Mechanistic Investigations of Horseradish Peroxidase-Catalyzed Degradation of Single-Walled Carbon Nanotubes

Details

• Personal Author:
  Allen BL ; Chen Y ; Kagan VE ; Klein-Seetharaman J ; Kotchey GP ; Star A ; Yanamala NV
• Description:
  Single-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. [Description provided by NIOSH]
• Subjects:
  Biochemistry Chemistry Chemistry, Analytic Chromatography Enzymes Hazardous Substances Occupational Health Safety Spectrum Analysis
• Keywords:
  Analytical-chemistry Biochemical-tests Biological-effects Chromatographic-analysis Enzymatic-effects Microscopy Nanoparticles Nanotechnology Nanotubes Peroxidases Spectrographic-analysis Toxic-effects

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• ISSN:
  0002-7863
• Document Type:
  Text
• Funding:
  Grant
• Genre:
  Journal Article
• Place as Subject:
  OSHA Region 3 ; Pennsylvania
• CIO:
  National Institute for Occupational Safety and Health (NIOSH)
• Topic:
  Workplace Safety & Health
• Location:
  North America
• Volume:
  131
• Issue:
  47
• NIOSHTIC Number:
  nn:20036298
• Citation:
  J Am Chem Soc 2009 Dec; 131(47):17194-17205
• Contact Point Address:
  University of Pittsburgh, Department of Chemistry, Chevron Science Center, 219 Parkman Avenue, Pittsburgh, PA 15260
• Email:
  astar@pitt.edu
• Federal Fiscal Year:
  2010
• NORA Priority Area:
  Manufacturing
• Performing Organization:
  University of Pittsburgh at Pittsburgh
• Peer Reviewed:
  True
• Start Date:
  20050701
• Source Full Name:
  Journal of the American Chemical Society
• End Date:
  20160630
• Collection(s):
  National Institute for Occupational Safety and Health
• Main Document Checksum:
  urn:sha-512:878928131a82325846fc54a2c662c43c06afdae99fd59c948863a1b291546e56067a053a1bc4a429cf679a40c25fd0aa8c283288d3e1a95304c7b817c7cc890e
• Download URL:
  https://stacks.cdc.gov/view/cdc/187778/cdc_187778_DS1.pdf
• File Type:
  [PDF - 4.66 MB ]