Three-Dimensional Phosphine Metal-Organic Frameworks Assembled from Cu(I) and Pyridyl Diphosphine | |
Department | OSSO国家重点实验室 |
Tan X(谭馨)1; Li L(李垒)1; Zhang JY(张建勇)1; Han XR(韩晓蕊)1; Jiang L(姜隆)1; Li FW(李福伟)2; Su CY(苏成勇)1; Zhang JY(张建勇) | |
2012 | |
Source Publication | Chemistry of Materials |
ISSN | 0897-4756 |
Volume | 24Issue:3Pages:480-485 |
Abstract | Metal−organic frameworks (MOFs) with phosphine based ligands are extremely attractive for catalysis. In this paper, phosphine has been successfully incorporated for the first time into three-dimensional (3D) MOFs. The MOFs are based on rigid L2M2 dimeric secondary building blocks assembled from Cu(I) and a pyridyl diphosphine ligand, 4-(3,5-bis(diphenylphosphino)phenyl)pyridine, with Br− (CuL-Br), Cl− (CuL-Br), or PF6− (CuL-PF6) as counteranions. The structures have a 4.122 net topology, which can be further simplified to 64.82-qtz. The MOFs contain 1D homochiral channels. The PF6− anions hosted in the 1D channel of CuL-PF6 can be readily exchanged with Br− or Cl− while keeping the framework intact. The materials show anion-tunable flexible porosity. CuL-Br reveals gradual uptake of MeOH, while CuL-PF6 exhibits stepwise sorption for MeOH. The heterogeneous Lewis acid catalytic activity of the MOFs has been shown in ketalization reaction. CuL-Br and CuL-PF6 are active in the reactions between ethylene glycol and 2-butanone/cyclohexanone, up to 93% yield with 0.2 mol % catalyst loading. In contrast, no reaction happens between ethylene glycol and bulky benzophenone, suggesting profound size selectivity. The catalysts can be reused with the framework left intact for three runs without loss of activity. |
Keyword | Metal-organic Framework Phosphine Copper Sorption Catalysis |
Subject Area | 物理化学与绿色催化 |
DOI | 10.1021/cm202608f |
Funding Organization | the Natural Science Foundation of China (20903121;20821001;U0934003);the Fundamental Research Funds for the Central Universities;the Specialized Research Fund for the Doctoral Program of Higher Education of China, and the SRF for ROCS of SEM |
Indexed By | SCI |
Language | 英语 |
Funding Project | 均相催化研究组 |
compositor | 第二作者单位 |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.licp.cn/handle/362003/3794 |
Collection | 羰基合成与选择氧化国家重点实验室(OSSO) |
Corresponding Author | Zhang JY(张建勇) |
Affiliation | 1.Sun Yat Sen Univ, Sch Chem & Chem Engn, KLGHEI Environm & Energy Chem, Guangzhou 510275, Guangdong, Peoples R China 2.Chinese Acad Sci, Lanzhou Inst Chem Phys, Lanzhou 730000, Peoples R China |
Recommended Citation GB/T 7714 | Tan X,Li L,Zhang JY,et al. Three-Dimensional Phosphine Metal-Organic Frameworks Assembled from Cu(I) and Pyridyl Diphosphine[J]. Chemistry of Materials,2012,24(3):480-485. |
APA | Tan X.,Li L.,Zhang JY.,Han XR.,Jiang L.,...&张建勇.(2012).Three-Dimensional Phosphine Metal-Organic Frameworks Assembled from Cu(I) and Pyridyl Diphosphine.Chemistry of Materials,24(3),480-485. |
MLA | Tan X,et al."Three-Dimensional Phosphine Metal-Organic Frameworks Assembled from Cu(I) and Pyridyl Diphosphine".Chemistry of Materials 24.3(2012):480-485. |
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14.Chem. Mater., 201(342KB) | 期刊论文 | 作者接受稿 | 开放获取 | CC BY-NC-SA | View Application Full Text |
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