DICP OpenIR
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
Corresponding AuthorLi, Wei-Xue(wxli70@ustc.edu.cn) ; Gao, Shuang(sgao@dicp.ac.cn)
KeywordN,B-codoped carbon mesoporous carbon primary amides oxidative dehydrogenation DFT calculations
Source PublicationACS CATALYSIS
2018-11-01
ISSN2155-5435
DOI10.1021/acscatal.8b02889
Volume8Issue:11Pages:9936-9944
Funding ProjectNational Natural Science Foundation of China[21773232] ; National Natural Science Foundation of China[21773227] ; National Natural Science Foundation of China[91645202] ; Frontier Science Key Project of the Chinese Academy of Sciences[QYZDJ-SSW-SLH054] ; National Key R&D Program of China[2017YFB0602205] ; National Key R&D Program of China[2018YFA0208603]
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; Frontier Science Key Project of the Chinese Academy of Sciences ; Frontier Science Key Project of the Chinese Academy of Sciences ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Frontier Science Key Project of the Chinese Academy of Sciences ; Frontier Science Key Project of the Chinese Academy of Sciences ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Frontier Science Key Project of the Chinese Academy of Sciences ; Frontier Science Key Project of the Chinese Academy of Sciences ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Frontier Science Key Project of the Chinese Academy of Sciences ; Frontier Science Key Project of the Chinese Academy of Sciences ; National Key R&D Program of China ; National Key R&D Program of China
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordTOTAL-ENERGY CALCULATIONS ; SOLID-STATE NMR ; WAVE BASIS-SET ; DOPED GRAPHENE ; AMINES ; CATALYST ; EFFICIENT ; NITRIDE ; WATER ; NANOSTRUCTURES
AbstractMetal-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.
Language英语
Funding OrganizationNational Natural Science Foundation of China ; National Natural Science Foundation of China ; Frontier Science Key Project of the Chinese Academy of Sciences ; Frontier Science Key Project of the Chinese Academy of Sciences ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Frontier Science Key Project of the Chinese Academy of Sciences ; Frontier Science Key Project of the Chinese Academy of Sciences ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Frontier Science Key Project of the Chinese Academy of Sciences ; Frontier Science Key Project of the Chinese Academy of Sciences ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Frontier Science Key Project of the Chinese Academy of Sciences ; Frontier Science Key Project of the Chinese Academy of Sciences ; National Key R&D Program of China ; National Key R&D Program of China
WOS IDWOS:000449723900004
PublisherAMER CHEMICAL SOC
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/166643
Collection中国科学院大连化学物理研究所
Corresponding AuthorLi, Wei-Xue; Gao, Shuang
Affiliation1.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
Recommended Citation
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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