Abstract
Microlithographically fabricated interdigitated microsensor electrodes (IMEs) were cleaned, surface activated, chemically functionalized (amine) and derivatized with an Acrloyl-PEG-NHS to receive a spun-applied monomer cocktail of UV polymerizable monomer. IMEs were 2050.5, 1550.5, 1050.5 and 0550.5 possessing lines and spaces that were 20, 15, 10, and 5 μm respectively; 5 mm line lengths and were 50 lines on each opposing bus. Bioactive hydrogels were synthesized from spun-applied and UV-crosslinked tetraethyleneglycol diacrylate (TEGDA) (crosslinker), 2-hydroxyethylmethacrylate (HEMA), polyethyleneglycol(200) monomethacrylate (PEGMA), N-[tris(hydroxymethyl)methyl]-acrylamide (HMMA) and poly(HEMA) (MW 60,000) (viscosity modifier) and 2,2-dimethoxy-2-phenylacetophenone (DMPA) (photoinitiator) to produce a 5 μm thick p(HEMA-co-PEGMA-co-HMMA) hydrogel membrane on the IMEs. Unmodified and hydrogel coated IMEs where characterized by AC electrical impedance spectroscopy using 50 mV p-t-p over the frequency range from 10 Hz to 100 kHz in aqueous PBS 7.4 buffer and in buffer containing 50 mM [Fe(CN)6]3-/4− solution at RT. Impedimetric responses were found to scale with the device geometric parameters. Equivalent circuit modeling revealed deviations from ideality at lower device dimensions suggesting an implication of the substrate surface charge on the double layer capacitance of the electrodes. Diffusion coefficients derived from the Warburg component are in accord with literature values.
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M.Y. Arica, G. Bayramoglu, Polyethyleneimine-grafted poly(hydroxyethyl methacrylate-co-glycidyl methacrylate) membranes for reversible glucose oxidase immobilization. Biochem. Eng. J. 20(1), 73–77 (2004a)
M.Y. Arica, G. Bayramoglu, Reversible immobilization of tyrosinase onto polyethyleneimine-grafted and Cu(II) chleated poly(HEMA-co-GMA) reactive membranes. J. Mol. Catal. B Enzym. 27(4–6), 255–265 (2004b)
S.H. Behrens, D.G. Grier, The charge of glass and silica surfaces. J. Chem. Phys. 115, 6716 (2001)
T. Blythe, D. Bloor, Electrical properties of polymers (Cambridge University Press, London, 2005)
A. Boztas, A. Guiseppi-Elie, Immobilization and release of the redox mediator ferrocene monocarboxylic acid from within cross-linked p(HEMA-co-PEGMA-co-HMMA) hydrogels. Biomacromolecules 10(8), 2135–2143 (2009)
S. Brahim, A.M. Wilson et al., Chemical and biological sensors based on impedimetric detection using conductive polymers. Microchim. Acta 143, 123–137 (2003)
L. Doretti, P. Gattolin et al., Amperometric choline sensor with enzyme immobilized by gamma-irradiation in a biocompatible membrane. Anal. Lett. 27(13), 2455–2470 (1994)
L. Doretti, P. Gattolin et al., Covalently immobilized choline oxidase and cholinesterases on a methacrylate copolymer for disposable membrane biosensors. Appl. Biochem. Biotechnol. 74(1), 1–12 (1998)
R. Ehret, W. Baumann et al., Monitoring of cellular behavior by impedance measurements on interdigitated electrode structures. Biosens. Bioelectrons. 12(1), 29–41 (1997)
R. Ehret, W. Baumann et al., On-line control of cellular adhesion with impedance measurements using interdigitated electrode structure. Med. Biol. Eng. Comput. 36, 365–370 (1998)
Y.A. Gao, N. Li et al., A cyclic voltammetric technique for the detection of micro-regions of bmimPF6/Tween 20/H2O microemulsions and their performance characterization by UV-Vis spectroscopy. Green Chem 8, 43–49 (2006)
K. Gawel, D. Barriet et al., Responsive hydrogels for label-free signal transduction within biosensors. Sensors 10(5), 4381–4409 (2010)
A. Guiseppi-Elie, Electroconductive hydrogels: synthesis, characterization and biomedical applications. Biomaterials 31(10), 2701–2716 (2010a)
A. Guiseppi-Elie, An implantable biochip to influence patient outcomes following trauma-induced hemorrhage. Anal Bioanal Chem (2010b). doi:10.1007/s00216-010-4271-x
T.C. Hang, A. Guiseppi-Elie, Frequency dependent and surface characterization of DNA immobilization and hybridization. Biosens. Bioelectron. 19, 1537–1548 (2004)
Y. Huang, B. Rubinsky, Microfabricated electroporation chip for single cell membrane permeabilization. Sens. Actuators, A 89(3), 242–249 (2001)
