Selective Hydrodeoxygenation of Aromatics to Cyclohexanols over Ru Single Atoms Supported on CeO2
文献类型：期刊论文
| ; | |
| 作者 | Zhang, KL ; Meng, QL; Wu, HH; Yan, J; Mei, XL; An, PF; Zheng, LR; Zhang, J; He, MY; Han, BX
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| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
 ; JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
|
| 出版日期 | 2022 ; 2022 |
| 卷号 | 144期号:45页码:20834-20846 |
| ISSN号 | 0002-7863 ; 0002-7863 |
| DOI | 10.1021/jacs.2c08992 ; 10.1021/jacs.2c08992 |
| 文献子类 | Article ; Article |
| 英文摘要 | Cyclohexanols are widely used chemicals, which are mainly produced by oxidation of fossil feedstocks. Selective hydrodeoxygenation of lignin derivatives has great potential for producing these chemicals but is challenging to obtain high yields. Here, we report that CeO2-supported Ru single-atom catalysts (SACs) enabled the hydrogenation of the benzene ring and catalyzed etheric C-O(R) bond cleavage without changing the C- O(H) bond, which could afford 99.9% yields of cyclohexanols. As far as we know, this is the first to report that SACs catalyze hydrogenation of the aromatic ring. The reaction mechanism was studied by control experiments and density functional theory calculations. In the catalysts, the Ru-O-Ce sites were formed and one Ru atom was coordinated with about four O atoms. These catalytic sites could realize both the hydrogenation and deoxygenation reactions efficiently, and thus desired cyclohexanols were generated. This work pioneers the single-atom catalysis in aromatic transformation and provides a novel route for synthesis of cyclohexanols.; Cyclohexanols are widely used chemicals, which are mainly produced by oxidation of fossil feedstocks. Selective hydrodeoxygenation of lignin derivatives has great potential for producing these chemicals but is challenging to obtain high yields. Here, we report that CeO2-supported Ru single-atom catalysts (SACs) enabled the hydrogenation of the benzene ring and catalyzed etheric C-O(R) bond cleavage without changing the C- O(H) bond, which could afford 99.9% yields of cyclohexanols. As far as we know, this is the first to report that SACs catalyze hydrogenation of the aromatic ring. The reaction mechanism was studied by control experiments and density functional theory calculations. In the catalysts, the Ru-O-Ce sites were formed and one Ru atom was coordinated with about four O atoms. These catalytic sites could realize both the hydrogenation and deoxygenation reactions efficiently, and thus desired cyclohexanols were generated. This work pioneers the single-atom catalysis in aromatic transformation and provides a novel route for synthesis of cyclohexanols. |
| 电子版国际标准刊号 | 1520-5126 ; 1520-5126 |
| 语种 | 英语 ; 英语 |
| WOS记录号 | WOS:000883022700001 ; WOS:000883022700001 |
| 源URL | [http://ir.ihep.ac.cn/handle/311005/299813]  |
| 专题 | 高能物理研究所_多学科研究中心 高能物理研究所_实验物理中心 |
| 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 | Zhang, KL,Meng, QL,Wu, HH,et al. Selective Hydrodeoxygenation of Aromatics to Cyclohexanols over Ru Single Atoms Supported on CeO2, Selective Hydrodeoxygenation of Aromatics to Cyclohexanols over Ru Single Atoms Supported on CeO2[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2022, 2022,144, 144(45):20834-20846, 20834-20846. |
| APA | Zhang, KL.,Meng, QL.,Wu, HH.,Yan, J.,Mei, XL.,...&Han, BX.(2022).Selective Hydrodeoxygenation of Aromatics to Cyclohexanols over Ru Single Atoms Supported on CeO2.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,144(45),20834-20846. |
| MLA | Zhang, KL,et al."Selective Hydrodeoxygenation of Aromatics to Cyclohexanols over Ru Single Atoms Supported on CeO2".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 144.45(2022):20834-20846. |
入库方式： OAI收割
来源：高能物理研究所
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