Ultrasensitive detection of DNA in diluted serum using NaBH4 electrooxidation mediated by [Ru(NH3)6]3+ at indium-tin oxide electrodes

Jagotamoy Das; Jeong Ah Lee; Haesik Yang

doi:10.1021/la904089e

Ultrasensitive detection of DNA in diluted serum using NaBH₄ electrooxidation mediated by [Ru(NH₃)₆]³⁺ at indium-tin oxide electrodes

Jagotamoy Das, Jeong Ah Lee, Haesik Yang^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

21 Scopus citations

Abstract

There is a crucial need for simple and highly sensitive techniques to detect DNA in complicated biological samples such as serum. Here we present an ultrasensitive electrochemical DNA sensor using (i) single DNA hybridization with peptide nucleic acid (PNA), (ii) selective binding of [Ru(NH ₃)₆]³⁺ to hybridized DNA, (iii) fast NaBH ₄ electrooxidation mediated by [Ru(NH₃)₆] ³⁺, and (iv) low background currents of NaBH₄ at indium-tin oxide (ITO) electrodes. The [Ru^III(NH₃) ₅NH₂]²⁺ formed from [Ru^III(NH ₃)₆]³⁺ in borate buffer (pH 11.0) is readily electrooxidized to both [Ru^IV(NH₃)₅NH ₂]³⁺ and Ru complex with a higher oxidation state. In the absence of [Ru(NH₃)₆]³⁺ bound to the DNA-sensing ITO electrodes, the oxidation currents of NaBH₄ are very low. However, in the presence of [Ru(NH₃)₆]³⁺, the oxidation currents of NaBH₄ are highly enhanced due to electron mediation of the oxidized Ru complexes. The significant enhancement in the electrocatalytic activity of sensing electrodes after [Ru(NH₃) ₆]³⁺ binding facilitates to obtain high signal-to-background ratios. PNA and ethylenediamine on DNA-sensing electrodes significantly decrease [Ru(NH₃)₆]³⁺ binding, also allowing for high signal-to-background ratios. The oxidation charges of NaBH₄ obtained from chronocoulometry are highly reproducible. All combined effects enable the detection of DNA with a detection limit of 1 fM in ten-fold diluted human serum. The simple and fast detection procedure and the ultrasensitivity make this approach highly promising for practical DNA detection.

Original language	English (US)
Pages (from-to)	6804-6808
Number of pages	5
Journal	Langmuir
Volume	26
Issue number	9
DOIs	https://doi.org/10.1021/la904089e
State	Published - May 4 2010
Externally published	Yes

ASJC Scopus subject areas

General Materials Science
Condensed Matter Physics
Surfaces and Interfaces
Spectroscopy
Electrochemistry

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10.1021/la904089e

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@article{f8f2c53937f74f618caafb3b8edafb02,

title = "Ultrasensitive detection of DNA in diluted serum using NaBH4 electrooxidation mediated by [Ru(NH3)6]3+ at indium-tin oxide electrodes",

abstract = "There is a crucial need for simple and highly sensitive techniques to detect DNA in complicated biological samples such as serum. Here we present an ultrasensitive electrochemical DNA sensor using (i) single DNA hybridization with peptide nucleic acid (PNA), (ii) selective binding of [Ru(NH 3)6]3+ to hybridized DNA, (iii) fast NaBH 4 electrooxidation mediated by [Ru(NH3)6] 3+, and (iv) low background currents of NaBH4 at indium-tin oxide (ITO) electrodes. The [RuIII(NH3) 5NH2]2+ formed from [RuIII(NH 3)6]3+ in borate buffer (pH 11.0) is readily electrooxidized to both [RuIV(NH3)5NH 2]3+ and Ru complex with a higher oxidation state. In the absence of [Ru(NH3)6]3+ bound to the DNA-sensing ITO electrodes, the oxidation currents of NaBH4 are very low. However, in the presence of [Ru(NH3)6]3+, the oxidation currents of NaBH4 are highly enhanced due to electron mediation of the oxidized Ru complexes. The significant enhancement in the electrocatalytic activity of sensing electrodes after [Ru(NH3) 6]3+ binding facilitates to obtain high signal-to-background ratios. PNA and ethylenediamine on DNA-sensing electrodes significantly decrease [Ru(NH3)6]3+ binding, also allowing for high signal-to-background ratios. The oxidation charges of NaBH4 obtained from chronocoulometry are highly reproducible. All combined effects enable the detection of DNA with a detection limit of 1 fM in ten-fold diluted human serum. The simple and fast detection procedure and the ultrasensitivity make this approach highly promising for practical DNA detection.",

