In vitro investigations of a pH- and ionic-strength-responsive polyelectrolytic hydrogel using a piezoresistive microsensor

Environmentally responsive or smart hydrogels show a volume phase transition due to changes of external stimuli such as pH or ionic strength of an ambient solution. Thus, they are able to convert reversibly chemical energy into mechanical energy and therefore they are suitable as sensitive material to be integrated in biochemical microsensors and MEMS devices. In this work, micro fabricated silicon pressure sensor chips with integrated piezoresistors were used as transducers for the conversion of mechanical work into an appropriate electrical output signal due to the deflection of a thin silicon bending plate. Within this work two different sensor designs have been studied. The biocompatible poly(hydroxypropyl methacrylate-N,N-dimethylaminoethyl methacrylate-tetra-ethyleneglycol dimethacrylate) (HPMADMA- TEGDMA) was used as an environmental-sensitive element in piezoresistive biochemical sensors. This polyelectrolytic hydrogel shows a very sharp volume phase transition at pH values below about 7.4 which is in the range of the physiological pH. The sensor's characteristic response was measured in-vitro for changes in pH of PBS buffer solution at fixed ionic strength. The experimental data was applied to the Hill equation and the sensor sensitivity as a function of pH was calculated out of it. The time-dependent sensor response was measured for small changes in pH, whereas different time constants have been observed. The same sensor principal was used for sensing the ionic strength. The time-dependent electrical output signal of both sensors was measured for variations in ionic strength at fixed pH value using PBS buffer solution. Both sensor types showed an asymmetric swelling behavior between the swelling and the deswelling cycle as well as different time constants, which was attributed to the different nature of mechanical hydrogel confinement inside the sensor.

[1]  K. Najafi,et al.  Special topic section on microtechniques, microsensors, microactuators, and microsystems , 2000, IEEE Transactions on Biomedical Engineering.

[2]  H. Westerhoff,et al.  Analyses of dose-response curves to compare the antimicrobial activity of model cationic alpha-helical peptides highlights the necessity for a minimum of two activity parameters. , 2006, Analytical biochemistry.

[3]  C. Hunt,et al.  Buffer Effects on Swelling Kinetics in Polybasic Gels , 2004, Pharmaceutical Research.

[4]  R. Schmidt,et al.  Physiologie des Menschen , 1993, Springer-Lehrbuch.

[5]  B. Ziaie,et al.  Novel swelling/shrinking behaviors of glucose-binding hydrogels and their potential use in a microfluidic insulin delivery system , 2004 .

[6]  A. Hill The Combinations of Haemoglobin with Oxygen and with Carbon Monoxide. I. , 1913, The Biochemical journal.

[7]  M. Lesho,et al.  A method for studying swelling kinetics based on measurement of electrical conductivity , 1998 .

[8]  A. Lowman,et al.  Controlling the collapse/swelling transition in charged hydrogels. , 2004, Biomaterials.

[9]  Margarita Guenther,et al.  Hydrogel-Based Sensor for a Rheochemical Characterization of Solutions , 2007 .

[10]  G. Gerlach,et al.  Application of polyelectrolytic temperature-responsive hydrogels in chemical sensors , 2007 .

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

[12]  Jules J. Magda,et al.  Catalase Effects on Glucose-Sensitive Hydrogels , 2000 .

[13]  G. Gerlach,et al.  Chemical sensors based on multiresponsive block copolymer hydrogels , 2007 .

[14]  R. Siegel,et al.  Kinetics and mechanisms of water sorption in hydrophobic, ionizable copolymer gels , 1991 .

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

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

[17]  Silverthorn Dee Unglaub Human Physiology: An Integrated Approach , 1998 .

[18]  A. Christopoulos,et al.  Fitting Models to Biological Data Using Linear and Nonlinear Regression: A Practical Guide to Curve Fitting , 2004 .

[19]  Margarita Guenther,et al.  Hydrogel-based piezoresistive pH sensors: investigations using FT-IR attenuated total reflection spectroscopic imaging. , 2008, Analytical chemistry.