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Solvent-free oxidation of cyclohexane over covalently anchored transition-metal salicylaldimine complexes to α-zirconium phosphate using tert-butylhydroperoxide
Journal of Molecular Catalysis A: Chemical Pub Date : 2016 , DOI: 10.1016/j.molcata.2015.10.010
Savita Khare , Priti Shrivastava

Heterogeneous catalysts were prepared by covalent bonding of transition-metal salicylaldimine complex to α-zirconium phosphate, abbreviated as {α-ZrP.M(salicylaldimine) where M = Co, Mn and Cu}. The resulting compounds were characterized by BET surface area, TGA analysis, X-ray diffraction, Scanning electron micrograph, energy dispersive X-ray analysis, Fourier transform infrared and Atomic absorption spectroscopy. The catalytic activity of α-ZrP.M(salicylaldimine) was studied for the liquid phase oxidation of cyclohexane using tert-butylhydroperoxide as an oxidant under solvent free condition. In the oxidation reaction, cyclohexane was oxidized to cyclohexanol, cyclohexanone and some unidentified products. It was found that the reactivity of α-ZrP.M(salicylaldimine) catalyst for the oxidation reaction decreased in the order α-ZrP.Co(salicylaldimine) > α-ZrP.Mn(salicylaldimine) > α-ZrP.Cu(salicylaldimine). A maximum conversion of cyclohexane (14.18%) and selectivity of cyclohexanol (4.99%), cyclohexanone (87.34%) and some other products (7.67%) was observed for catalyst, α-ZrP.Co(salicylaldimine) after 6 h at 353 K. The catalyst, α-ZrP.Co(salicylaldimine) was reused for four cycles without significant loss of catalytic activity.

中文翻译:

使用叔丁基氢过氧化物在共价锚定的过渡金属水杨醛亚胺络合物上无溶剂氧化环己烷生成磷酸α-锆

通过将过渡金属水杨醛亚胺络合物与α-磷酸锆共价键合制备多相催化剂,缩写为{α-ZrP.M(水杨醛亚胺),其中M = Co,Mn和Cu}。通过BET表面积,TGA分析,X射线衍射,扫描电子显微照片,能量色散X射线分析,傅立叶变换红外光谱和原子吸收光谱对所得化合物进行表征。研究了α-ZrP.M(水杨醛亚胺)对叔丁基环己烷液相氧化的催化活性-在无溶剂条件下用作氧化剂的过氧化氢丁基酯。在氧化反应中,环己烷被氧化为环己醇,环己酮和一些未鉴定的产物。发现α-ZrP.M(水杨醛亚胺)催化剂对氧化反应的反应性以α-ZrP.Co(水杨醛亚胺)>α-ZrP.Mn(水杨醛亚胺)>α-ZrP.Cu(水杨醛亚胺)的顺序降低。 。在353 K下反应6小时后,观察到催化剂α-ZrP.Co(水杨醛亚胺)的最大环己烷转化率(14.18%)和环己醇(4.99%),环己酮(87.34%)和一些其他产物的选择性(7.67%)。催化剂α-ZrP.Co(水杨醛亚胺)被重复使用了四个循环,而没有明显的催化活性损失。
更新日期:2017-01-31
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