A wireless chemical sensor featuring iron oxide nanoparticle-embedded hydrogels ☆

Abstract In this paper, we introduce a wireless chemical sensor based on a magnetically functionalized hydrogels (ferrogels). By embedding superparamagnetic nanoparticles into the hydrogel network and laminating the hydrogel on a planar coil, the swelling state of the hydrogel, which depends on the chemical environment, can be interrogated by measuring its magnetic permeability. To validate the chemical sensing principle, a pH sensor is fabricated using a poly(methacrylic acid- co -acrylamide) pH sensitive hydrogel, and repeatable, reversible responses are obtained to pH changes, which are easily discriminated down to 0.1 pH unit. It is anticipated that the same scheme can be applied to hydrogels sensitive to different stimuli (e.g., glucose, specific ions, antigens, temperature, etc.), and that this sensor can be configured for implantation and wireless monitoring.

[1]  F. Horkay,et al.  Constant-volume hydrogel osmometer: a new device concept for miniature biosensors. , 2002, Biomacromolecules.

[2]  Hui Jiang,et al.  Increased in vivo stability and functional lifetime of an implantable glucose sensor through platinum catalysis. , 2013, Journal of biomedical materials research. Part A.

[3]  Vladimir V. Tsukruk,et al.  Buckling instabilities in periodic composite polymeric materials , 2010 .

[4]  Igor K Lednev,et al.  High ionic strength glucose-sensing photonic crystal. , 2003, Analytical chemistry.

[5]  Bismuth Hall probes: Preparation, properties and application , 2010 .

[6]  Toyoichi Tanaka Kinetics of phase transition in polymer gels , 1986 .

[7]  Kinam Park,et al.  Environment-sensitive hydrogels for drug delivery , 2001 .

[8]  Toyoichi Tanaka,et al.  Volume phase transition in a nonionic gel , 1984 .

[9]  T. Okano,et al.  Glucose-Responsive Gel from Phenylborate Polymer and Poly (Vinyl Alcohol): Prompt Response at Physiological pH Through the Interaction of Borate with Amino Group in the Gel , 1997, Pharmaceutical Research.

[10]  K. Najafi,et al.  A wireless batch sealed absolute capacitive pressure sensor , 2001 .

[11]  Zoe A. Strong,et al.  Hydrogel-Actuated Capacitive Transducer for Wireless Biosensors , 2002 .

[12]  Jeff Blyth,et al.  Holographic glucose sensors. , 2005, Biosensors & bioelectronics.

[13]  Robin H. Liu,et al.  Functional hydrogel structures for autonomous flow control inside microfluidic channels , 2000, Nature.

[14]  Ronald A. Siegel,et al.  pH-Dependent Equilibrium Swelling Properties of Hydrophobic Polyelectrolyte Copolymer Gels , 1988 .

[15]  Takashi Miyata,et al.  Tumor marker-responsive behavior of gels prepared by biomolecular imprinting , 2006, Proceedings of the National Academy of Sciences of the United States of America.

[16]  P Tathireddy,et al.  Osmotic Swelling Pressure Response of Smart Hydrogels Suitable for Chronically-Implantable Glucose Sensors. , 2010, Sensors and actuators. B, Chemical.

[17]  L. Brannon-Peppas,et al.  Dynamic and equilibrium swelling behaviour of pH-sensitive hydrogels containing 2-hydroxyethyl methacrylate. , 1990, Biomaterials.

[18]  C. Niu,et al.  A novel ion‐imprinted hydrogel for recognition of potassium ions with rapid response , 2010 .

[19]  Bjørn T. Stokke,et al.  Toehold of dsDNA exchange affects the hydrogel swelling kinetics of a polymer–dsDNA hybrid hydrogel , 2011 .

[20]  F Solzbacher,et al.  Free swelling and confined smart hydrogels for applications in chemomechanical sensors for physiological monitoring. , 2009, Sensors and actuators. B, Chemical.

[21]  K. Takahata,et al.  A hydrogel-based passive wireless sensor using a flex-circuit inductive transducer , 2009 .

[22]  F Solzbacher,et al.  Hydrogel based sensor arrays (2 × 2) with perforated piezoresistive diaphragms for metabolic monitoring (in vitro). , 2010, Sensors and actuators. B, Chemical.

[23]  Paul V. Braun,et al.  Sensors and Actuators B: Chemical Fast Response Photonic Crystal Ph Sensor Based on Templated Photo-polymerized Hydrogel Inverse Opal , 2022 .

[24]  A. Horgan,et al.  Crosslinking of phenylboronic acid receptors as a means of glucose selective holographic detection. , 2006, Biosensors & bioelectronics.

[25]  A. Khademhosseini,et al.  Hydrogels in Biology and Medicine: From Molecular Principles to Bionanotechnology , 2006 .

[26]  Babak Ziaie,et al.  Hydrogel-based microsensors for wireless chemical monitoring , 2009, Biomedical microdevices.

[27]  J. Feijen,et al.  Mutual influence of pH and temperature on the swelling of ionizable and thermosensitive hydrogels , 1992 .

[28]  Takashi Miyata,et al.  A reversibly antigen-responsive hydrogel , 1999, Nature.

