Catalytic Oxidation of Cyclohexane on Small Silver Clusters Supported by Graphene Oxide | |
Anumula, Rajini; Cui, Chaonan; Yang, Mengzhou; Li, Jie; Luo, Zhixun | |
刊名 | JOURNAL OF PHYSICAL CHEMISTRY C |
2019-09-05 | |
卷号 | 123期号:35页码:21504-21512 |
ISSN号 | 1932-7447 |
英文摘要 | Metal clusters including those supported on graphene-based materials have attracted extensive research interest in the past decade allowing dissection of the interfaces, stability, electronic properties, and catalytic activities at an atomically precise scale. Here, we have synthesized glutathione-protected Ag-6 clusters via a facile green reaction route, transferred onto graphene oxide (GO) and exploit as catalyst for cyclohexane oxidation under ambient conditions. High selectivity and high yields to produce cyclohexanone are attained with tert-butyl hydroperoxide (TBHP) as the oxidant in the oxygen-flowing atmosphere. Based on density functional theory calculations, it is demonstrated that both TBHP and oxygen interact with the GO-supported Ag-6 clusters, giving rise to the peroxide structure and hence facilitating the catalytic oxidation of cyclohexane. It is interestingly found that the hydrogen-added hydroperoxyl (-OOH) brings forth largely decreased activation barrier for the O-O bond dissociation. The O-O dissociated intermediate then reacts with cyclohexane to form cyclohexanol, followed by successive oxidative dehydrogenation to produce cyclohexanone. This finding verifies the enhanced catalysis of TBHP and O-2 for the conversion of cyclohexane to cyclohexanone and helps to develop heterogeneous catalysts of metal clusters for efficient C-H activation. |
内容类型 | 期刊论文 |
源URL | [http://ir.rcees.ac.cn/handle/311016/42624] |
专题 | 生态环境研究中心_环境水质学国家重点实验室 |
作者单位 | 1.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Beijing 100085, Peoples R China 2.Chinese Acad Sci, State Key Lab Struct Chem Unstable & Stable Speci, Lab Photochem, Inst Chem, Beijing 100190, Peoples R China 3.Univ Chinese Acad Sci, Beijing 100049, Peoples R China |
推荐引用方式 GB/T 7714 | Anumula, Rajini,Cui, Chaonan,Yang, Mengzhou,et al. Catalytic Oxidation of Cyclohexane on Small Silver Clusters Supported by Graphene Oxide[J]. JOURNAL OF PHYSICAL CHEMISTRY C,2019,123(35):21504-21512. |
APA | Anumula, Rajini,Cui, Chaonan,Yang, Mengzhou,Li, Jie,&Luo, Zhixun.(2019).Catalytic Oxidation of Cyclohexane on Small Silver Clusters Supported by Graphene Oxide.JOURNAL OF PHYSICAL CHEMISTRY C,123(35),21504-21512. |
MLA | Anumula, Rajini,et al."Catalytic Oxidation of Cyclohexane on Small Silver Clusters Supported by Graphene Oxide".JOURNAL OF PHYSICAL CHEMISTRY C 123.35(2019):21504-21512. |
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