文章摘要
TEMPO功能化共轭微孔聚合物催化氧化醇性能
TEMPO radical functionalized conjugated microporous polymers for selective oxidation of alcohols
投稿时间:2019-05-14  修订日期:2019-06-26
DOI:
中文关键词: 共轭微孔聚合物  醇氧化  TEMPO自由基  异相催化  Sonogashira偶联反应
英文关键词: conjugated microporous polymers, alcohol oxidation, TEMPO radicals, heterogeneous catalysis, Sonogashira coupling
基金项目:国家自然科学基金项目(面上项目,重点项目,重大项目)
作者单位E-mail
王晨 贵州师范大学 wangchen941013@163.com 
毛会玲 贵州师范大学  
薛云 贵州师范大学  
晏秘 贵州师范大学  
申妍铭 贵州师范大学  
庄金亮 贵州师范大学 jlzhuang@xmu.edu.cn 
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中文摘要:
      将2,2,6,6-四甲基哌啶氧自由基(TEMPO)嫁接到2,5-二溴苯甲酸侧链,并与1,3,5-三乙炔苯通过Sonogashira偶联反应,合成出TEMPO自由基功能化共轭微孔聚合物CMP-3-TEMPO。利用SEM、XRD、FT-IR和EPR等测试了CMP-3-TEMPO的形貌和结构组成。催化性能测试结果表明:CMP-3-TEMPO在氧气氛围、较温和条件下(80℃,常压),可将各种一级醇、二级醇以及杂原子醇氧化成相应的醛或酮化合物,转化率为70%~100%。CMP-3-TEMPO经过3次循环利用后,催化性能有所降低,可能的原因是反应过程CMP-3-TEMPO存在局部解体,导致催化活性位点降低。
英文摘要:
      By the incorporation of 2,2,6,6-tetramethylpiperidineoxyl (TEMPO) radicals into 2,5-dibromobenoic acid, and further reacted with 1,3,5-triethynylbenzene through Sononashira coupling reaction, a TEMPO radical decorated conjugated microporous polymer (CMP), named CMP-3-TEMPO, was successfully synthesized. The chemical composition and structural information of CMP-3-TEMPO are characterized by SEM, XRD, FT-IR, and EPR spectra. CMP-3-TEMPO enables selective oxide a broad range of primary and secondary aromatic alcohols, and heteroatom aromatic alcohols to their corresponding aldehydes and ketones with conversion at the range of 70-100% under mild aerobic conditions (80?C, normal atmospheres). However, the catalytic activity of CMP-3-TEMPO was significantly decreased after three catalytic cycles. The partial decomposition of CMP-3-TEMPO and the leakage of TEMPO radicals from inner might be responsible for the decreased catalytic activity.
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