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学科主题: 物理化学
题名: Tuning the redox activity of encapsulated metal clusters via the metallic and semiconducting character of carbon nanotubes
作者: Zhang, Fan1;  Pan, Xiulian1;  Hu, Yongfeng2;  Yu, Liang1;  Chen, Xiaoqi1;  Jiang, Peng1;  Zhang, Hongbo1;  Deng, Shibin1, 3;  Zhang, Jin3;  Bolin, Trudy B.4;  Zhang, Shuo5;  Huang, Yuying5;  Bao, Xinhe1
通讯作者: 潘秀莲 ;  包信和
关键词: confined catalysis ;  confinement effect
刊名: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
发表日期: 2013-09-10
DOI: 10.1073/pnas.1306784110
卷: 110, 期:37, 页:14861-14866
收录类别: SCI
合作性质: 
文章类型: Article
部门归属: 5
项目归属: 502
产权排名: 待补充
WOS标题词: Science & Technology
类目[WOS]: Multidisciplinary Sciences
资助者: 1,1
研究领域[WOS]: Science & Technology - Other Topics
英文摘要: We demonstrate that reactions confined within single-walled carbon nanotube (SWCNT) channels are modulated by the metallic and semiconducting character of the hosts. In situ Raman and X-ray absorption near-edge structure spectroscopies provide complementary information about the electronic state of carbon nanotubes and the encapsulated rhenium species, which reveal electronic interactions between encapsulated species and nanotubes. More electrons are transferred from metallic tubes (m-SWCNTs) to oxidic rhenium clusters, leading to a lower valence state rhenium oxide than that in semiconducting tubes (s-SWCNTs). Reduction in 3.5% (vol/vol) H-2/Ar leads to weakened host-guest electronic interaction. The high valence state Re within s-SWCNTs is more readily reduced when raising the temperature, whereas only a sluggish change is observed for Re within m-SWCNTs. Only at 400 degrees C does Re reach a similar electronic state (mixture of Re-0 and Re4+) in both types of tubes. Subsequent oxidation in 1% O-2/Ar does not show changes for Re in s-SWCNTs up to 200 degrees C. In comparison, m-SWCNTs facilitate the oxidation of reduced rhenium (160 degrees C). This can be exploited for rational design of active catalysts with stable species as a desired valence state can be obtained by selecting specific-type SWCNTs and a controlled thermal treatment. These results also provide a chemical approach to modulate reversibly the electronic structure of SWCNTs without damaging the sidewalls of SWCNTs.
关键词[WOS]: RAMAN-SPECTROSCOPY ;  CHARGE-TRANSFER ;  IN-SITU ;  OLEFIN METATHESIS ;  ATOMIC-SCALE ;  CATALYSIS ;  FUNCTIONALIZATION ;  CONFINEMENT ;  OXIDATION ;  DIAMETER
语种: 英语
原文出处: 查看原文
WOS记录号: WOS:000324125100024
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/119667
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
2.Canadian Light Source Inc, Saskatoon, SK S7N 2V3, Canada
3.Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
4.Argonne Natl Lab, Adv Photon Source, Argonne, IL 60439 USA
5.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China

Recommended Citation:
Zhang, Fan,Pan, Xiulian,Hu, Yongfeng,et al. Tuning the redox activity of encapsulated metal clusters via the metallic and semiconducting character of carbon nanotubes[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2013,110(37):14861-14866.
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