Self-assembled metalloporphyrins-inorganic hybrid flowers and their application to efficient epoxidation of olefins

Self-assembled metalloporphyrins-inorganic hybrid flowers and their application to efficient epoxidation of olefins
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自组装金属卟啉-无机杂化花及其在烯烃高效环氧化中的应用

DOI:
10.1002/jctb.5275
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发表时间:
2017-10-01
影响因子:
3.4
通讯作者:
Ji, Hongbing
Ji, Hongbing
中科院分区:
工程技术4区
文献类型:
--
作者:
He, Xiaohui;Chen, Long;Ji, Hongbing

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背景利用多种蛋白质或酶作为有机组分形成杂交花,它们表现出优异的催化、吸附和传感性能。然而,目前还没有基于金属卟啉的杂交花卉的报道。基于金属卟啉在催化反应中的重要性,制备了金属卟啉-磷酸铜杂化花,并对其在环氧化反应中的催化性能进行了评价.结果表明,杂化花的组成、形态和微晶结构强烈地依赖于孵育时间(0.1- 72 h)和母液中金属卟啉的浓度(0-47 μ g mL(-1))。与游离金属卟啉相比,杂交花表现出增强的稳定性,而没有任何降低的催化活性。活性与金属卟啉表面含量呈线性相关,表明表面金属卟啉是催化剂的关键活性物种。此外,杂交花表现出良好的兼容性与广泛的溶剂和substrate. CONCLUSION杂交花的形成机制,提出了涉及四个主要的连续步骤:协调,成核,形成,和增长。研究结果表明,以金属卟啉为有机组分的纳米杂化材料具有良好的催化性能,有望在工业催化领域得到应用。(c)2017年化学工业协会
BACKGROUNDVarious proteins or enzymes were employed as organic components to form hybrid flowers, and they exhibited excellent properties in catalysis, adsorption, and sensing. However, there is no previous report of metalloporphyrins-based hybrid flowers. Based on the importance of metalloporphyrins in catalytic reactions, metalloporphyrins-copper phosphate hybrid flowers were prepared and their catalytic performance in epoxidation reactions was evaluated.RESULTSThe composition, morphology, and crystallite structure of the hybrid flowers strongly depended on the incubation time (0.1-72h) and concentration of metalloporphyrins in the mother liquor (0-47 mu g mL(-1)). In comparison with the free metalloporphyrins, the hybrid flowers exhibited enhanced stability without any decrease in the catalytic activity. Moreover, the activity was linearly correlated with the surface content of metalloporphyrins which indicated that the metalloporphyrins on the surface were the key active species. Furthermore, the hybrid flowers showed good compatibility with a wide range of solvents and substrates.CONCLUSIONThe mechanism of formation of the hybrid flowers was proposed that involves four major successive steps: coordination, nucleation, formation, and growth. The catalytic results suggest that well-designed hybrid materials with hierarchical nano-structures and metalloporphyrins as organic component would be potential candidates for industrial catalysis applications. (c) 2017 Society of Chemical Industry