Aerobic oxidation of the C-H bond under ambient conditions using highly dispersed Co over highly porous N-doped carbon

被引:18
|
作者
Nie, Renfeng [1 ,2 ,3 ]
Chen, Jingwen [3 ]
Chen, Minda [3 ]
Qi, Zhiyuan [3 ]
Goh, Tian-Wei [3 ]
Ma, Tao [4 ]
Zhou, Lin [4 ]
Pei, Yuchen [3 ]
Huang, Wenyu [3 ,4 ]
机构
[1] Hubei Univ, Hubei Collaborat Innovat Ctr Adv Organ Chem Mat, Wuhan 430062, Hubei, Peoples R China
[2] Hubei Univ, Sch Chem & Chem Engn, Key Lab Synth & Applicat Organ Funct Mol, Minist Educ, Wuhan 430062, Hubei, Peoples R China
[3] Iowa State Univ, Dept Chem, Ames, IA 50011 USA
[4] US DOE, Ames Lab, Ames, IA 50011 USA
基金
中国国家自然科学基金;
关键词
SELECTIVE OXIDATION; CATALYTIC PERFORMANCE; COBALT NANOPARTICLES; SUPPORTED RU; ALCOHOLS; EFFICIENT; HYDROGENATION; CONVERSION; OXYGEN; SITES;
D O I
10.1039/c8gc03653e
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Highly dispersed Co sites in highly porous N-doped carbon (Co-NC) were synthesized by high-temperature pyrolysis of Zn/Co bimetallic zeolitic imidazolate framework-8 (CoxZn100-x-ZIF). Wide characterization indicated that the pyrolysis atmosphere and temperature play crucial roles in the metal dispersion and pore structure of the resulting materials. A hydrogen treatment at elevated temperatures is found to favour the Zn volatilization and restrict the pore shrinkage of the ZIF precursor, thus yielding efficient catalysts with highly dispersed Co, a high surface area (1090 m(2) g(-1)) and pore volume (0.89 cm(3) g(-1)). When used as a catalyst for aerobic oxidation of ethylbenzene (EB), Co1Zn99-ZIF-800-H-2 contributes to 98.9% EB conversion and 93.1% ketone selectivity under mild conditions (60 degrees C, 1 atm O-2), which is 41.3 times more active in comparison to the ZIF-67-derived Co catalyst. Co-NC is stable and could be reused four times without obvious deactivation. This catalyst displays good chemoselectivity to the corresponding ketones when using a broad scope of hydrocarbon compounds.
引用
收藏
页码:1461 / 1466
页数:6
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