Page 201 - Organic Electronics in Sensors and Biotechnology
P. 201

178    Chapter  Five

               integration of the OLED/O  sensor. This multiple bioanalyte sensor is
                                      2
               obviously important for various clinical, health, industrial, and envi-
               ronmental applications.
                   The glucose, lactate, and ethanol sensing methods were similar,
               so we describe the method for glucose only. The glucose level was
               determined from the DO level following the enzymatic oxidation of
               glucose by glucose oxidase (GOx) (the GOx was embedded in a thin
               sol-gel film or dissolved in solution):

                        glucose + O + GOx → H O + gluconic acid      (5.2)
                                  2          2  2
                   Hence, in the presence of glucose, the PL quenching of the O -
                                                                        2
               sensitive dye is reduced (i.e., I and τ increase) due to O  consumption
                                                             2
               during the enzymatic oxidation. 13, 16, 62, 63  A similar reaction in the pres-
               ence of lactate oxidase (LOx) or alcohol oxidase (AOx) results in lac-
               tate or ethanol oxidation, respectively.
                   The multianalyte measurements were performed in sealed cells,
               since the DO in such cells could not be replenished from the air, and,
               consequently, its final level yielded the initial analyte level directly.
               Indeed, the responses from cells open to air were more complex,
                                            16
               clearly due to such replenishment.  The O -sensitive dye, embedded
                                                   2
               in a PS film, was deposited on the bottom of the reaction cells. Each
               cell contained a buffered solution of GOx, LOx, or AOx. The total
               volume of each cell was 100 to 200 μL.
                   Measurements in sealed cells also resulted in a low LOD of ~0.01
               to 0.02 mM for glucose, lactate, and ethanol. In our previous studies
               on the OLED-based glucose sensor, the GOx was embedded in a sol-
               gel film, rather than dissolved in solution. The sol-gel film was depos-
               ited on the PtOEP:PS film, and the monitored sample was simply
               dropped on the sol-gel film. While the dynamic range was a much
               higher 0 to 5 mg/mL, the LOD was also higher. In reports on other
               PL-based glucose sensors, the excitation sources have included Ar +
               lasers (operated at 20 to 40 mW), Hg lamps, or a fluorimeter with a
               150 W Xe lamp light source. 4, 62, 63  The glucose concentration c  was
                                                                    Gl
               usually monitored via changes in I.
                   The OLED sensor array was assembled in a back-detection geom-
               etry and operated in the τ mode. The analytes were monitored both
               sequentially, using a single PD, and simultaneously, using a compat-
               ible array of Si photodiodes. The sequential and simultaneous modes
               yielded similar results. Calibration curves were obtained by using a
               modified SV equation suitable for these analytes in sealed cells, where
               there is no supply of DO beyond the initial concentration. The modi-
               fied SV equation was based on the following considerations: Let the
               initial analyte, initial DO, and final DO levels be [analyte]  ,
                                                                      initial
               [DO]   , and [DO]  , respectively. Then if
                    initial    final
                                [analyte]   ≤ [DO]                   (5.3)
                                        initial   initial
   196   197   198   199   200   201   202   203   204   205   206