Sensitive Chronocoulometric Detection of miRNA at Screen printed Electrodes modified by gold decorated MoS2 Nanosheets

Research output: Contribution to journalArticle

Abstract

Developing novel simple and ultrasensitive strategies for detecting microRNAs
(miRNAs) is highly desirable because of their association with early cancer diagnostic and prognostic processes. Here a new chronocoulometric sensor, based on semiconducting 2H MoS2 nanosheets (MoS2 NSs) decorated with a controlled density of monodispersed small gold nanoparticles (AuNPs@MoS2), was fabricated via electrodeposition, for the highly sensitive detection of miRNA-21. The size and interparticle spacing of AuNPs was optimized by
controlling nucleation and growth rates through tuning of deposition-potential and Au-precursor concentration and by getting simultaneous feedback from morphological and electrochemical activity studies. The sensing strategy, involved the selective immobilization of thiolated capture probe DNA (CP) at AuNPs and hybridization of CP to a part of miRNA target, whereas the
remaining part of the target was complementary to a signaling non-labelled DNA sequence that served to amplify the target upon hybridization. Chronocoulometry provided precise quantification of nucleic acids at each step of the sensor assay by interrogating [Ru(NH3)6]3+ electrostatically bound to phosphate backbones of oligonucleotides. A detailed and systematic optimization study demonstrated that the thinnest and smallest MoS2 NSs improved the sensitivity of the AuNP@MoS2 sensor achieving an impressive detection limit of ≈100 aM, which is 2 orders of magnitude lower than that of bare Au electrode and also enhanced the DNA miRNA hybridization efficiency by 25%. Such improved performance can be attributed to the controlled packing density of CPs achieved by their self -assembly on AuNPs, large interparticle density, small size and the intimate coupling between AuNPs and MoS2. Alongside the outstanding sensitivity, the sensor exhibited excellent selectivity down to femtomolar concentrations, for discriminating complementary miRNA-21 target in a complex system composed of different foreign targets including mismatched and non-complementary miRNA-155. These advantages make our sensor a promising contender in the point of care miRNA sensor family for medical diagnostics
LanguageEnglish
Article numberDOI: 10.1021/acsabm.8b00398
Pages1184-1194
Number of pages10
JournalACS Applied Bio Materials
Volume1
Issue number4
DOIs
Publication statusPublished - 10 Sep 2018

Fingerprint

Nanosheets
MicroRNAs
Gold
Electrodes
Sensors
DNA Probes
DNA sequences
Electrodeposition
Oligonucleotides
Self assembly
Nucleic Acids
Large scale systems
Assays
Nucleation
Tuning
Phosphates
Association reactions
Nanoparticles
Feedback
DNA

Keywords

  • Molybdenum disulfide (MoS2) Nanosheets
  • Ionic Liquid Assisted Grinding Exfoliation
  • Gold Decorated MoS2 Hybrid Nanosheets
  • Electrochemical microRNA-sensor
  • Chronocoulometric Detection
  • microRNA-21 (miRNA-21)
  • Electrochemical Deposition
  • Screen-Printed Gold Electrodes
  • 2D Materials
  • 2 Dimensional Materials

Cite this

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title = "Sensitive Chronocoulometric Detection of miRNA at Screen printed Electrodes modified by gold decorated MoS2 Nanosheets",
abstract = "Developing novel simple and ultrasensitive strategies for detecting microRNAs (miRNAs) is highly desirable because of their association with early cancer diagnostic and prognostic processes. Here a new chronocoulometric sensor, based on semiconducting 2H MoS2 nanosheets (MoS2 NSs) decorated with a controlled density of monodispersed small gold nanoparticles (AuNPs@MoS2), was fabricated via electrodeposition, for the highly sensitive detection of miRNA-21. The size and interparticle spacing of AuNPs was optimized by controlling nucleation and growth rates through tuning of deposition-potential and Au-precursor concentration and by getting simultaneous feedback from morphological and electrochemical activity studies. The sensing strategy, involved the selective immobilization of thiolated capture probe DNA (CP) at AuNPs and hybridization of CP to a part of miRNA target, whereas the remaining part of the target was complementary to a signaling non-labelled DNA sequence that served to amplify the target upon hybridization. Chronocoulometry provided precise quantification of nucleic acids at each step of the sensor assay by interrogating [Ru(NH3)6]3+ electrostatically bound to phosphate backbones of oligonucleotides. A detailed and systematic optimization study demonstrated that the thinnest and smallest MoS2 NSs improved the sensitivity of the AuNP@MoS2 sensor achieving an impressive detection limit of ≈100 aM, which is 2 orders of magnitude lower than that of bare Au electrode and also enhanced the DNA miRNA hybridization efficiency by 25{\%}. Such improved performance can be attributed to the controlled packing density of CPs achieved by their self -assembly on AuNPs, large interparticle density, small size and the intimate coupling between AuNPs and MoS2. Alongside the outstanding sensitivity, the sensor exhibited excellent selectivity down to femtomolar concentrations, for discriminating complementary miRNA-21 target in a complex system composed of different foreign targets including mismatched and non-complementary miRNA-155. These advantages make our sensor a promising contender in the point of care miRNA sensor family for medical diagnostics",
keywords = "Molybdenum disulfide (MoS2) Nanosheets , Ionic Liquid Assisted Grinding Exfoliation , Gold Decorated MoS2 Hybrid Nanosheets , Electrochemical microRNA-sensor, Chronocoulometric Detection , microRNA-21 (miRNA-21), Electrochemical Deposition, Screen-Printed Gold Electrodes, 2D Materials, 2 Dimensional Materials",
author = "Abhijit Ganguly and John Benson and P Papakonstantinou",
year = "2018",
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Sensitive Chronocoulometric Detection of miRNA at Screen printed Electrodes modified by gold decorated MoS2 Nanosheets. / Ganguly, Abhijit; Benson, John; Papakonstantinou, P.

