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Cited by 149Electrochemical sensors and biosensorsIonic liquids properties and applicationsAdvanced Sensor and Energy Harvesting Materials

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A new paradigm in sweat based wearable diagnostics biosensors using Room Temperature Ionic Liquids (RTILs)

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Munje, Rujuta D., Muthukumar, Sriram, Jagannath, Badrinath, Prasad, Shalini·2017·Scientific Reports
DOI 10.1038/s41598-017-02133-0PMC PMC5434046
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Abstract

Successful commercialization of wearable diagnostic sensors necessitates stability in detection of analytes over prolonged and continuous exposure to sweat. Challenges are primarily in ensuring target disease specific small analytes (i.e. metabolites, proteins, etc.) stability in complex sweat buffer with varying pH levels and composition over time. We present a facile approach to address these challenges using RTILs with antibody functionalized sensors on nanoporous, flexible polymer membranes. Temporal studies were performed using both infrared spectroscopic, dynamic light scattering, and impedimetric spectroscopy to demonstrate stability in detection of analytes, Interleukin-6 (IL-6) and Cortisol, from human sweat in RTILs. Temporal stability in sensor performance was performed as follows: (a) detection of target analytes after 0, 24, 48, 96, and 168 hours post-antibody sensor functionalization; and (b) continuous detection of target analytes post-antibody sensor functionalization. Limit of detection of IL-6 in human sweat was 0.2 pg/mL for 0–24 hours and 2 pg/mL for 24–48 hours post-antibody sensor functionalization. Continuous detection of IL-6 over 0.2–200 pg/mL in human sweat was demonstrated for a period of 10 hours post-antibody sensor functionalization. Furthermore, combinatorial detection of IL-6 and Cortisol in human sweat was established with minimal cross-talk for 0–48 hours post-antibody sensor functionalization.

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Crossref · 10.1038/s41598-017-02133-0

