A hybrid DNA-templated gold nanocluster for enhanced enzymatic reduction of oxygen
Abstract
We report the synthesis and characterization of a new DNA-templated gold nanocluster (AuNC) of ~1 nm in diameter and possessing ~7 Au atoms. When integrated with bilirubin oxidase (BOD) and single walled carbon nanotubes (SWNTs), the AuNC acts as an enhancer of electron transfer (ET) and lowers the overpotential of electrocatalytic oxygen reduction reaction (ORR) by ~15 mV as compared to the enzyme alone. In addition, the presence of AuNC causes significant enhancements in the electrocatalytic current densities at the electrode. Control experiments show that such enhancement of ORR by the AuNC is specific to nanoclusters and not to plasmonic gold particles. Rotating ring disk electrode (RRDE) measurements confirm 4e– reduction of O2 to H2O with minimal production of H2O2, suggesting that the presence of AuNC does not perturb the mechanism of ORR catalyzed by the enzyme. This unique role of the AuNC as enhancer of ET at the enzyme-electrode interface makes it a potential candidate for the development of cathodes in enzymatic fuel cells, which often suffer from poor electronic communication between the electrode surface and the enzyme active site. In conclusion, the AuNC displays phosphorescence with large Stokes shift and microsecond lifetime.
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- The Univ. of New Mexico, Albuquerque, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1227636
- Report Number(s):
- LA-UR-15-23188
Journal ID: ISSN 0002-7863
- Grant/Contract Number:
- FA9550-12-1-0112; W911NF-14-1-0263; AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 137; Journal Issue: 36; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 59 BASIC BIOLOGICAL SCIENCES; 32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY
Citation Formats
Chakraborty, Saumen, Babanova, Sofia, Rocha, Reginaldo C., Desireddy, Anil, Artyushkova, Kateryna, Boncella, Amy E., Atanassov, Plamen, and Martinez, Jennifer S. A hybrid DNA-templated gold nanocluster for enhanced enzymatic reduction of oxygen. United States: N. p., 2015.
Web. doi:10.1021/jacs.5b05338.
Chakraborty, Saumen, Babanova, Sofia, Rocha, Reginaldo C., Desireddy, Anil, Artyushkova, Kateryna, Boncella, Amy E., Atanassov, Plamen, & Martinez, Jennifer S. A hybrid DNA-templated gold nanocluster for enhanced enzymatic reduction of oxygen. United States. https://doi.org/10.1021/jacs.5b05338
Chakraborty, Saumen, Babanova, Sofia, Rocha, Reginaldo C., Desireddy, Anil, Artyushkova, Kateryna, Boncella, Amy E., Atanassov, Plamen, and Martinez, Jennifer S. Wed .
"A hybrid DNA-templated gold nanocluster for enhanced enzymatic reduction of oxygen". United States. https://doi.org/10.1021/jacs.5b05338. https://www.osti.gov/servlets/purl/1227636.
@article{osti_1227636,
title = {A hybrid DNA-templated gold nanocluster for enhanced enzymatic reduction of oxygen},
author = {Chakraborty, Saumen and Babanova, Sofia and Rocha, Reginaldo C. and Desireddy, Anil and Artyushkova, Kateryna and Boncella, Amy E. and Atanassov, Plamen and Martinez, Jennifer S.},
abstractNote = {We report the synthesis and characterization of a new DNA-templated gold nanocluster (AuNC) of ~1 nm in diameter and possessing ~7 Au atoms. When integrated with bilirubin oxidase (BOD) and single walled carbon nanotubes (SWNTs), the AuNC acts as an enhancer of electron transfer (ET) and lowers the overpotential of electrocatalytic oxygen reduction reaction (ORR) by ~15 mV as compared to the enzyme alone. In addition, the presence of AuNC causes significant enhancements in the electrocatalytic current densities at the electrode. Control experiments show that such enhancement of ORR by the AuNC is specific to nanoclusters and not to plasmonic gold particles. Rotating ring disk electrode (RRDE) measurements confirm 4e– reduction of O2 to H2O with minimal production of H2O2, suggesting that the presence of AuNC does not perturb the mechanism of ORR catalyzed by the enzyme. This unique role of the AuNC as enhancer of ET at the enzyme-electrode interface makes it a potential candidate for the development of cathodes in enzymatic fuel cells, which often suffer from poor electronic communication between the electrode surface and the enzyme active site. In conclusion, the AuNC displays phosphorescence with large Stokes shift and microsecond lifetime.},
doi = {10.1021/jacs.5b05338},
journal = {Journal of the American Chemical Society},
number = 36,
volume = 137,
place = {United States},
year = {Wed Aug 19 00:00:00 EDT 2015},
month = {Wed Aug 19 00:00:00 EDT 2015}
}
Web of Science
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