C. Jimenez, J. Bartrol et al., Use of photopolymerizable membranes based on polyacrylamide hydrogels for enzymatic microsensor construction. Anal. Chim. Acta 351(1–3), 169–176 (1997)
G. Justin, A.R. Abdur Rahman et al., Bioactive hydrogel layers on microdisc electrode arrays: cyclic voltammetry experiments and simulations. Electroanalysis 21(10), 1125–1134 (2009a)
G. Justin, S. Finley et al., Biomimetic hydrogels for biosensor implant biocompatibility: electrochemical characterization using micro-disc electrode arrays (MDEAs). Biomed. Microdevices 11(1), 103–115 (2009b)
S.J. Kim, S.J. Park et al., Electroactive characteristics of interpenetrating polymer network hydrogels composed of Poly(vinyl alcohol) and Poly(N-isopropylacrylamide). J. Appl. Polym. Sci. 89, 890–894 (2003)
D.-N. Kim, W. Lee et al., Micropatterning of proteins on the surface of three-dimensional poly(ethylene glycol) hydrogel microstructures. Anal. Chim. Acta 609(1), 59–65 (2008)
S.J. Konopka, B. McDuffie, Diffusion coefficients of ferricyanide and ferrocyanide ions in aqueous media using twin electrode thin layer electrochemistry. Anal. Chem. 42(14), 1741–1746 (1970)
A. Kyritsis, P. Pissis et al., Dielectric relaxation spectroscopy in poly (hydroxyethyl acrylates)/water hydrogels. J. Polym. Sci., B: Polym. Phys. 33(12), 1737–1750 (1995)
W. Laureyn, F. Frederix, et al. Nanoscaled interdigititated gold electrodes for impedimetric immunosensing. Transducer’99. Sendai, Japan, Digest of Technical Papers, pp 1884–1185 (1999a)
W. Laureyn, D. Nelis, et al. Nanoscaled interdigititated titanium electrode for impedimetric biosensing. Eurosensors XIII. Hague, The Netherland. Proceeding for the 13th European Conference on Solid-State Transducers. (1999b).
L. Li, D.R. Walt, Dual-analyte fiber-optic sensor for the simultaneous and continuous measurement of glucose and oxygen. Anal. Chem. 67(20), 3746–3752 (1995)
H. Li, D.Q. Wang et al., Synthesis of a novel gelatin–carbon nanotubes hybrid hydrogel. Colloids Surf., B 33(2), 85–88 (2004)
C.C. Lin, A.T. Metters, Hydrogels in controlled release formulations: Network design and mathematical modeling. Adv. Drug Deliv. Rev. 58(12–13), 1379–1408 (2006)
P. Linderholm, J. Vannod et al., Bipolar resistivity profiling of 3D tissue culture. Biosens. Bioelectron. 22, 789–796 (2007)
Y. Luo, K.R. Kirker et al., Cross-linked hyaluronic acid hydrogel films: new biomaterials for drug delivery. J. Control. Release 69(1), 169–184 (2000)
V.F. Lvovich, C.C. Liu et al., Optimization and fabrication of planar interdigitated impedance sensors for highly resistive non-aqueous industrial fluids. Sens. Actuators, B 119(2), 490–496 (2006)
E. Mack, T. Okano et al., Hydrogels in medicine and pharmacy. Polymers vol II (CRC Press, Boca Raton, 1988)
A.V. Manishev, Y. Du et al., Evaluation of diffusion driven material property profiles using three wavelength interdigital sensor. IEEE Trans. Dielectr. Electr. Insul. 8(5), 785–798 (2001)
A.T. Metters, K.S. Anseth et al., Fundamental studies of a novel, biodegradable PEG-b-PLA hydrogel. Polymer 41(11), 3993–4004 (2000)
W. Olthuis, W. Streekstra et al., Theoretical and experimental determination of cell constants of planar-interdigitated electrolyte conductivity sensors. Sens. Actuators, B 24(1–3), 252–256 (1995)
R.M. Ottenbrite, K. Park et al. (eds.), Biomedical applications of hydrogels handbook (New York, Springer, 2010)
N. Pekel, B. Salih et al., Enhancement of stability of glucose oxidase by immobilization onto metal ion-chelated poly (N-vinyl imidazole) hydrogels. J. Biomater. Sci. Polym. Ed. 16(2), 253–266 (2005)
M. Pellissier, D. Zigah et al., Optimized preparation and scanning electrochemical microscopy analysis in feedback mode of glucose oxidase layers grafted onto conducting carbon surfaces. Langmuir 24(16), 9089–9095 (2008)
N.A. Peppas, J.J. Sahlin, Hydrogels as mucoadhesive and bioadhesive materials: a review. Biomaterials 17(16), 1553–1561 (1996)
R. Pethig, Dielectric properties of biological materials: biophysical and medical applications. IEEE Trans. Electr. Insul. EI-19(5), 453–474 (1984)
M.V. Pishko, A. Revzin et al., Mass transfer in amperometric biosensors based on nanocomposite thin films of redox polymers and oxidoreductases. Sensors 2(3), 79–90 (2002)
