Molecular Containers Derived from [60]Fullerene through Peroxide Chemistry
文献类型：期刊论文
| 作者 | Gan, Liangbing1,2 |
| 刊名 | ACCOUNTS OF CHEMICAL RESEARCH
 |
| 出版日期 | 2019-07-01 |
| 卷号 | 52期号:7页码:1793-1801 |
| ISSN号 | 0001-4842 |
| DOI | 10.1021/acs.accounts.9b00212 |
| 通讯作者 | Gan, Liangbing(gan@pku.edu.cn) |
| 英文摘要 | CONSPECTUS: Molecular containers can keep guest molecules in a confined space that is completely separated from the solution. They have wide potential applications, including selective trapping of reactive intermediates, catalysis within the cavity, and molecular delivery. Numerous molecular containers have been prepared through covalent bonds, metal-ligand interactions and H-bonding or hydrophobic interactions. Fullerenes are all-carbon molecules with a spherical structure. Partial opening of the cage structure results in open-cage fullerenes, which can serve as molecular containers for various small molecules and atoms. Compared with classical molecular containers, open-cage fullerenes exhibit some unusual phenomena because of the unique structure of the fullerene cage. The synthesis of an open-cage fullerene with a large enough orifice as a molecular container requires consecutive cleavage of multiple fullerene skeleton bonds within a local area on the cage surface. In spite of the difficulty, remarkable progress has been achieved. Several reactions have been reported to cleave fullerene C-C bonds selectively to form open-cage fullerenes, some of which have been successfully used as molecular containers for molecules such as H2O. The size and shape of the orifice play a key role in the encapsulation of the guest molecule. To date the focus in this area has been the preparation of open-cage fullerenes and encapsulation of small molecules. Little information has been reported about the functional properties of these host-guest systems. Potential applications of these systems need to be explored. This Account mainly presents our results on the encapsulation of small molecules in open-cage fullerenes prepared in my group. The preparation of our open-cage fullerenes is based on fullerene-mixed peroxides, which are briefly mentioned herein. The encapsulation and release of a single molecule of water is discussed in detail. Quantitative water encapsulation was achieved by heating the open-cage fullerene in a homogeneous CDCl3/H2O/EtOH mixture at 80 degrees C for 18 h. The kinetics of the water release process was studied by blackbody IR radiation-induced dissociation (BIRD) and theoretical calculations. The trapped water could also be released by H-bonding with HF. To control the encapsulation and release processes, we prepared open-cage fullerenes with a switchable stopper on the rim of the orifice. Besides H2O, encapsulations of H-2, HF, CO, O-2, and H2O2 were also achieved by using different open-cage fullerenes. The encapsulation of CO is quite unusual in that the trapped CO is derived from a fullerene skeleton carbon that was pushed into the cavity by oxidation under ambient conditions at room temperature. The trapped O-2/H2O2 could be released slowly under mild conditions, and these systems are now being studied as a new type of oxygen-releasing materials for biomedical research. The present results demonstrate that open-cage fullerenes are suitable molecular containers for small molecules. Our future work will focus on optimizing the conditions for the preparation of open-cage fullerenes and applications of open-cage fullerenes in areas such as oxygen delivery for photodynamic therapy. |
| WOS关键词 | OPEN-CAGE FULLERENE ; X-RAY STRUCTURES ; HYDROGEN-CYANIDE ; MIXED PEROXIDES ; OXYGEN DELIVERY ; SKELETON BONDS ; WATER ; DERIVATIVES ; C-60 ; ENCAPSULATION |
| 资助项目 | National Natural Science Foundation of China[21672009] ; National Natural Science Foundation of China[21871015] ; MOST[2015CB856600] |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:000476568400006 |
| 出版者 | AMER CHEMICAL SOC |
| 资助机构 | National Natural Science Foundation of China ; National Natural Science Foundation of China ; MOST ; MOST ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; MOST ; MOST ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; MOST ; MOST ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; MOST ; MOST |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/173910]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 通讯作者 | Gan, Liangbing |
| 作者单位 | 1.Peking Univ, Key Lab Bioorgan Chem & Mol Engn, Beijing Natl Lab Mol Sci, Minist Educ,Coll Chem & Mol Engn, Beijing 100871, Peoples R China 2.Shanghai Inst Organ Chem, State Key Lab Organometall Chem, Shanghai 200032, Peoples R China |
| 推荐引用方式 GB/T 7714 | Gan, Liangbing. Molecular Containers Derived from [60]Fullerene through Peroxide Chemistry[J]. ACCOUNTS OF CHEMICAL RESEARCH,2019,52(7):1793-1801. |
| APA | Gan, Liangbing.(2019).Molecular Containers Derived from [60]Fullerene through Peroxide Chemistry.ACCOUNTS OF CHEMICAL RESEARCH,52(7),1793-1801. |
| MLA | Gan, Liangbing."Molecular Containers Derived from [60]Fullerene through Peroxide Chemistry".ACCOUNTS OF CHEMICAL RESEARCH 52.7(2019):1793-1801. |
入库方式： OAI收割
来源：大连化学物理研究所
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