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

	Tuning the redox activity of encapsulated metal clusters via the metallic and semiconducting character of carbon nanotubes
	Zhang, Fan 1; Pan, Xiulian 1; Hu, Yongfeng 2; Yu, Liang 1; Chen, Xiaoqi 1; Jiang, Peng 1; Zhang, Hongbo 1; Deng, Shibin 1,3; Zhang, Jin 3; Bolin, Trudy B.4
刊名	proceedings of the national academy of sciences of the united states of america
	2013-09-10
卷号	110 期号:37 页码:14861-14866
关键词	confined catalysis confinement effect
通讯作者	潘秀莲 ; 包信和
产权排序	待补充
合作状况	英
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.
学科主题	物理化学
WOS标题词	science & technology
类目[WOS]	multidisciplinary sciences
研究领域[WOS]	science & technology - other topics
关键词[WOS]	raman-spectroscopy ; charge-transfer ; in-situ ; olefin metathesis ; atomic-scale ; catalysis ; functionalization ; confinement ; oxidation ; diameter
收录类别	SCI
资助信息	1，1
原文出处	14866
语种	英语
WOS记录号	WOS:000324125100024
公开日期	2014-09-11
内容类型	期刊论文
源URL	[http://159.226.238.44/handle/321008/119667]
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
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
推荐引用方式 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.,...&Bao, Xinhe.(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.