Raman spectroscopy of charge transfer interactions between single wall carbon nanotubes and [FeFe] hydrogenase

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We report a Raman spectroscopy study of charge transfer interactions in complexes formed by single-walled carbon nanotubes (SWNTs) and [FeFe] hydrogenase I (CaHydl) from clostridium acetobutylicum. The choice of Raman excitation wavelength and sample preparation conditions allows differences to be observed for complexes involving metallic (m) and semiconducting (s) species. Adsorbed CaHydl can reversibly inject electronic charge into the LUMOs of s-SWNTs, while charge can be injected and removed from m-SWNTs at lower potentials just above the Fermi energy. Time-dependent enzymatic assays demonstrated that the reduced and oxidized forms of CaHydl are deactivated by oxygen, but at rates that varied by an order of magnitude. The time evolution of the oxidative decay of the CaHydl activity reveals different time constants when complexed with m-SWNTs and s-SWNTs. The correlation of enzymatic assays with time-dependent Raman spectroscopy provides a novel method by which the charge transfer interactions may be investigated in the various SwNT. CaHydl complexes. Surprisingly, an oxidized form of CaHydl is apparently more resistant to oxygen deactivation when complexed to m-SWNTs rather than s-SWNTs.
Publisher
ROYAL SOC CHEMISTRY
Issue Date
2008-10
Language
English
Article Type
Article
Keywords

DESULFOVIBRIO-DESULFURICANS; ELECTRONIC-STRUCTURE; DISPERSIONS; PROTONATION; RESONANCE; OXIDATION

Citation

DALTON TRANSACTIONS, pp.5454 - 5461

ISSN
1477-9226
DOI
10.1039/b806379f
URI
http://hdl.handle.net/10203/90704
Appears in Collection
NT-Journal Papers(저널논문)
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