DICP OpenIR
Subject Area物理化学
Tuning the redox activity of encapsulated metal clusters via the metallic and semiconducting character of carbon nanotubes
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; Pan XL(潘秀莲); Bao XH(包信和)
KeywordConfined Catalysis Confinement Effect
Source PublicationPROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
2013-09-10
DOI10.1073/pnas.1306784110
Volume110Issue:37Pages:14861-14866
Indexed BySCI
Cooperation Status
SubtypeArticle
Department5
Funding Project502
Contribution Rank待补充
WOS HeadingsScience & Technology
Funding Organization1,1 ; 1,1 ; 1,1 ; 1,1
WOS SubjectMultidisciplinary Sciences
WOS Research AreaScience & Technology - Other Topics
WOS KeywordRAMAN-SPECTROSCOPY ; CHARGE-TRANSFER ; IN-SITU ; OLEFIN METATHESIS ; ATOMIC-SCALE ; CATALYSIS ; FUNCTIONALIZATION ; CONFINEMENT ; OXIDATION ; DIAMETER
AbstractWe 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.
Language英语
Funding Organization1,1 ; 1,1 ; 1,1 ; 1,1
URL查看原文
WOS IDWOS:000324125100024
Citation statistics
Cited Times:37[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/119667
Collection中国科学院大连化学物理研究所
Corresponding AuthorPan XL(潘秀莲); Bao XH(包信和)
Affiliation1.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
GB/T 7714
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.
APA Zhang, Fan.,Pan, Xiulian.,Hu, Yongfeng.,Yu, Liang.,Chen, Xiaoqi.,...&包信和.(2013).Tuning the redox activity of encapsulated metal clusters via the metallic and semiconducting character of carbon nanotubes.PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,110(37),14861-14866.
MLA Zhang, Fan,et al."Tuning the redox activity of encapsulated metal clusters via the metallic and semiconducting character of carbon nanotubes".PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA 110.37(2013):14861-14866.
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