Highly Efficient Metal-Free Nitrogen-Doped Nanocarbons with Unexpected Active Sites for Aerobic Catalytic Reactions
文献类型：期刊论文
| 作者 | Lin, Yangming1,2; Liu, Zigeng2; Niu, Yiming1; Zhang, Bingsen1; Lu, Qing2; Wu, Shuchang1; Centi, Gabriele3; Perathoner, Siglinda3; Heumann, Saskia2; Yu, Linhui2,4 |
| 刊名 | ACS NANO
 |
| 出版日期 | 2019-12-01 |
| 卷号 | 13期号:12页码:13995-14004 |
| ISSN号 | 1936-0851 |
| 关键词 | nanodiamond carbon materials metal-free nitrogen-doped catalysis model catalyst kinetic isotope effect |
| DOI | 10.1021/acsnano.9b05856 |
| 通讯作者 | Lin, Yangming(yang-ming.lin@cec.mpg.de) ; Yu, Linhui(linhui.yu@cec.mpg.de) |
| 英文摘要 | Nitrogen (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. |
| 资助项目 | Strategic Priority Research Program of the Chinese Academy of Sciences[XDA09030103] ; National Natural Science Foundation of China[91545119] ; Max Planck Society |
| WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science |
| 语种 | 英语 |
| 出版者 | AMER CHEMICAL SOC |
| WOS记录号 | WOS:000505633300038 |
| 资助机构 | Strategic Priority Research Program of the Chinese Academy of Sciences ; National Natural Science Foundation of China ; Max Planck Society |
| 源URL | [http://ir.imr.ac.cn/handle/321006/136367]  |
| 专题 | 金属研究所_中国科学院金属研究所 |
| 通讯作者 | Lin, Yangming; Yu, Linhui |
| 作者单位 | 1.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 |
| 推荐引用方式 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. |
入库方式： OAI收割
来源：金属研究所
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