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	Metal-free nitrogen- and boron-codoped mesoporous carbons for primary amides synthesis from primary alcohols via direct oxidative dehydrogenation
	Shang, Sensen1; Chen, Pei-Pei2,3; Wang, Lianyue1; Lv, Ying1; Li, Wei-Xue2,4,5; Gao, Shuang1
刊名	Acs catalysis
	2018-11-01
卷号	8期号:11页码:9936-9944
关键词	N,b-codoped carbon Mesoporous carbon Primary amides Oxidative dehydrogenation Dft calculations
ISSN号	2155-5435
DOI	10.1021/acscatal.8b02889
通讯作者	Li, wei-xue(wxli70@ustc.edu.cn) ; Gao, shuang(sgao@dicp.ac.cn)
英文摘要	Metal-free catalysts show environmental friendliness and cost-effectiveness, as well as less susceptibility to poisoning over metal and metal oxide catalysts. in this respect, we present the synthesis and characterization of metal-free mesoporous nitrogen- and boron-codoped nanocarbon (meso-n,b/c), which exhibits good catalytic performance with conversion of 89% and selectivity of 83% toward amide synthesis from primary alcohols using nh4oac as an ammonia resource under an oxygen atmosphere. the facile codoping synthetic strategy was executed by pyrolysis of nitrogen-enriched ligand 4,5-diazafluorene-9-one azine (daa) and h3bo3 as a nitrogen and boron content modulator, respectively. significantly, control experiments revealed that the reaction proceeded through direct oxidative dehydrogenation of hemiaminal after aldehyde-ammonia condensation, which was remarkably different from that in the previous literature. density functional theory (dft) calculations further demonstrate that the selective preference for benzamide largely benefits from the strong adsorption and enhanced activity of oxygen molecules via the interaction with a b atom doped in the catalyst. the active sites in the meso-n,b/c catalyst are proposed to be b atom bonded with n within the graphitic carbon sheets. this founding opens up avenues for the development of modified carbon materials on metal-free catalysis.
WOS关键词	TOTAL-ENERGY CALCULATIONS ; SOLID-STATE NMR ; WAVE BASIS-SET ; DOPED GRAPHENE ; AMINES ; CATALYST ; EFFICIENT ; NITRIDE ; WATER ; NANOSTRUCTURES
WOS研究方向	Chemistry
WOS类目	Chemistry, Physical
语种	英语
出版者	AMER CHEMICAL SOC
WOS记录号	WOS:000449723900004
内容类型	期刊论文
URI标识	http://www.corc.org.cn/handle/1471x/2373078
专题	大连化学物理研究所
通讯作者	Li, Wei-Xue; Gao, Shuang
作者单位	1.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Liaoning, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Liaoning, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 4.Univ Sci & Technol China, CAS Ctr Excellence Nanosci, iChEM, Sch Chem & Mat Sci, Hefei 230026, Anhui, Peoples R China 5.Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
推荐引用方式 GB/T 7714	Shang, Sensen,Chen, Pei-Pei,Wang, Lianyue,et al. Metal-free nitrogen- and boron-codoped mesoporous carbons for primary amides synthesis from primary alcohols via direct oxidative dehydrogenation[J]. Acs catalysis,2018,8(11):9936-9944.
APA	Shang, Sensen,Chen, Pei-Pei,Wang, Lianyue,Lv, Ying,Li, Wei-Xue,&Gao, Shuang.(2018).Metal-free nitrogen- and boron-codoped mesoporous carbons for primary amides synthesis from primary alcohols via direct oxidative dehydrogenation.Acs catalysis,8(11),9936-9944.
MLA	Shang, Sensen,et al."Metal-free nitrogen- and boron-codoped mesoporous carbons for primary amides synthesis from primary alcohols via direct oxidative dehydrogenation".Acs catalysis 8.11(2018):9936-9944.

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