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000007756 0247_ $$2DOI$$a10.1021/ja9083623
000007756 0247_ $$2WOS$$aWOS:000272207300042
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000007756 041__ $$aeng
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000007756 084__ $$2WoS$$aChemistry, Multidisciplinary
000007756 1001_ $$0P:(DE-HGF)0$$aAllen, B..$$b0
000007756 245__ $$aMechanistic Investigations of Horseradish Peroxidase-Catalyzed Degradation of Single-Walled Carbon Nanotubes
000007756 260__ $$aWashington, DC$$bAmerican Chemical Society$$c2009
000007756 300__ $$a17194 - 17205
000007756 3367_ $$0PUB:(DE-HGF)16$$2PUB:(DE-HGF)$$aJournal Article
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000007756 3367_ $$2BibTeX$$aARTICLE
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000007756 440_0 $$08502$$aJournal of the American Chemical Society$$v131$$x0002-7863$$y47
000007756 500__ $$aThis work was supported by AFOSR, Grant no. FA 9550-09-1-0478; NIOSH OH008282 and the 7th Framework Programme of the European Commission (NANOMMUNE).
000007756 520__ $$aSingle-walled carbon nanotubes (SWNTs) have been investigated for a variety of applications including composite materials, electronics, and drug delivery. However, these applications may be compromised depending on the negative effects of SWNTs to living systems. While reports of toxicity induced by SWNTs vary, means to alleviate or quell these effects are in small abundance. We have reported recently the degradation of carboxylated SWNTs through enzymatic catalysis with horseradish peroxidase (HRP). In this full Article, we investigated the degradation of both carboxylated and pristine SWNTs with HRP and compared these results with chemical degradation by hemin and FeCl(3). The interaction between pristine and carboxylated SWNTs with HRP was further studied by computer modeling, and the products of the enzymatic degradation were identified. By examining these factors with both pristine and carboxylated SWNTs through a variety of techniques including atomic force microscopy (AFM), transmission electron microscopy (TEM), Raman spectroscopy, ultraviolet-visible-near-infrared (UV-vis-NIR) spectroscopy, gas chromatography-mass spectrometry (GC-MS), high-performance liquid chromatography (HPLC), and liquid chromatography-mass spectrometry (LC-MS), degradation pathways were elucidated. It was observed that pristine SWNTs demonstrate no degradation with HRP incubation but display significant degradation when incubated with either hemin or FeCl(3). Such data signify a heterolytic cleavage of H(2)O(2) with HRP as pristine nanotubes do not degrade, whereas Fenton catalysis results in the homolytic cleavage of H(2)O(2) producing free radicals that oxidize pristine SWNTs. Product analysis shows complete degradation produces CO(2) gas. Conversely, incomplete degradation results in the formation of different oxidized aromatic hydrocarbons.
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000007756 650_2 $$2MeSH$$aBiocatalysis
000007756 650_2 $$2MeSH$$aHorseradish Peroxidase: metabolism
000007756 650_2 $$2MeSH$$aMicroscopy, Atomic Force
000007756 650_2 $$2MeSH$$aMicroscopy, Electron, Transmission
000007756 650_2 $$2MeSH$$aNanotubes, Carbon
000007756 650_2 $$2MeSH$$aSpectrum Analysis: methods
000007756 650_7 $$00$$2NLM Chemicals$$aNanotubes, Carbon
000007756 650_7 $$0EC 1.11.1.-$$2NLM Chemicals$$aHorseradish Peroxidase
000007756 650_7 $$2WoSType$$aJ
000007756 7001_ $$0P:(DE-HGF)0$$aKotchey, G.$$b1
000007756 7001_ $$0P:(DE-HGF)0$$aChen, Y.$$b2
000007756 7001_ $$0P:(DE-HGF)0$$aYanamala, N.$$b3
000007756 7001_ $$0P:(DE-Juel1)VDB44599$$aKlein-Seetharaman, J.$$b4$$uFZJ
000007756 7001_ $$0P:(DE-HGF)0$$aKagan, V.$$b5
000007756 7001_ $$0P:(DE-HGF)0$$aStar, A.$$b6
000007756 773__ $$0PERI:(DE-600)1472210-0$$a10.1021/ja9083623$$gVol. 131, p. 17194 - 17205$$p17194 - 17205$$q131<17194 - 17205$$tJournal of the American Chemical Society$$v131$$x0002-7863$$y2009
000007756 8567_ $$uhttp://dx.doi.org/10.1021/ja9083623
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000007756 9201_ $$0I:(DE-Juel1)ISB-2-20090406$$d31.12.2010$$gISB$$kISB-2$$lMolekulare Biophysik$$x0
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