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Oxidative dehydrogenation reaction of short alkanes on nanostructured carbon catalysts: a computational account
Sun, XY; Han, P; Li, B; Mao, SJ; Liu, TF; Ali, S; Lian, Z; Su, DS; Su, DS (reprint author), Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, 72 Wenhua Rd, Shenyang 110016, Liaoning, Peoples R China.
2018-01-25
Source PublicationCHEMICAL COMMUNICATIONS
ISSN1359-7345
Volume54Issue:8Pages:864-875
AbstractRecent progress from first principles computational studies is presented for catalytic properties of nanostructured carbon catalysts in the oxidative dehydrogenation (ODH) reaction of short alkanes. Firstly, a brief introduction is given on the development of carbon catalysts in ODH since 1970. Oxygen functional groups have pivotal importance for ODH on nanostructured carbon catalysts. We discuss the oxidation process by HNO3 on pristine and defective carbon materials. The interactions between the oxygen molecule (oxidant) and the nanostructured carbon catalysts are quantitatively calibrated. Moreover the different nucleophilic abilities of oxygen functional groups are carefully compared and the strongest nucleophilic sites are proposed. The active sites and detailed reaction pathway are revealed from several computational studies. Diketone/quinone groups are generally considered to be the active centers in ODH. A reaction pathway via radical formation is considered as the favorable path. Furthermore, single ketone and carbon sites are verified to be active in ODH from the analysis of aromaticity. Heteroatom doping effects in ODH are examined. Nitrogen doping is found to be very reactive towards oxygen molecule activation. Other dopants such as boron, phosphorous and sulfur also have positive effects on the reactivity of ODH. Extensive calculations suggest that the BEP relation is applicable for the doped nanostructured carbon catalysts. In the end, an outlook for the future direction of the computational study is supplied.; Recent progress from first principles computational studies is presented for catalytic properties of nanostructured carbon catalysts in the oxidative dehydrogenation (ODH) reaction of short alkanes. Firstly, a brief introduction is given on the development of carbon catalysts in ODH since 1970. Oxygen functional groups have pivotal importance for ODH on nanostructured carbon catalysts. We discuss the oxidation process by HNO3 on pristine and defective carbon materials. The interactions between the oxygen molecule (oxidant) and the nanostructured carbon catalysts are quantitatively calibrated. Moreover the different nucleophilic abilities of oxygen functional groups are carefully compared and the strongest nucleophilic sites are proposed. The active sites and detailed reaction pathway are revealed from several computational studies. Diketone/quinone groups are generally considered to be the active centers in ODH. A reaction pathway via radical formation is considered as the favorable path. Furthermore, single ketone and carbon sites are verified to be active in ODH from the analysis of aromaticity. Heteroatom doping effects in ODH are examined. Nitrogen doping is found to be very reactive towards oxygen molecule activation. Other dopants such as boron, phosphorous and sulfur also have positive effects on the reactivity of ODH. Extensive calculations suggest that the BEP relation is applicable for the doped nanostructured carbon catalysts. In the end, an outlook for the future direction of the computational study is supplied.
description.department[sun, xiaoying ; han, peng] shenyang normal univ, inst catalysis energy & environm, coll chem & chem engn, shenyang 110034, liaoning, peoples r china ; [li, bo ; mao, shanjun ; liu, tianfu ; ali, sajjad ; lian, zan ; su, dangsheng] chinese acad sci, inst met res, shenyang natl lab mat sci, 72 wenhua rd, shenyang 110016, liaoning, peoples r china ; [liu, tianfu ; lian, zan] univ sci & technol china, sch mat sci & engn, shenyang 110016, liaoning, peoples r china ; [ali, sajjad] univ chinese acad sci, beijing 100049, peoples r china
Keywordh Bond Activation Initio Molecular-dynamics Density-functional Theory Vanadium-oxide Catalysts Metal-free Catalysts Nitric-acid Mediated Catalysis Oxygen-adsorption Styrene Synthesis 1st Principles
Subject AreaChemistry, Multidisciplinary
Funding OrganizationNSFC [21573255, 51521091]; Chinese Academy of Sciences [XDA09030103]; LiaoNing Natural Science Foundation [201602676]; Special Program for Applied Research on Super Computation of the NSFC Guangdong Joint Fund [U1501501]
Indexed BySCI
Language英语
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/79565
Collection中国科学院金属研究所
Corresponding AuthorLi, B; Su, DS (reprint author), Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, 72 Wenhua Rd, Shenyang 110016, Liaoning, Peoples R China.
Recommended Citation
GB/T 7714
Sun, XY,Han, P,Li, B,et al. Oxidative dehydrogenation reaction of short alkanes on nanostructured carbon catalysts: a computational account[J]. CHEMICAL COMMUNICATIONS,2018,54(8):864-875.
APA Sun, XY.,Han, P.,Li, B.,Mao, SJ.,Liu, TF.,...&Su, DS .(2018).Oxidative dehydrogenation reaction of short alkanes on nanostructured carbon catalysts: a computational account.CHEMICAL COMMUNICATIONS,54(8),864-875.
MLA Sun, XY,et al."Oxidative dehydrogenation reaction of short alkanes on nanostructured carbon catalysts: a computational account".CHEMICAL COMMUNICATIONS 54.8(2018):864-875.
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