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Nitrogen-doped carbon nanotubes encapsulate cobalt nanoparticles as efficient catalysts for aerobic and solvent-free selective oxidation of hydrocarbons
Lin, Xiu; Nie, Zhenzhen; Zhang, Liyun; Mei, Shuchuan; Chen, Yuan; Zhang, Bingsen; Zhu, Runliang; Liu, Zhigang; Liu, ZG (reprint author), Hunan Univ, Sch Chem & Chem Engn, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Hunan, Peoples R China.; Zhang, BS (reprint author), Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China.
2017-05-07
发表期刊GREEN CHEMISTRY
ISSN1463-9262
卷号19期号:9页码:2164-2173
摘要The selective oxidation of hydrocarbons to the corresponding ketones with solvent-free and molecular oxygen as an oxidant is of great importance in academic and industrial fields in view of economy and environment. In this respect, we present the facile synthesis and characterization of excellent catalysts comprising cobalt nanoparticles encapsulated into graphitic nitrogen-doped carbon nanotubes (Co@GCNs) via one-pot pyrolysis of a chelate compound containing citric acid, melamine, and CoCl2 center dot 6H(2)O. The selective oxidation of ethylbenzene under molecular oxygen and solvent-free conditions is employed as a probe reaction to investigate the catalytic performance; the optimized catalyst shows the best conversion (68%) and selectivity for acetophenone (93%). Combination of the catalytic results of the control group and the different characterization methods demonstrates that high catalytic activity is due to the synergistic effect between metallic cobalt and nitrogen-doped carbon nanotubes. Moreover, the catalyst has high catalytic activity for the aerobic and solvent-free oxidation of other aryl-alkane substrates. The proposed mechanistic study illustrates that the reaction is a free radical reaction progressing through superoxide radical anions (O-center dot(2-)).; The selective oxidation of hydrocarbons to the corresponding ketones with solvent-free and molecular oxygen as an oxidant is of great importance in academic and industrial fields in view of economy and environment. In this respect, we present the facile synthesis and characterization of excellent catalysts comprising cobalt nanoparticles encapsulated into graphitic nitrogen-doped carbon nanotubes (Co@GCNs) via one-pot pyrolysis of a chelate compound containing citric acid, melamine, and CoCl2 center dot 6H(2)O. The selective oxidation of ethylbenzene under molecular oxygen and solvent-free conditions is employed as a probe reaction to investigate the catalytic performance; the optimized catalyst shows the best conversion (68%) and selectivity for acetophenone (93%). Combination of the catalytic results of the control group and the different characterization methods demonstrates that high catalytic activity is due to the synergistic effect between metallic cobalt and nitrogen-doped carbon nanotubes. Moreover, the catalyst has high catalytic activity for the aerobic and solvent-free oxidation of other aryl-alkane substrates. The proposed mechanistic study illustrates that the reaction is a free radical reaction progressing through superoxide radical anions (O-center dot(2-)).
部门归属[lin, xiu ; nie, zhenzhen ; mei, shuchuan ; chen, yuan ; liu, zhigang] hunan univ, sch chem & chem engn, state key lab chemo biosensing & chemometr, changsha 410082, hunan, peoples r china ; [zhang, liyun ; zhang, bingsen] chinese acad sci, inst met res, shenyang natl lab mat sci, shenyang 110016, peoples r china ; [zhu, runliang] chinese acad sci, guangzhou inst geochem, guangdong prov key lab mineral phys & mat res & d, guangzhou 510640, guangdong, peoples r china
学科领域Chemistry, Multidisciplinary ; Green & Sustainable Science & Technology
收录类别SCI
语种英语
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/78142
专题中国科学院金属研究所
通讯作者Liu, ZG (reprint author), Hunan Univ, Sch Chem & Chem Engn, State Key Lab Chemo Biosensing & Chemometr, Changsha 410082, Hunan, Peoples R China.; Zhang, BS (reprint author), Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China.
推荐引用方式
GB/T 7714
Lin, Xiu,Nie, Zhenzhen,Zhang, Liyun,et al. Nitrogen-doped carbon nanotubes encapsulate cobalt nanoparticles as efficient catalysts for aerobic and solvent-free selective oxidation of hydrocarbons[J]. GREEN CHEMISTRY,2017,19(9):2164-2173.
APA Lin, Xiu.,Nie, Zhenzhen.,Zhang, Liyun.,Mei, Shuchuan.,Chen, Yuan.,...&Zhang, BS .(2017).Nitrogen-doped carbon nanotubes encapsulate cobalt nanoparticles as efficient catalysts for aerobic and solvent-free selective oxidation of hydrocarbons.GREEN CHEMISTRY,19(9),2164-2173.
MLA Lin, Xiu,et al."Nitrogen-doped carbon nanotubes encapsulate cobalt nanoparticles as efficient catalysts for aerobic and solvent-free selective oxidation of hydrocarbons".GREEN CHEMISTRY 19.9(2017):2164-2173.
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