Cobalt-nitrogen co-doped porous carbon sphere as highly efficient catalyst for liquid-phase cyclohexane oxidation with molecular oxygen and the active sites investigation  

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作  者:Lei Chen Yuan Sun Jinshan Chi Wei Xiong Pingle Liu Fang Hao 

机构地区:[1]College of Chemical Engineering,National&Local United Engineering Research Centre for Chemical Process Simulation and Intensification,Xiangtan University,Xiangtan,411105,China

出  处:《Frontiers of Chemical Science and Engineering》2024年第3期101-112,共12页化学科学与工程前沿(英文版)

基  金:supported by National Natural Science Foundation of China(Grant No.22178294);Science and Technology Innovation Program of Hunan Province(Grant No.2022RC1117);Project of Hunan Provincial Education Department(Grant No.22A0125);Hunan Provincial Natural Science Foundation of China(Grant No.2021JJ30663);Postgraduates Scientific Research Innovation Project of Xiangtan University(Grant No.QL20220146)。

摘  要:The selective oxidation of cyclohexane to cyclohexanone and cyclohexanol(KA oil)is a challenging issue in the chemical industry.At present the industrial conversion of cyclohexane to cyclohexanone and cyclohexanol is normally controlled at less than 5%selectivity.Thus,the development of highly active and stable catalysts for the aerobic oxidation of cyclohexane is necessary to overcome this low-efficiency process.Therefore,we have developed a cobalt-nitrogen co-doped porous sphere catalyst,Co-NC-x(x is the Zn/Co molar ratio,where x=0,0.5,1,2,and 4)by pyrolyzing resorcinol-formaldehyde resin microspheres.It achieved 88.28%cyclohexanone and cyclohexanol selectivity and a cyclohexane conversion of 8.88%under Co-NC-2.The results showed that the introduction of zinc effectively alleviated the aggregation of Co nanoparticles and optimized the structural properties of the material.In addition,Co0 and pyridinic-N are proposed to be the possible active species,and their proportion efficiently increased in the presence of Zn^(2+)species.In this study,we developed a novel strategy to design highly active catalysts for cyclohexane oxidation.

关 键 词:KA oil production cyclohexane selective oxidation cobalt-nitrogen co-doped porous carbon spheres metal-organic framework 

分 类 号:O64[理学—物理化学]

 

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