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N-Doped Sub-3 nm Co Nanoparticles as Highly Efficient and Durable Aerobic Oxidative Coupling Catalysts
Han, Junxing1; Gu, Feifei2; Li, Yuchao1,3
2016-09-01
发表期刊CHEMISTRY-AN ASIAN JOURNAL
ISSN1861-4728
卷号11期号:18页码:2594-2601
摘要

A nano-coating associated with sulfuric acid leaching protocol was developed to prepare N-doped sub-3 nm Co-based nanoparticle catalyst (Co-N/C) using melamine-formaldehyde resin as the N-containing precursor, active carbon as the support, and Co(NO3)(2) as the Co-containing precursor. By thermal treatment under nitrogen atmosphere at 800 degrees C and leached with sulfuric acid solution, a stable and highly dispersive Co-N coordination structure was uniformly dispersed on the formed Co-N/C catalyst with a Co loading of 0.47 wt% and Co nanoparticle size of 2.55 nm. The Co-N/C catalyst was characterized with XRD, XPS, Raman, SEM, TEM, ICP, and elemental analysis. The Co-N/C catalyst showed extremely high catalytic efficiency with a TON of 257 for the aerobic oxidative coupling of aldehydes with methanol to directly synthesize methyl esters with molecular oxygen as the final oxidant. The Co-N/C catalyst also showed broad substrate range and stable recyclability. After recycling for 7 times, no obvious deactivation was detected. It was confirmed that the sub-3 nm Co-N coordination structure formed between metallic Co nanoparticles and pyridinic nitrogen doping into graphitic layers functions as the active site to activate molecular oxygen for the b-H elimination from generated hemiacetal intermediates to produce methyl esters. The nano-coating associated with acid leaching protocol provides a novel strategy to prepare highly efficient non-precious metal-based catalysts.

关键词Aldehydes Cobalt Methanol Nitrogen Oxidative Coupling
文章类型Article
WOS标题词Science & Technology ; Physical Sciences
DOI10.1002/asia.201600921
收录类别SCI
语种英语
关键词[WOS]HIGH-PERFORMANCE ELECTROCATALYSTS ; OXYGEN REDUCTION REACTION ; COBALT OXIDE CATALYSTS ; SELECTIVE OXIDATION ; ALCOHOLS ; ESTERIFICATION ; ALDEHYDES ; GOLD ; HYDROGEN ; ESTERS
WOS研究方向Chemistry
WOS类目Chemistry, Multidisciplinary
项目资助者Beijing Municipal Natural Science Foundation(2153042) ; National Natural Science Foundation of China(21306203)
WOS记录号WOS:000387462100013
引用统计
被引频次:4[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.ipe.ac.cn/handle/122111/21651
专题研究所(批量导入)
作者单位1.Chinese Acad Sci, Inst Proc Engn, Beijing 100190, Peoples R China
2.Beijing City Univ, Beijing 101399, Peoples R China
3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
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Han, Junxing,Gu, Feifei,Li, Yuchao. N-Doped Sub-3 nm Co Nanoparticles as Highly Efficient and Durable Aerobic Oxidative Coupling Catalysts[J]. CHEMISTRY-AN ASIAN JOURNAL,2016,11(18):2594-2601.
APA Han, Junxing,Gu, Feifei,&Li, Yuchao.(2016).N-Doped Sub-3 nm Co Nanoparticles as Highly Efficient and Durable Aerobic Oxidative Coupling Catalysts.CHEMISTRY-AN ASIAN JOURNAL,11(18),2594-2601.
MLA Han, Junxing,et al."N-Doped Sub-3 nm Co Nanoparticles as Highly Efficient and Durable Aerobic Oxidative Coupling Catalysts".CHEMISTRY-AN ASIAN JOURNAL 11.18(2016):2594-2601.
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