Metal-free nitrogen- and boron-codoped mesoporous carbons for primary amides synthesis from primary alcohols via direct oxidative dehydrogenation
文献类型：期刊论文
| 作者 | Shang, Sensen1; Chen, Pei-Pei2,3; Wang, Lianyue1; Lv, Ying1; Li, Wei-Xue2,4,5; Gao, Shuang1 |
| 刊名 | Acs catalysis
 |
| 出版日期 | 2018-11-01 |
| 卷号 | 8期号:11页码:9936-9944 |
| ISSN号 | 2155-5435 |
| 关键词 | N,b-codoped carbon Mesoporous carbon Primary amides Oxidative dehydrogenation Dft calculations |
| 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 |
| URI标识 | http://www.irgrid.ac.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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来源：大连化学物理研究所
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