A.R.A. Rahman, A. Guiseppi-Elie, Design considerations in the development and application of Microdisc Electrode Arrays (MDEAs) for implantable biosensors. Biomed. Microdevices 11, 701–710 (2009)
A.R.A. Rahman, D.T. Price et al., Effect of electrode geometry on the impedance evaluation of tissue and cell culture. Sens. Actuators, B 127, 89–96 (2007)
A.R.A. Rahman, G. Justin et al., Towards an implantable biochip for glucose and lactate monitoring using microdisc electrode arrays (MDEAs). Biomed. Microdevices 11(1), 75–85 (2009)
B. Roffel, J.J. van de Graaf, The diffusion coefficient of ferricyanide ions in aqueous potassium chloride solutions with and without polyethylene oxide addition. J. Chem. Eng. Data 22(3), 301–302 (1977)
A.Y. Rubina, S.V. Pan’kov et al., Hydrogel drop microchips with immobilized DNA: properties and methods for large-scale production. Anal. Biochem. 325(1), 92–106 (2004)
B. Schulz, A. Riedel et al., Influence of polymerization parameters and entrapment in poly(hydroxyethyl methacrylate) on activity and stability of GOD. J. Mol. Catal. B Enzym. 7(1–4), 85–91 (1999)
S. Sengupta, D.A. Battigelli et al., A micro-scale multi-frequency reactance measurement technique to detect bacterial growth at low bio-particle concentrations. Lab Chip 6, 1–11 (2006)
N.F. Sheppard Jr., R.C. Tucker et al., Electrical conductivity measurements using microfabricated interdigitated electrodes. Anal. Chem. 65(9), 1199–1202 (1993)
N.F. Sheppard Jr., M.J. Lesho et al., Microfabricated conductimetric pH sensor. Sens. Actuators, B 28(2), 95–102 (1995)
N.F. Sheppard Jr., D.J. Mears et al., Model of a conductimetric urea biosensor. Biosens. Bioelectron. 11(10), 967–979 (1996)
C. Soto, C. Patterson et al., Immobilization and hybridization of DNA in a sugar polyacrylate hydrogel. Biotechnol. Bioeng. 92(7), 934–942 (2005)
M.M. Sung, G.J. Kluth et al., Formation of alkylsiloxane self-assembled monolayers on Si3N4. J. Vac. Sci. Technol., A 17(2), 540–544 (1999)
R. Trigo, M. Blanco, et al., L-Ascorbic acid release from poly(2-hydroxyethyl methacrylate) hydrogels. Polym. Bull. 31, 577–584 (1993)
Y. Wang, G. Tan et al., Influence of water states in hydrogels on the transmissibility and permeability of oxygen in contact lens materials. Appl. Surf. Sci. 255(2), 604–606 (2008)
L. Yang, A. Guiseppi-Elie, Impedimetric biosensors for nano and microfluidics, in Encyclopedia of microfluidics and nanofluidics, ed. by D. Li, vol. 2 (Springer-Verlag GmbH, Berlin Heidelberg, 2008), pp. 811–823
L. Yang, Y. Li, Detection of viable Salmonella using microelectrode-based capacitance measurement coupled with immunomagnetic separation. J. Microbiol. Methods 64, 9–16 (2006)
X. Yang, G. Zhang, The voltammetric performance of interdigitated electrodes with different electron-transfer rate constants. Sens. Actuators, B 126(2), 624–631 (2007)
L. Yang, Y. Li et al., Interdigited microelectrode (IME) impedance sensor for the detection of viable Salmonella typhimurium. Biosens. Bioelectron. 19, 1139–1147 (2004)
B. Yu, C. Wang et al., Use of hydrogel coating to improve the performance of implanted glucose sensors. Biosens. Bioelectron. 23(8), 1278–1284 (2008)
M.C. Zaretsky, L. Mouayad et al., Continuum properties from interdigital electrode dielectrometry. IEEE Trans. Elect. Insul. 23, 897–917 (1988)
Acknowledgements
L. Yang acknowledges support from NC BIOIMPACT initiative and the Gold Leaf foundation. A Guiseppi-Wilson acknowledges the support of ABTECH Scientific, Inc. and A. Guiseppi-Elie acknowledges support from the US Department of Defense (DoDPRMRP) grant PR023081/DAMD17-03-1-0172 and the Consortium of the Clemson University Center for Bioelectronics, Biosensors and Biochips (C3B).
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Yang, L., Guiseppi-Wilson, A. & Guiseppi-Elie, A. Design considerations in the use of interdigitated microsensor electrode arrays (IMEs) for impedimetric characterization of biomimetic hydrogels. Biomed Microdevices 13, 279–289 (2011). https://doi.org/10.1007/s10544-010-9492-4
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DOI: https://doi.org/10.1007/s10544-010-9492-4