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Figures

Figure 1 (A) Schematic showing our vision of a wearable diagnostic sweat based biosensing and relative size of the developed sensor with RTIL and immunoassay functionalized semiconducting ZnO films on nanoporous polyamide substrates. (B) Image showing restricted wicking of fluid in active region of sensor along with a schematic showing capture probe–target biomarker interaction in RTIL and immunoassay with ZnO thin film on a porous membrane within the wicked region of the fluid.
Figure 1 (A) Schematic showing our vision of a wearable diagnostic sweat based biosensing and relative size of the developed sensor with RTIL and immunoassay functionalized semiconducting ZnO films on nanoporous polyamide substrates. (B) Image showing restricted wicking of fluid in active region of sensor along with a schematic showing capture probe–target biomarker interaction in RTIL and immunoassay with ZnO thin film on a porous membrane within the wicked region of the fluid.CC BY · PubMed Central
Figure 2 (A) SEM of nanoporous flexible membrane with inset showing EDAX spectra of the polyamide membrane surface. (B) SEM of ZnO sputtered polyamide membrane with inset showing EDAX spectra of the membrane surface. Zn peaks are only seen on the sputtered polyamide surface. (C) Structural parameters of membrane and ZnO thin film D) AFM image of ZnO thin film on silicon wafer.
Figure 2 (A) SEM of nanoporous flexible membrane with inset showing EDAX spectra of the polyamide membrane surface. (B) SEM of ZnO sputtered polyamide membrane with inset showing EDAX spectra of the membrane surface. Zn peaks are only seen on the sputtered polyamide surface. (C) Structural parameters of membrane and ZnO thin film D) AFM image of ZnO thin film on silicon wafer.CC BY · PubMed Central
Figure 3 XPS plots of (A) Zn 2p3/2 peak (B) O 1 s peak in bare ZnO and (C) Zn 2p3/2 peak (D) O 1 s peak (E) S 2p3/2 peak in DSP functionalized ZnO substrate.
Figure 3 XPS plots of (A) Zn 2p3/2 peak (B) O 1 s peak in bare ZnO and (C) Zn 2p3/2 peak (D) O 1 s peak (E) S 2p3/2 peak in DSP functionalized ZnO substrate.CC BY · PubMed Central
Figure 4 FTIR of polyamide surface on the side directly opposite to the surface used for applying the RTIL with IL-6 solution. The spectra establish no hindrance to the wicking and diffusion of IL-6 in RTIL through the nanoporous membrane thickness.
Figure 4 FTIR of polyamide surface on the side directly opposite to the surface used for applying the RTIL with IL-6 solution. The spectra establish no hindrance to the wicking and diffusion of IL-6 in RTIL through the nanoporous membrane thickness.CC BY · PubMed Central
Figure 5 FTIR spectra of DSP linker immobilized on ZnO surface (top), α-IL-6 antibody immobilized on DSP linker after T0, T24 and T48 hours (bottom).
Figure 5 FTIR spectra of DSP linker immobilized on ZnO surface (top), α-IL-6 antibody immobilized on DSP linker after T0, T24 and T48 hours (bottom).CC BY · PubMed Central
Figure 6 DLS and zeta potential measurements. (A) α-IL-6 antibody spiked in synthetic sweat (SS) of varying pH and RTIL ratios; (B) IL-6 antibody-antigen interactions in 50% RTIL in SS solutions. The dotted line in (B) represent the zero dose antigen zeta potential value for the respective proteins.
Figure 6 DLS and zeta potential measurements. (A) α-IL-6 antibody spiked in synthetic sweat (SS) of varying pH and RTIL ratios; (B) IL-6 antibody-antigen interactions in 50% RTIL in SS solutions. The dotted line in (B) represent the zero dose antigen zeta potential value for the respective proteins.CC BY · PubMed Central
Figure 7 (A) Percent change in Zmod ratio of antigen IL-6 concentration varying from 0.2 pg/mL to 200 pg/mL tested for varying storage time of antibody IL-6 for time T0, T24, T48, T96 and T168 at 4 °C. The dashed line represents specific signal threshold (SST). (B) Continuous time based detection of IL-6 in human sweat through impedance change.
Figure 7 (A) Percent change in Zmod ratio of antigen IL-6 concentration varying from 0.2 pg/mL to 200 pg/mL tested for varying storage time of antibody IL-6 for time T0, T24, T48, T96 and T168 at 4 °C. The dashed line represents specific signal threshold (SST). (B) Continuous time based detection of IL-6 in human sweat through impedance change.CC BY · PubMed Central
Figure 8 Specificity of antibody IL-6 interactions towards antigen IL-6 and non-specific interactions with cortisol and glucose biomolecules for time intervals of antibody functionalized ZnO sensors stored at T0 to T168.
Figure 8 Specificity of antibody IL-6 interactions towards antigen IL-6 and non-specific interactions with cortisol and glucose biomolecules for time intervals of antibody functionalized ZnO sensors stored at T0 to T168.CC BY · PubMed Central

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Metadata

Authors
Munje, R. D., Muthukumar, S., Jagannath, B., & Prasad, S.
Affiliations
The University of Texas at Dallas (US)
Corresponding author
Prasad, Shalini
ORCID
Venue
Scientific Reports
Publisher
Springer Science and Business Media LLC
Published
2017-05-16
Volume
7
Issue
1
Pages
1950-1950
ISSN
2045-2322 (ISSN-L)
DOI
10.1038/s41598-017-02133-0
PMC
PMC5434046
OpenAlex
W2612250156
Cited by
149
References
46
Citations by year
2026: 13 · 2025: 16 · 2024: 24 · 2023: 16 · 2022: 23 · 2021: 19 · 2020: 12 · 2019: 12 · 2018: 12 · 2017: 2
FWCI
4.32
Type
journal article
Language
en
Open access
Licence
Locations
  • Scientific Reports (publishedVersion, cc-by)
  • Europe PMC (PubMed Central) (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
Topics
  • Physical Sciences › Chemistry › Analytical Chemistry › Electrochemical sensors and biosensors
  • Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Ionic liquids properties and applications
  • Physical Sciences › Engineering › Biomedical Engineering › Advanced Sensor and Energy Harvesting Materials
Keywords
wearable diagnostics, room temperature ionic liquids, interleukin-6 detection, cortisol detection, nanoporous membranes, sensor stability
MeSH terms
Dynamic Light Scattering, Wearable Electronic Devices, Humans, Hydrocortisone, Nylons, Sweat, Temperature, Zinc Oxide, Biosensing Techniques, Porosity, Spectroscopy, Fourier Transform Infrared, Ionic Liquids

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