号：O643.3[理学—物理化学]