A hybrid DNA-templated gold nanocluster for enhanced enzymatic reduction of oxygen

Chakraborty, Saumen; Babanova, Sofia; Rocha, Reginaldo C.; Desireddy, Anil; Artyushkova, Kateryna; Boncella, Amy E.; Atanassov, Plamen; Martinez, Jennifer S.

doi:10.1021/jacs.5b05338

Title: A hybrid DNA-templated gold nanocluster for enhanced enzymatic reduction of oxygen

Journal Article · Wed Aug 19 00:00:00 EDT 2015 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b05338· OSTI ID:1227636

Chakraborty, Saumen ^[1]; Babanova, Sofia ^[2]; Rocha, Reginaldo C. ^[1]; Desireddy, Anil ^[1]; Artyushkova, Kateryna ^[2]; Boncella, Amy E. ^[1]; Atanassov, Plamen ^[2]; Martinez, Jennifer S. ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
The Univ. of New Mexico, Albuquerque, NM (United States)

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.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: FA9550-12-1-0112; W911NF-14-1-0263; AC52-06NA25396

OSTI ID:: 1227636

Report Number(s):: LA-UR-15-23188

Journal Information:: Journal of the American Chemical Society, Vol. 137, Issue 36; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 110 works

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Preparation and Photoluminescent Properties of Gold(I)−Alkanethiolate Complexes Having Highly Ordered Supramolecular Structures Cha, Sang-Ho; Kim, Jong-Uk; Kim, Ki-Hyun Chemistry of Materials, Vol. 19, Issue 25 https://doi.org/10.1021/cm7024944	journal	December 2007
Enzyme-based biofuel cells Minteer, Shelley D.; Liaw, Bor Yann; Cooney, Michael J. Current Opinion in Biotechnology, Vol. 18, Issue 3 https://doi.org/10.1016/j.copbio.2007.03.007	journal	June 2007
Nanostructured materials for advanced energy conversion and storage devices Aricò, Antonino Salvatore; Bruce, Peter; Scrosati, Bruno Nature Materials, Vol. 4, Issue 5, p. 366-377 https://doi.org/10.1038/nmat1368	journal	May 2005
Synthesis of DNA-templated fluorescent gold nanoclusters Liu, Guiying; Shao, Yong; Ma, Kun Gold Bulletin, Vol. 45, Issue 2 https://doi.org/10.1007/s13404-012-0049-6	journal	May 2012
Implanted biofuel cells operating in vivo – methods, applications and perspectives – feature article Katz, Evgeny; MacVittie, Kevin Energy & Environmental Science, Vol. 6, Issue 10 https://doi.org/10.1039/c3ee42126k	journal	January 2013
Improving the Environment for Immobilized Dehydrogenase Enzymes by Modifying Nafion with Tetraalkylammonium Bromides Moore, Christine M.; Akers, Nick L.; Hill, Adam D. Biomacromolecules, Vol. 5, Issue 4 https://doi.org/10.1021/bm0345256	journal	July 2004
Synthesis, Characterization, and Bioconjugation of Fluorescent Gold Nanoclusters toward Biological Labeling Applications Lin, Cheng-An J.; Yang, Ting-Ya; Lee, Chih-Hsien ACS Nano, Vol. 3, Issue 2 https://doi.org/10.1021/nn800632j	journal	January 2009
Ag K-Edge EXAFS Analysis of DNA-Templated Fluorescent Silver Nanoclusters: Insight into the Structural Origins of Emission Tuning by DNA Sequence Variations Neidig, Michael L.; Sharma, Jaswinder; Yeh, Hsin-Chih Journal of the American Chemical Society, Vol. 133, Issue 31 https://doi.org/10.1021/ja202797w	journal	August 2011
Catalysis opportunities of atomically precise gold nanoclusters Zhu, Yan; Qian, Huifeng; Jin, Rongchao Journal of Materials Chemistry, Vol. 21, Issue 19 https://doi.org/10.1039/c1jm10082c	journal	January 2011
DNA-hosted fluorescent gold nanoclusters: sequence-dependent formation Liu, Guiying; Shao, Yong; Wu, Fei Nanotechnology, Vol. 24, Issue 1 https://doi.org/10.1088/0957-4484/24/1/015503	journal	December 2012
Experimental and Computational Investigation of Au ₂₅ Clusters and CO ₂ : A Unique Interaction and Enhanced Electrocatalytic Activity Kauffman, Douglas R.; Alfonso, Dominic; Matranga, Christopher Journal of the American Chemical Society, Vol. 134, Issue 24 https://doi.org/10.1021/ja303259q	journal	June 2012
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An overview on the current understanding of the photophysical properties of metal nanoclusters and their potential applications Maity, Subarna; Bain, Dipankar; Patra, Amitava Nanoscale, Vol. 11, Issue 47 https://doi.org/10.1039/c9nr07963g	journal	January 2019
Single Platform for Gene and Protein Expression Analyses Using Luminescent Gold Nanoclusters Sailapu, Sunil Kumar; Dutta, Deepanjalee; Sahoo, Amaresh Kumar ACS Omega, Vol. 3, Issue 2 https://doi.org/10.1021/acsomega.7b01739	journal	February 2018
Kojic acid capped gold nanoclusters with aggregation-induced emission for fluorometric screening of the activity of alkaline phosphatase Li, Yuanyuan; Du, Qianqian; Zhang, Xiaodan Microchimica Acta, Vol. 186, Issue 8 https://doi.org/10.1007/s00604-019-3681-5	journal	July 2019

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