史秀锋,胡晓虹,范彬彬,李瑞丰.钒席夫碱官能化PMOs的制备及在环己烷氧化中的点击催化作用[J].分子催化,2015,(2):126-134
钒席夫碱官能化PMOs的制备及在环己烷氧化中的点击催化作用
Preparation and Cyclohexane Oxidation Click Catalysis of Periodic Mesoporous Organosilicas Functionalized with V-Schiff-base
投稿时间:2015-03-05  修订日期:2015-03-23
DOI:
中文关键词:  PMOs  氯甲基化  钒席夫碱  环己烷氧化
英文关键词:PMOs  chloromethylation  vanadium-schiff-base  cyclohexane oxidation
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
史秀锋 太原理工大学 shixiufeng@tyut.edu.cn 
胡晓虹 太原理工大学 hujie168@qq.com 
范彬彬* 太原理工大学 fanbinbin@tyut.edu.cn 
李瑞丰 太原理工大学 rfli@tyut.edu.cn 
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中文摘要:
      以周期性介孔有机硅(periodic mesoporous organosilicas, PMOs)中的有机桥联基团亚苯基为反应位对其进行氯甲基化反应,得到氯甲基官能化的PMOs-CH2Cl,然后再通过-CH2Cl和V-Saldien配合物中的-NH-进行反应得到钒席夫碱配合物官能化的杂化材料V-PMOs催化剂。采用XRD、N2吸附、FTIR、UV-vis、ICP和催化反应等手段对所制杂化材料的物化和催化性能进行了较为详细的研究,结果表明采用该法可将钒席夫碱配合物成功键联到PMOs上,且所制杂化材料同采用类似方法制备的V-SBA-15催化材料相对比,在无溶剂以叔丁基过氧化氢为引发剂,氧气为氧化剂的环己烷氧化反应中表现出定向转化为环己酮和环己醇的总选择性,具有点击反应的特性。
英文摘要:
      PMOs-CH2Cl was synthesized by chloromethylation of phenylene moieties in the framework of periodic mesoporous organosilicas (PMOs). Then V-PMOs catalysts were obtained by grafting vanadium-Saldien on PMOs-CH2Cl. The physicochemical properties and catalytic performance of the samples were characterized by XRD, N2 adsorption, FTIR, UV-vis, ICP and cyclohexane oxidation reaction. The results showed that vanadium-Saldien complexes can be successfully immobilized on the PMOs by that route. For comparison, vanadium-Saldien complexes functionalized SBA-15 (V-SBA-15) was prepared by the similar method. In the solvent-free aerobic cyclohexane oxidation reaction system, V-PMOs showed the total selectivity to cyclohexanone and cyclohexanol with the characteristic of click reaction.
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