Towards the real-time monitoring of glucose in tear fluid: holographic glucose sensors with reduced interference from lactate and pH.

Glucose-selective holographic sensors were fabricated from unique tetrahedral 2-acrylamidophenylboronic acid (2-APB) incorporated with co-monomers poly(ethylene glycol) acrylate (PEG), (3-acrylamidopropyl)trimethylammonium chloride (ATMA) and [2-(acryloyloxy)ethyl]-trimethylammonium chloride (AETA) into thin hydrogel films which were transformed into volume holograms using a diffusion method coupled with holographic recording using a frequency-doubled Nd:YAG laser (532 nm). The results showed that the 2-APB-based holographic sensors contracted upon addition of glucose due to the formation of a 2:1 complex between the tetrahedral 2-APB and glucose. More significantly, the 2-APB-based holographic sensors had greatly reduced lactate dependence and a hugely reduced pH effect over the physiological range of pH. These features are vital for development of contact lens-based glucose sensor, where the pH variability is greater (pH 5.8-7.8) and the lactate concentration is substantially higher than in blood. Furthermore, the 2-APB-based holographic sensors also displayed fast response to glucose. The successful union of holograms and the tetrahedral 2-APB receptor for glucose detection in artificial tear fluid is also demonstrated. This new type of holographic sensors responding to glucose with features of minor pH effect and negligible interference from lactate is applicable to the detection of glucose concentrations in tear fluid for the management of diabetes.

[1]  C. Lowe,et al.  Metabolite-sensitive holographic biosensors. , 2004, Analytical Chemistry.

[2]  Jeff Blyth,et al.  Glucose-sensitive holographic sensors for monitoring bacterial growth. , 2004, Analytical chemistry.

[3]  Jeff Blyth,et al.  pH-sensitive holographic sensors. , 2003, Analytical chemistry.

[4]  D. Capitani,et al.  Water in Hydrogels. An NMR Study of Water/Polymer Interactions in Weakly Cross-Linked Chitosan Networks , 2001 .

[5]  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 .

[6]  C. W. Gray,et al.  Boronic acid receptors for alpha-hydroxycarboxylates: high affinity of Shinkai's glucose receptor for tartrate. , 2002, The Journal of organic chemistry.

[7]  M. Duer Solid-state NMR spectroscopy : principles and applications , 2002 .

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

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

[10]  Joseph R Lakowicz,et al.  Noninvasive continuous monitoring of physiological glucose using a monosaccharide-sensing contact lens. , 2004, Analytical chemistry.

[11]  Felicity Sartain,et al.  Designed boronate ligands for glucose-selective holographic sensors. , 2006, Chemistry.

[12]  Nicholas A Peppas,et al.  Stimuli-sensitive hydrogels: ideal carriers for chronobiology and chronotherapy , 2004, Journal of biomaterials science. Polymer edition.

[13]  Jeff Blyth,et al.  Metal ion-sensitive holographic sensors. , 2002, Analytical chemistry.

[14]  John O. Edwards,et al.  Polyol Complexes and Structure of the Benzeneboronate Ion , 1959 .

[15]  Jeff Blyth,et al.  A Holographic Alcohol Sensor , 1999 .

[16]  E. Denkbaş,et al.  Implantable 5-fluorouracil loaded chitosan scaffolds prepared by wet spinning , 2000 .

[17]  N. Peppas,et al.  Structure and Interactions in Covalently and Ionically Crosslinked Chitosan Hydrogels for Biomedical Applications , 2003 .

[18]  S. Asher,et al.  Photonic crystal glucose-sensing material for noninvasive monitoring of glucose in tear fluid. , 2004, Clinical chemistry.

[19]  S. Asher,et al.  Acetylcholinesterase-based organophosphate nerve agent sensing photonic crystal. , 2005, Analytical chemistry.

[20]  C. D. Geddes,et al.  Fluorescence sensors for monosaccharides based on the 6-methylquinolinium nucleus and boronic acid moiety: potential application to ophthalmic diagnostics. , 2005, Talanta.

[21]  Christopher R Lowe,et al.  Holographic lactate sensor. , 2006, Analytical chemistry.

[22]  N. J. Van Haeringen,et al.  Clinical biochemistry of tears , 1981 .

[23]  Sanford A. Asher,et al.  Photoswitchable Spirobenzopyran‐ Based Photochemically Controlled Photonic Crystals , 2005 .

[24]  S. Asher,et al.  Polymerized colloidal crystal hydrogel films as intelligent chemical sensing materials , 1997, Nature.

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

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

[27]  Mark E. Smith,et al.  Multinuclear solid-state NMR of inorganic materials , 2002 .

[28]  M. Abelson,et al.  Normal human tear pH by direct measurement. , 1981, Archives of ophthalmology.

[29]  Roger Bradley Millington,et al.  A diffusion method for making silver bromide based holographic recording material , 1999 .