[29]  G. Gerlach,et al.  Chemical and pH sensors based on the swelling behavior of hydrogels , 2005 .

[30]  Mark D. Losego,et al.  Hydrogel-Based Glucose Sensors: Effects of Phenylboronic Acid Chemical Structure on Response , 2013 .

[31]  S. Asher,et al.  Polymerized crystalline colloidal array sensing of high glucose concentrations. , 2009, Analytical chemistry.

[32]  T. Okano,et al.  A new thermo-sensitive hydrogel: Interpenetrating polymer networks from N-acryloylpyrrolidine and poly(oxyethylene) , 1988 .

[33]  S. Asher,et al.  Electrochemical investigation of Pb2+ binding and transport through a polymerized crystalline colloidal array hydrogel containing benzo-18-crown-6. , 2005, Analytical chemistry.

[34]  Thomas Wallmersperger,et al.  Piezoresistive biochemical sensors based on hydrogels , 2010 .

[35]  Alexei R. Khokhlov,et al.  pH-Responsive Gels of Hydrophobically Modified Poly(acrylic acid) , 1997 .

[36]  Igor K Lednev,et al.  Photonic crystal carbohydrate sensors: low ionic strength sugar sensing. , 2003, Journal of the American Chemical Society.

[37]  Oguz H. Elibol,et al.  Micromechanical cantilever as an ultrasensitive pH microsensor , 2002 .

[38]  J. Burdick,et al.  Kinetic study of swelling-induced surface pattern formation and ordering in hydrogel films with depth-wise crosslinking gradient , 2010 .

[39]  Edward L Cussler,et al.  Temperature sensitive gels as extraction solvents , 1987 .

[40]  Toyoichi Tanaka,et al.  Volume‐phase transitions of ionized N‐isopropylacrylamide gels , 1987 .

[41]  J. Rühe,et al.  Swelling Behavior of Thin, Surface-Attached Polymer Networks , 2004 .

[42]  M. Lesho,et al.  Electrical conductivity of pH-responsive hydrogels. , 1997, Journal of biomaterials science. Polymer edition.

[43]  B. T. Stokke,et al.  Glucose sensors based on a responsive gel incorporated as a Fabry-Perot cavity on a fiber-optic readout platform. , 2009, Biosensors & bioelectronics.

[44]  S. Lai,et al.  Design of a Self-Regulated Drug Delivery Device , 2001 .

[45]  A. Katchalsky,et al.  Potentiometric titration of polyelectrolyte gels , 1957 .

[46]  S. Asher,et al.  Fast responsive crystalline colloidal array photonic crystal glucose sensors. , 2006, Analytical chemistry.

[47]  Zhibing Hu,et al.  Pattern formation of constrained acrylamide/sodium acrylate copolymer gels in acetone/water mixture , 1994 .

[48]  M. Zrínyi,et al.  Magnetic Field-Responsive Smart Polymer Composites , 2007 .

[49]  Babak Ziaie,et al.  A hydrogel-based implantable micromachined transponder for wireless glucose measurement. , 2006, Diabetes technology & therapeutics.

[50]  J. Z. Hilt,et al.  Magnetic nanoparticles in biomedicine: synthesis, functionalization and applications. , 2010, Nanomedicine.

[51]  Babak Ziaie,et al.  Integration of hydrogels with hard and soft microstructures. , 2007, Journal of nanoscience and nanotechnology.

[52]  Akira Matsumoto,et al.  Swelling and Shrinking Kinetics of Totally Synthetic, Glucose-Responsive Polymer Gel Bearing Phenylborate Derivative as a Glucose-Sensing Moiety , 2004 .

[53]  Yuandong Gu,et al.  Hard and soft micro- and nanofabrication: An integrated approach to hydrogel-based biosensing and drug delivery. , 2010, Journal of controlled release : official journal of the Controlled Release Society.

[54]  Jeff Blyth,et al.  Towards the real-time monitoring of glucose in tear fluid: holographic glucose sensors with reduced interference from lactate and pH. , 2008, Biosensors & bioelectronics.

[55]  B. Ziaie,et al.  Squeeze-film hydrogel deposition and dry micropatterning. , 2010, Analytical chemistry.

[56]  Babak Ziaie,et al.  A Minimally Invasive Implantable Wireless Pressure Sensor for Continuous IOP Monitoring , 2011, IEEE Transactions on Biomedical Engineering.

[57]  Kamila Gawel,et al.  Responsive Hydrogels for Label-Free Signal Transduction within Biosensors , 2010, Sensors.

[58]  R. Siegel Hydrophobic weak polyelectrolyte gels: Studies of swelling equilibria and kinetics , 1993 .

[59]  T. Okano,et al.  Totally Synthetic Polymer Gels Responding to External Glucose Concentration: Their Preparation and Application to On−Off Regulation of Insulin Release , 1998 .

[60]  K. G. Ong,et al.  A wireless pH sensor based on the use of salt-independent micro-scale polymer spheres , 2003 .

[61]  Shoji Kimura,et al.  Development of a molecular recognition ion gating membrane and estimation of its pore size control. , 2002, Journal of the American Chemical Society.