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Oxyfunctionalization of Alkanes Based on a Tricobalt(II)-Substituted Dawson-Type Rhenium Carbonyl Derivative as Catalyst.
Inorganic Chemistry ( IF 4.6 ) Pub Date : 2020-06-17 , DOI: 10.1021/acs.inorgchem.0c00111
Xinyi Ma 1 , Ping Wang 1 , Zhihao Liu 1 , Changhui Xin 1 , Siyu Wang 1 , Jiage Jia 1 , Pengtao Ma 1 , Jingyang Niu 1 , Jingping Wang 1
Affiliation  

POM-supported metal carbonyl derivatives (PMCDs) represent a family of tremendous potential catalysts owing to their peculiar physical and chemical properties. Yet low-valence transition metal-substituted Dawson-type PMCD catalysts are uncommon. Hence, we synthesized a tricobalt-substituted PMCDs by conventional aqueous solution method, [Na(H2O)5](NH4)7[P2W15O56Co3(H2O)3(OH)3Re(CO)3]·13H2O (1), and characterized by single crystal X-ray diffraction crystallography, IR, and thermogravimetric analyses (TGA), etc. The obtained compound 1 was employed as a catalyst for the oxidation of diphenylmethane (DPM) to benzophenone, giving 96.8% yield in the presence of tert-butyl hydroperoxide (TBHP) and pyridine. The control experiments indicate that Co metal ion plays an important role in the catalytic reactions. As a side note, the electrospray ionization mass spectrometry (ESI-MS) and UV spectroscopy showed that 1 can retain its integrity in solution, and magnetic measurements indicated that 1 exhibited a weaker ferromagnetic interaction at low temperature.

中文翻译:

基于三钴(II)取代的道森型R羰基衍生物作为催化剂的烷烃的氧化官能化。

POM负载的金属羰基衍生物(PMCD)由于其独特的物理和化学性质而代表了一系列巨大的潜在催化剂。低价过渡金属取代的道森型PMCD催化剂并不常见。因此,我们通过常规水溶液法[Na(H 2 O)5 ](NH 47 [P 2 W 15 O 56 Co 3(H 2 O)3(OH)3 Re( CO)3 ]·13H 2 O(1),并通过单晶X射线衍射晶体学,IR和热重分析(TGA)等进行表征。获得的化合物1被用作将二苯甲烷(DPM)氧化为二苯甲酮的催化剂,其收率达96.8%。的存在下丁基过氧化氢(TBHP)和吡啶。对照实验表明,Co金属离子在催化反应中起重要作用。附带说明,电喷雾电离质谱(ESI-MS)和紫外光谱表明1可以在溶液中保持其完整性,磁测量表明1在低温下显示出较弱的铁磁相互作用。
更新日期:2020-07-06
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