Research Papers

Neutron Imaging and Electrochemical Characterization of a Glucose Oxidase-Based Enzymatic Electrochemical Cell

[+] Author and Article Information
Ryan S. Longchamps

Department of Mechanical and
Aerospace Engineering,
University of Alabama in Huntsville,
301 Sparkman Drive,
Huntsville, AL 35899
e-mail: rsl0002@uah.edu

Zachary K. van Zandt

Department of Mechanical and
Aerospace Engineering,
University of Alabama in Huntsville,
301 Sparkman Drive,
Huntsville, AL 35899
e-mail: zkz0001@uah.edu

Hassina Z. Bilheux

Chemical and Engineering Materials Division,
Oak Ridge National Laboratory,
P.O. Box 2008,
Oak Ridge, TN 37831
e-mail: bilheuxhn@ornl.gov

Indu Dhiman

Chemical and Engineering Materials Division,
Oak Ridge National Laboratory,
P.O. Box 2008,
Oak Ridge, TN 37831
e-mail: dhimani@ornl.gov

Louis J. Santodonato

Instrument and Source Division,
Oak Ridge National Laboratory,
P.O. Box 2008,
Oak Ridge, TN 37831
e-mail: santodonatol@ornl.gov

Yevgenia Ulyanova

Hexcel Corporation,
3300 Mallard Fox Drive,
Decatur, AL 35601
e-mail: jenny.ulyanova@hexcel.com

Sameer Singhal

CFD Research Corporation,
701 McMillian Way NW,
Huntsville, AL 35806
e-mail: ss2@cfdrc.com

George J. Nelson

Department of Mechanical and
Aerospace Engineering,
University of Alabama in Huntsville,
301 Sparkman Drive,
Huntsville, AL 35899
e-mail: george.nelson@uah.edu

1Corresponding author.

Manuscript received May 31, 2017; final manuscript received September 12, 2017; published online November 7, 2017. Assoc. Editor: Partha P. Mukherjee. The United States Government retains, and by accepting the article for publication, the publisher acknowledges that the United States Government retains, a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work, or allow others to do so, for United States Government purposes.

J. Electrochem. En. Conv. Stor. 15(1), 011007 (Nov 07, 2017) (10 pages) Paper No: JEECS-17-1059; doi: 10.1115/1.4038244 History: Received May 31, 2017; Revised September 12, 2017

Enzymatic electrochemical cells (EECs) are a candidate for providing “green” solutions to a plethora of low-power, long-lifetime applications. A prototype three-electrode biobattery configuration of an EEC has been designed and fabricated for neutron imaging and electrochemical testing to characterize cell performance. The working electrode (WE) was catalyzed by a polymer ink-based biocatalyst with carbon felt (CF) serving as the supporting material. Results of both ex situ and in operando neutron imaging are presented as methods for relating fuel distribution, the distribution of the enzymes, and cell electrochemical performance. Neutron radiography (NR) was also performed on fuel solutions of varied concentrations to calibrate fuel solution thickness and allow for transient mapping of the fuel distribution. The calibration data proved useful in mapping the thickness of fuel solution during transient radiography. When refueled after electrochemical testing and neutron imaging, the cell surpassed its original performance, indicating that exposure to the neutron beam had not detrimentally affected enzyme activity. In operando mapping of the fuel solution suggests that increased wetting of the catalyst region increases cell performance. The relation of this performance increase to active region wetting is further supported by fuel distributions observed via the ex situ tomography. While useful in mapping aggregate solution wetting, the calibration data did not support reliable mapping of detailed glucose concentration in the WE. The results presented further demonstrate potential for the application of neutron imaging for the study of EECs, particularly with respect to mapping the distribution of aqueous fuel solutions.

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Grahic Jump Location
Fig. 1

Prototype, three-electrode cell schematic (a) and images (b), illustrating the assembly of the final cell for electrochemical testing and neutron imaging. (c) A representative radiograph of the cell prior to the introduction of any fuel, with the expanded ROI shown in (d) demonstrating the observable difference in transmission behavior between the CF and the biocatalyst ink.

Grahic Jump Location
Fig. 2

Sample slice and isosurface from reconstructed tomograms of the dry cell. (a) Shows the full field of view of the tomogram with two distinct regions indicated: region 1 and region 2. (b) Presents the cropping of (a) to region 1 with the CF and biocatalyst ink indicated with distinct intensity differences. (c) Represents (a) cropped to region 2 with the image data presented in grayscale. (d) Represents the same region as (c); however, the data are presented in binary for after the threshold was applied. (e) Shows the isosurface of the biocatalyst region and its orientation with respect to the WE holder.

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Fig. 3

Solution thickness maps for the first wetting on the left and the second wetting on the right. The solution attenuation thickness is correlated with the map via the values on the right in millimeters.

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Fig. 4

(a) Calibration image resulting from the average of the 20 individual images taken. The calibration tubes from left to right correspond to 0.05 M glucose, 0.1 M glucose, and 0.0 M glucose fuel solutions with diameters of 9.09 mm, 9.13 mm, and 9.01 mm, respectively. (b) An illustration of the chord length, c as it is referenced to a lateral distance from the centerline of the calibration cell, a, and how this is oriented with respect to the neutron flux.

Grahic Jump Location
Fig. 5

Average calibration transmission data extracted from the three sample solutions of concentration 0.1 M, 0.05 M, and 0.0 M glucose in 0.243 M sodium phosphate. The data are plotted versus chord length along with the associated fit curve determined through a standard, least squares fitting technique. The 95% confidence interval for the mean values is plotted as the two black lines displaced evenly from the mean values.

Grahic Jump Location
Fig. 6

(a) Fuel solution thickness distribution in mm calculated for the three radiographs taken at 1, 10, and 60 min after the onset of the long CA scan for the first wetting case. (b) The percent difference between the solution thickness calculated via the calibration fit curve and the solution thickness calculated through the reconstructed CT scan data for the same elapsed times. The associated scale for each set of images is shown to the right. (c) Presents the trend of the average percentage deviation of the calibrated length values from the CT scan data. The electrochemical data associated with this image data are presented in (d).

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Fig. 7

Average calibration data for all three solution concentrations imaged with the uncertainty bands presented as the shaded regions

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Fig. 8

Averaged CV results for the first wetting case shown for the state of the cell just prior to the stepped CA scan, after the stepped CA scan, and after the long discharge. The approximate locations of peak oxidation current are indicated by the diamond markers.

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Fig. 9

Average CV results for the scans take prior to and after the long discharge for both wettings. The data for the CV scan performed before and after the long discharge are shown in upper and lower series, respectively. The approximate locations of the oxidation peaks are identified by the diamond marker on each series.

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Fig. 10

(a) shows the increase in the normalized solution volume as the volumetric ROI is decreased with a shift of the left edge moving toward the right edge (i.e., x*) and the volume of enzymes normalized on the total volume of a slice present at x*. (b) Shows a radiograph of the fueled sample cell with the WE ROI identified and magnified with the definition of the reference for the left edge of the ROI, x, and the overall length, L. (c) Presents a high-level flowchart describing the process carried out to achieve the data shown in (a) with the nomenclature, CT1 and CT2, corresponding to the CT scan data for the first and second wetting cases, respectively.




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