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Tuning the redox activity of encapsulated metal clusters via the metallic and semiconducting character of carbon nanotubes

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... Full description

Journal Title: Proceedings of the National Academy of Sciences 10 September 2013, Vol.110(37), p.14861
Main Author: Fan Zhang
Other Authors: Xiulian Pan , Yongfeng Hu , Liang Yu , Xiaoqi Chen , Peng Jiang , Hongbo Zhang , Shibin Deng , Jin Zhang , Trudy B. Bolin , Shuo Zhang , Yuying Huang , Xinhe Bao
Format: Electronic Article Electronic Article
Language: English
Subjects:
ID: ISSN: 0027-8424 ; E-ISSN: 1091-6490 ; DOI: 10.1073/pnas.1306784110
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recordid: pnas_s110_37_14861
title: Tuning the redox activity of encapsulated metal clusters via the metallic and semiconducting character of carbon nanotubes
format: Article
creator:
  • Fan Zhang
  • Xiulian Pan
  • Yongfeng Hu
  • Liang Yu
  • Xiaoqi Chen
  • Peng Jiang
  • Hongbo Zhang
  • Shibin Deng
  • Jin Zhang
  • Trudy B. Bolin
  • Shuo Zhang
  • Yuying Huang
  • Xinhe Bao
subjects:
  • Sciences (General)
ispartof: Proceedings of the National Academy of Sciences, 10 September 2013, Vol.110(37), p.14861
description: 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.sub.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.sup.0] and [Re.sup.4+]) in both types of tubes. Subsequent oxidation in 1% [O.sub.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. confined catalysis | confinement effect www.pnas.org/cgi/doi/10.1073/pnas.1306784110
language: eng
source:
identifier: ISSN: 0027-8424 ; E-ISSN: 1091-6490 ; DOI: 10.1073/pnas.1306784110
fulltext: fulltext_linktorsrc
issn:
  • 0027-8424
  • 00278424
  • 1091-6490
  • 10916490
url: Link


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titleTuning the redox activity of encapsulated metal clusters via the metallic and semiconducting character of carbon nanotubes
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descriptionWe 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.sub.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.sup.0] and [Re.sup.4+]) in both types of tubes. Subsequent oxidation in 1% [O.sub.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. confined catalysis | confinement effect www.pnas.org/cgi/doi/10.1073/pnas.1306784110
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