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Issue 26, 2014
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Effect of enzymatic orientation through the use of syringaldazine molecules on multiple multi-copper oxidase enzymes

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Abstract

The effect of proper enzyme orientation at the electrode surface was explored for two multi-copper oxygen reducing enzymes: Bilirubin Oxidase (BOx) and Laccase (Lac). Simultaneous utilization of “tethering” agent (1-pyrenebutanoic acid, succinimidyl ester; PBSE), for stable enzyme immobilization, and syringaldazine (Syr), for enzyme orientation, of both Lac and BOx led to a notable enhancement of the electrode performance. For Lac cathodes tested in solution it was established that PBSE–Lac and PBSE–Syr–Lac modified cathodes demonstrated approximately 6 and 9 times increase in current density, respectively, compared to physically adsorbed and randomly oriented Lac cathodes. Further testing in solution utilizing BOx showed an even higher increase in achievable current densities, thus BOx was chosen for additional testing in air-breathing mode. In subsequent air-breathing experiments the incorporation of PBSE and Syr with BOx resulted in current densities of 0.65 ± 0.1 mA cm−2; 2.5 times higher when compared to an unmodified BOx cathode. A fully tethered/oriented BOx cathode was combined with a NAD-dependent Glucose Dehydrogenase anode for the fabrication of a complete enzymatic membraneless fuel cell. A maximum power of 1.03 ± 0.06 mW cm−2 was recorded for the complete fuel cell. The observed significant enhancement in the performance of “oriented” cathodes was a result of proper enzyme orientation, leading to facilitated enzyme/electrode interface interactions.

Graphical abstract: Effect of enzymatic orientation through the use of syringaldazine molecules on multiple multi-copper oxidase enzymes

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Publication details

The article was received on 25 Mar 2014, accepted on 15 May 2014 and first published on 30 May 2014


Article type: Paper
DOI: 10.1039/C4CP01296H
Author version available: Download Author version (PDF)
Citation: Phys. Chem. Chem. Phys., 2014,16, 13367-13375
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    Effect of enzymatic orientation through the use of syringaldazine molecules on multiple multi-copper oxidase enzymes

    Y. Ulyanova, S. Babanova, E. Pinchon, I. Matanovic, S. Singhal and P. Atanassov, Phys. Chem. Chem. Phys., 2014, 16, 13367
    DOI: 10.1039/C4CP01296H

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