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Highly Efficient Metal-Free Nitrogen-Doped Nanocarbons with Unexpected Active Sites for Aerobic Catalytic Reactions
Lin, Yangming1,2; Liu, Zigeng2; Niu, Yiming1; Zhang, Bingsen1; Lu, Qing2; Wu, Shuchang1; Centi, Gabriele3; Perathoner, Siglinda3; Heumann, Saskia2; Yu, Linhui2,4; Su, Dang Sheng1,5
Corresponding AuthorLin, Yangming(yang-ming.lin@cec.mpg.de) ; Yu, Linhui(linhui.yu@cec.mpg.de)
2019-12-01
Source PublicationACS NANO
ISSN1936-0851
Volume13Issue:12Pages:13995-14004
AbstractNitrogen (N)-doped nanocarbons (NDN) as metal-free catalysts have elicited considerable attention toward selective oxidation of alcohols with easily oxidizable groups to aldehydes in the past few years. However, finding a new NDN catalytic material that can meet the requirement of the feasibility on the aerobic catalytics for other complicated alcohols is a big challenge. The real active sites and the corresponding mechanisms on NDN are still unambiguous because of inevitable coexistence of diverse edge sites and N species based on recently reported doping methods. Here, four NDN catalysts with enriched pyridinic N species and without any graphitic N species are simply fabricated via a chemical-vapor-deposition-like method. The results of X-ray photoelectron spectroscopy and X-ray absorption near-edge structure spectra suggest that the dominating N species on NDN are pyridinic N. It is demonstrated that NDN catalysts perform impressive reactivity for aerobic oxidation of complicated alcohols at an atmospheric pressure. Eleven kinds of aromatic molecules with single N species and tunable pi conjugation systems are used as model catalysts to experimentally identify the actual role of each N species at a real molecular level. It is suggested that pyridinic N species play an unexpected role in catalytic reactions. Neighboring carbon atoms in pyridinic N species are responsible for facilitating the rate-determining step process clarified by kinetic isotope effects, in situ nuclear magnetic resonance, in situ attenuated total reflectance infrared, and theoretical calculation. Moreover, NDN catalysts exhibit a good catalytic feasibility on the synthesis of important natural products (e.g., intermediates of vitamin E and K3) from phenol oxidation.
Keywordnanodiamond carbon materials metal-free nitrogen-doped catalysis model catalyst kinetic isotope effect
Funding OrganizationStrategic Priority Research Program of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; Max Planck Society
DOI10.1021/acsnano.9b05856
Indexed BySCI
Language英语
Funding ProjectStrategic Priority Research Program of the Chinese Academy of Sciences[XDA09030103] ; National Natural Science Foundation of China[91545119] ; Max Planck Society
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science
WOS SubjectChemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS IDWOS:000505633300038
PublisherAMER CHEMICAL SOC
Citation statistics
Cited Times:2[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/136368
Collection中国科学院金属研究所
Corresponding AuthorLin, Yangming; Yu, Linhui
Affiliation1.Chinese Acad Sci, Inst Met Res, 72 Wenhua Rd, Shenyang 110016, Peoples R China
2.Max Planck Inst Chem Energy Convers, Stiftstr 34-36, D-45470 Mulheim, Germany
3.Univ Messina, Vle F Stagno DAlcontres 31, I-98166 Messina, Italy
4.Fuzhou Univ, Fuzhou 350002, Peoples R China
5.Max Planck Gesell, Fritz Haber Inst, Dept Inorgan Chem, Faradayweg 4-6, D-14195 Berlin, Germany
Recommended Citation
GB/T 7714
Lin, Yangming,Liu, Zigeng,Niu, Yiming,et al. Highly Efficient Metal-Free Nitrogen-Doped Nanocarbons with Unexpected Active Sites for Aerobic Catalytic Reactions[J]. ACS NANO,2019,13(12):13995-14004.
APA Lin, Yangming.,Liu, Zigeng.,Niu, Yiming.,Zhang, Bingsen.,Lu, Qing.,...&Su, Dang Sheng.(2019).Highly Efficient Metal-Free Nitrogen-Doped Nanocarbons with Unexpected Active Sites for Aerobic Catalytic Reactions.ACS NANO,13(12),13995-14004.
MLA Lin, Yangming,et al."Highly Efficient Metal-Free Nitrogen-Doped Nanocarbons with Unexpected Active Sites for Aerobic Catalytic Reactions".ACS NANO 13.12(2019):13995-14004.
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