Vol. 1, No. 4, DOI: 10.1021/acsabm.8b00398, 10.09.2018, p. 1184-1194.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Sensitive Chronocoulometric Detection of miRNA at Screen printed Electrodes modified by gold decorated MoS2 Nanosheets

AU - Ganguly, Abhijit

AU - Benson, John

AU - Papakonstantinou, P

PY - 2018/9/10

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N2 - Developing novel simple and ultrasensitive strategies for detecting microRNAs (miRNAs) is highly desirable because of their association with early cancer diagnostic and prognostic processes. Here a new chronocoulometric sensor, based on semiconducting 2H MoS2 nanosheets (MoS2 NSs) decorated with a controlled density of monodispersed small gold nanoparticles (AuNPs@MoS2), was fabricated via electrodeposition, for the highly sensitive detection of miRNA-21. The size and interparticle spacing of AuNPs was optimized by controlling nucleation and growth rates through tuning of deposition-potential and Au-precursor concentration and by getting simultaneous feedback from morphological and electrochemical activity studies. The sensing strategy, involved the selective immobilization of thiolated capture probe DNA (CP) at AuNPs and hybridization of CP to a part of miRNA target, whereas the remaining part of the target was complementary to a signaling non-labelled DNA sequence that served to amplify the target upon hybridization. Chronocoulometry provided precise quantification of nucleic acids at each step of the sensor assay by interrogating [Ru(NH3)6]3+ electrostatically bound to phosphate backbones of oligonucleotides. A detailed and systematic optimization study demonstrated that the thinnest and smallest MoS2 NSs improved the sensitivity of the AuNP@MoS2 sensor achieving an impressive detection limit of ≈100 aM, which is 2 orders of magnitude lower than that of bare Au electrode and also enhanced the DNA miRNA hybridization efficiency by 25%. Such improved performance can be attributed to the controlled packing density of CPs achieved by their self -assembly on AuNPs, large interparticle density, small size and the intimate coupling between AuNPs and MoS2. Alongside the outstanding sensitivity, the sensor exhibited excellent selectivity down to femtomolar concentrations, for discriminating complementary miRNA-21 target in a complex system composed of different foreign targets including mismatched and non-complementary miRNA-155. These advantages make our sensor a promising contender in the point of care miRNA sensor family for medical diagnostics

AB - Developing novel simple and ultrasensitive strategies for detecting microRNAs (miRNAs) is highly desirable because of their association with early cancer diagnostic and prognostic processes. Here a new chronocoulometric sensor, based on semiconducting 2H MoS2 nanosheets (MoS2 NSs) decorated with a controlled density of monodispersed small gold nanoparticles (AuNPs@MoS2), was fabricated via electrodeposition, for the highly sensitive detection of miRNA-21. The size and interparticle spacing of AuNPs was optimized by controlling nucleation and growth rates through tuning of deposition-potential and Au-precursor concentration and by getting simultaneous feedback from morphological and electrochemical activity studies. The sensing strategy, involved the selective immobilization of thiolated capture probe DNA (CP) at AuNPs and hybridization of CP to a part of miRNA target, whereas the remaining part of the target was complementary to a signaling non-labelled DNA sequence that served to amplify the target upon hybridization. Chronocoulometry provided precise quantification of nucleic acids at each step of the sensor assay by interrogating [Ru(NH3)6]3+ electrostatically bound to phosphate backbones of oligonucleotides. A detailed and systematic optimization study demonstrated that the thinnest and smallest MoS2 NSs improved the sensitivity of the AuNP@MoS2 sensor achieving an impressive detection limit of ≈100 aM, which is 2 orders of magnitude lower than that of bare Au electrode and also enhanced the DNA miRNA hybridization efficiency by 25%. Such improved performance can be attributed to the controlled packing density of CPs achieved by their self -assembly on AuNPs, large interparticle density, small size and the intimate coupling between AuNPs and MoS2. Alongside the outstanding sensitivity, the sensor exhibited excellent selectivity down to femtomolar concentrations, for discriminating complementary miRNA-21 target in a complex system composed of different foreign targets including mismatched and non-complementary miRNA-155. These advantages make our sensor a promising contender in the point of care miRNA sensor family for medical diagnostics

KW - Molybdenum disulfide (MoS2) Nanosheets

KW - Ionic Liquid Assisted Grinding Exfoliation

KW - Gold Decorated MoS2 Hybrid Nanosheets

KW - Electrochemical microRNA-sensor

KW - Chronocoulometric Detection

KW - microRNA-21 (miRNA-21)

KW - Electrochemical Deposition

KW - Screen-Printed Gold Electrodes

KW - 2D Materials

KW - 2 Dimensional Materials

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DO - 10.1021/acsabm.8b00398

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