author = "Jagotamoy Das and Lee, {Jeong Ah} and Haesik Yang",

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AU - Lee, Jeong Ah

AU - Yang, Haesik

PY - 2010/5/4

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N2 - There is a crucial need for simple and highly sensitive techniques to detect DNA in complicated biological samples such as serum. Here we present an ultrasensitive electrochemical DNA sensor using (i) single DNA hybridization with peptide nucleic acid (PNA), (ii) selective binding of [Ru(NH 3)6]3+ to hybridized DNA, (iii) fast NaBH 4 electrooxidation mediated by [Ru(NH3)6] 3+, and (iv) low background currents of NaBH4 at indium-tin oxide (ITO) electrodes. The [RuIII(NH3) 5NH2]2+ formed from [RuIII(NH 3)6]3+ in borate buffer (pH 11.0) is readily electrooxidized to both [RuIV(NH3)5NH 2]3+ and Ru complex with a higher oxidation state. In the absence of [Ru(NH3)6]3+ bound to the DNA-sensing ITO electrodes, the oxidation currents of NaBH4 are very low. However, in the presence of [Ru(NH3)6]3+, the oxidation currents of NaBH4 are highly enhanced due to electron mediation of the oxidized Ru complexes. The significant enhancement in the electrocatalytic activity of sensing electrodes after [Ru(NH3) 6]3+ binding facilitates to obtain high signal-to-background ratios. PNA and ethylenediamine on DNA-sensing electrodes significantly decrease [Ru(NH3)6]3+ binding, also allowing for high signal-to-background ratios. The oxidation charges of NaBH4 obtained from chronocoulometry are highly reproducible. All combined effects enable the detection of DNA with a detection limit of 1 fM in ten-fold diluted human serum. The simple and fast detection procedure and the ultrasensitivity make this approach highly promising for practical DNA detection.

AB - There is a crucial need for simple and highly sensitive techniques to detect DNA in complicated biological samples such as serum. Here we present an ultrasensitive electrochemical DNA sensor using (i) single DNA hybridization with peptide nucleic acid (PNA), (ii) selective binding of [Ru(NH 3)6]3+ to hybridized DNA, (iii) fast NaBH 4 electrooxidation mediated by [Ru(NH3)6] 3+, and (iv) low background currents of NaBH4 at indium-tin oxide (ITO) electrodes. The [RuIII(NH3) 5NH2]2+ formed from [RuIII(NH 3)6]3+ in borate buffer (pH 11.0) is readily electrooxidized to both [RuIV(NH3)5NH 2]3+ and Ru complex with a higher oxidation state. In the absence of [Ru(NH3)6]3+ bound to the DNA-sensing ITO electrodes, the oxidation currents of NaBH4 are very low. However, in the presence of [Ru(NH3)6]3+, the oxidation currents of NaBH4 are highly enhanced due to electron mediation of the oxidized Ru complexes. The significant enhancement in the electrocatalytic activity of sensing electrodes after [Ru(NH3) 6]3+ binding facilitates to obtain high signal-to-background ratios. PNA and ethylenediamine on DNA-sensing electrodes significantly decrease [Ru(NH3)6]3+ binding, also allowing for high signal-to-background ratios. The oxidation charges of NaBH4 obtained from chronocoulometry are highly reproducible. All combined effects enable the detection of DNA with a detection limit of 1 fM in ten-fold diluted human serum. The simple and fast detection procedure and the ultrasensitivity make this approach highly promising for practical DNA detection.

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Ultrasensitive detection of DNA in diluted serum using NaBH₄ electrooxidation mediated by [Ru(NH₃)₆]³⁺ at indium-tin oxide electrodes

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