Silica-metalloporphyrins hybrid materials: preparation and catalysis to hydroxylate cyclohexane with molecular oxygen

Silica-metalloporphyrins hybrid materials: preparation and catalysis to hydroxylate cyclohexane with molecular oxygen
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二氧化硅-金属卟啉杂化材料的制备及催化环己烷分子氧羟基化

DOI:
10.1007/s10971-009-1961-y
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发表时间:
2009-06-01
影响因子:
2.5
通讯作者:
Ji, Liang-Nian
Ji, Liang-Nian
中科院分区:
材料科学3区
文献类型:
--
作者:
Cai, Jin-Hua;Huang, Jin-Wang;Ji, Liang-Nian

文献摘要

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以5-(4-烯丙氧基)苯基-10,15,20-三(4-氯苯基)卟啉(APTCPP)和3-巯丙基三甲氧基硅烷(MPS)为原料,采用溶胶-凝胶法在室温下通过硫醇烯聚合反应制备了Si-S-APTCPPFe、Si-S-APTCPPMn和Si-S-APTCPPCo三种新型硅基金属卟啉杂化材料。采用XRD、SEM、FT-IR、UV-Vis和TG等手段对杂化材料进行了表征,并将其作为环己烷有氧氧化催化剂进行了考察。结果表明,在金属卟啉-O-2-抗坏血酸盐体系中,这些杂化材料比类似的非负载金属卟啉具有更高的催化活性,且金属离子对杂化材料的催化活性有显著影响.
Three types of novel silica-metalloporphyrins hybrid materials, Si-S-APTCPPFe, Si-S-APTCPPMn and Si-S-APTCPPCo, were prepared at room temperature by sol-gel method involving a thiol-ene polymerization reaction of 5-(4-allyloxy)phenyl-10,15,20-tri(4-chlorophenyl)porphyrin (APTCPP) with 3-mercaptopropyltrimethoxysilane (MPS). The hybrid materials were characterized by XRD, SEM, FT-IR, UV-Vis and TG, and were investigated as catalysts for the aerobic oxidation of cyclohexane. It is found that these hybrid materials are more efficient catalysts than the analogous non-supported metalloporphyrins for cyclohexane hydroxylation in metalloporphyrin-O-2-ascrobate system and the metal ion in the porphyrins significantly affected the catalytic efficiencies of these hybrid materials.