Uniform single atomic Cu-1-C-4 sites anchored in graphdiyne for hydroxylation of benzene to phenol
文献类型：期刊论文
| 作者 | Yu, Jia; Cao, Changyan; Jin, Hongqiang; Chen, Weiming; Shen, Qikai; Li, Peipei; Zheng, Lirong ; He, Feng; Song, Weiguo; Li, Yuliang
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| 刊名 | NATIONAL SCIENCE REVIEW
 |
| 出版日期 | 2022 |
| 卷号 | 9期号:9页码:nwac018 |
| ISSN号 | 2095-5138 |
| 关键词 | single-atom catalysis graphdiyne copper benzene oxidation phenol |
| DOI | 10.1093/nsr/nwac018 |
| 文献子类 | Article |
| 英文摘要 | Cu single atoms anchored on graphdiyne with uniform Cu-1-C-4 single sites exhibit superior activity and selectivity in direct benzene oxidation to phenol with H2O2. For single-atom catalysts (SACs), the catalyst supports are not only anchors for single atoms, but also modulators for geometric and electronic structures, which determine their catalytic performance. Selecting an appropriate support to prepare SACs with uniform coordination environments is critical for achieving optimal performance and clarifying the relationship between the structure and the property of SACs. Approaching such a goal is still a significant challenge. Taking advantage of the strong d-pi interaction between Cu atoms and diacetylenic in a graphdiyne (GDY) support, we present an efficient and simple strategy for fabricating Cu single atoms anchored on GDY (Cu-1/GDY) with uniform Cu-1-C-4 single sites under mild conditions. The Cu atomic structure was confirmed by combining synchrotron radiation X-ray absorption spectroscopy, X-ray photoelectron spectroscopy and density functional theory (DFT) calculations. The as-prepared Cu-1/GDY exhibits much higher activity than state-of-the-art SACs in direct benzene oxidation to phenol with H2O2 reaction, with turnover frequency values of 251 h(-1) at room temperature and 1889 h(-1) at 60 degrees C, respectively. Furthermore, even with a high benzene conversion of 86%, high phenol selectivity (96%) is maintained, which can be ascribed to the hydrophobic and oleophyllic surface nature of Cu-1/GDY for benzene adsorption and phenol desorption. Both experiments and DFT calculations indicate that Cu-1-C-4 single sites are more effective at activating H2O2 to form Cu=O bonds, which are important active intermediates for benzene oxidation to phenol. |
| 电子版国际标准刊号 | 2053-714X |
| 语种 | 英语 |
| WOS记录号 | WOS:000870422400001 |
| 源URL | [http://ir.ihep.ac.cn/handle/311005/299941]  |
| 专题 | 高能物理研究所_多学科研究中心 |
| 作者单位 | 中国科学院高能物理研究所 |
| 推荐引用方式 GB/T 7714 | Yu, Jia,Cao, Changyan,Jin, Hongqiang,et al. Uniform single atomic Cu-1-C-4 sites anchored in graphdiyne for hydroxylation of benzene to phenol[J]. NATIONAL SCIENCE REVIEW,2022,9(9):nwac018. |
| APA | Yu, Jia.,Cao, Changyan.,Jin, Hongqiang.,Chen, Weiming.,Shen, Qikai.,...&Li, Yuliang.(2022).Uniform single atomic Cu-1-C-4 sites anchored in graphdiyne for hydroxylation of benzene to phenol.NATIONAL SCIENCE REVIEW,9(9),nwac018. |
| MLA | Yu, Jia,et al."Uniform single atomic Cu-1-C-4 sites anchored in graphdiyne for hydroxylation of benzene to phenol".NATIONAL SCIENCE REVIEW 9.9(2022):nwac018. |
入库方式： OAI收割
来源：高能物理研究所
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