Immobilization of manganese tetraphenylporphyrin on boehmite and its catalysis for aerobic oxidation of cyclohexane
Immobilization of manganese tetraphenylporphyrin on boehmite and its catalysis for aerobic oxidation of cyclohexane
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DOI：
10.1016/j.apcata.2009.02.011
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发表时间：
2009-05
影响因子：
5.5
通讯作者：
Guan Huang;Shang-Yue Liu;Yong-An Guo;Aiqing Wang;Jin Luo;Chun-Cai Cai-Chun-Cai-Cai-2075301405
中科院分区：
文献类型：
--
作者：
Guan Huang;Shang-Yue Liu;Yong-An Guo;Aiqing Wang;Jin Luo;Chun-Cai Cai-Chun-Cai-Cai-2075301405
寻找可重复使用的材料作为烃氧化的高效且经济的催化剂是一个重要的研究领域。在这项研究中，我们研究了吸附在新鲜沉淀的氢氧化铝前体上的四苯基卟啉锰提供的载体和金属卟啉的高效组合，然后转化为锰卟啉/勃姆石化合物。使用 FT-IR、紫外-可见光谱技术、N2BET 分析、X 射线粉末衍射、透射电子显微技术和热分析对其进行了表征。在温和条件下、不存在任何溶剂和还原剂的情况下，使用该化合物作为催化剂，研究了环己烷的有氧氧化。结果表明，它比四苯基锰卟啉和相应的壳聚糖负载催化剂具有更高的催化活性。特别是，该催化剂对于环己烷氧化表现出良好的原子经济性、高的催化剂周转数以及良好的酮和醇选择性。特别是具有优异的重复使用性，不改变原有的催化活性；仅含1mg Mn TPP的催化剂在Beomite（BM）的促进下可重复使用8次。此外，我们还研究了使用这种纳米颗粒负载的四苯基卟啉锰作为温和且环境友好的氧化催化剂的反应条件。
The search for a reusable material as an efficient and economic catalyst for hydrocarbon oxidation is an important field of research. In this study, we investigated the highly effective combination of support and metalloporphyrin provided by manganese tetraphenylporphyrin adsorbed onto a precursor of freshly precipitated aluminium hydroxide, followed by conversion to a manganese porphyrin/boehmite compound. This was characterized using FT-IR, UV–vis spectroscopic techniques, N2BET analysis, X-ray powder diffraction, transmission electron micrograph technique and thermal analysis. Aerobic oxidation of cyclohexane has been investigated using the compound as a catalyst under mild conditions and in the absence of any solvent and reductant. The results indicate that it has higher catalytic activity than manganese tetraphenylporphyrin and the corresponding chitosan-supported catalyst. In particular, the catalyst exhibits good atom economy for cyclohexane oxidation, high catalyst turnover number, and good ketone and alcohol selectivity. In particular, it has excellent reusability, with no change in original catalytic activity; a quantity of catalyst containing only 1mg of Mn TPP can be reused 8 times under the promotion of beomite (BM). In addition, we examined the reaction conditions for the use of such nanoparticle-supported manganese tetraphenylporphyrin as a mild and environmental friendly oxidation catalyst.