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Manganese Peroxidase Degrades Pristine but Not Surface-Oxidized (Carboxylated) Single-Walled Carbon Nanotubes

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† College of Environmental Science and Engineering/Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria/Tianjin Key Laboratory of Environmental Remediation and Pollution Control, Nankai University, Tianjin 300071, People’s Republic of China
‡ Department of Civil and Environmental Engineering, Rice University, Houston, Texas 77005, United States
*Telephone: 86-22-6229517. E-mail: [email protected]
*Telephone: 713-348-5903 and/or 713-348-5203. E-mail: [email protected]
Cite this: Environ. Sci. Technol. 2014, 48, 14, 7918–7923
Publication Date (Web):June 20, 2014
https://doi.org/10.1021/es5011175
Copyright © 2014 American Chemical Society
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    Abstract

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    The transformation of engineered nanomaterials in the environment can significantly affect their transport, fate, bioavailability, and toxicity. Little is known about the biotransformation potential of single-walled carbon nanotubes (SWNTs). In this study, we compared the enzymatic transformation of SWNTs and oxidized (carboxylated) SWNTs (O-SWNTs) using three ligninolytic enzymes: lignin peroxidase, manganese peroxidase (MnP), and laccase. Only MnP was capable of transforming SWNTs, as determined by Raman spectroscopy, near-infrared spectroscopy, and transmission electron microscopy. Interestingly, MnP degraded SWNTs but not O-SWNTs. The recalcitrance of O-SWNTs to enzymatic transformation is likely attributable to the binding of Mn2+ by their surface carboxyl groups at the enzyme binding site, which inhibits critical steps in the MnP catalytic cycle (i.e., Mn2+ oxidation and Mn3+ dissociation from the enzyme). Our results suggest that oxygen-containing surface functionalities do not necessarily facilitate the biodegradation of carbonaceous nanomaterials, as is commonly assumed.

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    TEM images of the SWNTs and O-SWNTs (Figure S1), XPS plots of the C 1s and O 1s core levels of the SWNTs and O-SWNTs (Figure S2), TGA plots of the SWNTs and O-SWNTs (Figure S3), additional Raman spectra of MnP treatments in triplicate (Figure S4), activities of the three enzymes during the 16 days of incubation (Figure S5), and adsorption of Mn2+ by the SWNTs and O-SWNTs (Figure S6). This material is available free of charge via the Internet at http://pubs.acs.org.

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