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Illustrating the Mass Transport Effect on Enzyme Cascade Reaction Kinetics Using a Rotating Ring Disk Electrode Zeng-Qiang Wu, Jun-Jun Liu, Jin-Yi Li, Dan Xu, and Xing-Hua Xia Anal. Chem., Just Accepted Manuscript • DOI: 10.1021/acs.analchem.7b03780 • Publication Date (Web): 07 Nov 2017 Downloaded from http://pubs.acs.org on November 8, 2017
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Analytical Chemistry
Illustrating the Mass Transport Effect on Enzyme Cascade Reaction Kinetics Using a Rotating Ring Disk Electrode Zeng-Qiang Wu‡, Jun-Jun Liu‡, Jin-Yi Li, Dan Xu, Xing-Hua Xia* State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210093, China. *Email:
[email protected] Tel: +86-025-89687436
ABSTRACT: Electrochemical biosensors based on enzymatic reaction have been applied into a wide range of fields. As the trend continues to grow, these biosensors are approaching to the limit imposed by physics and chemistry. To further improve the performance of the biosensors, the interplay of mass transport and enzymatic reaction kinetics, especially in the enzyme cascade systems, should be considered at the design of biosensors. Herein, we propose a simple approach to the studying on the influence of mass transport and enzyme molecules motion on the kinetics of enzyme cascade reactions. β-galactosidase (β-Gal) and glucose oxidase (GOx) of the enzyme cascade reaction are precisely immobilized onto the disk and ring electrodes of rotating ring disk electrode (RRDE) via covalent attachment method, respectively. At a low rotating speed (600 rpm in the present case), the kinetics control and product inhibition effect of enzymatic catalytic reaction become obvious, resulting in decreased activity of enzymes and in turn the kinetics of enzyme cascade reaction. Thus, the highest kinetics of the enzyme cascade reaction can be achieved at intermediate rotating speed (e.g., 600 rpm) where difference between the positive contribution from convective flow and enzymatic catalytic reaction reaches maximum. In addition, the conformation change of the enzymes caused by larger centrifugal force might not be neglected, which would also result in a decrease of the enzymes activity. The present RRDE approach may help in exploring the influence of centrifugal force on the conformation change of proteins which is undergoing in our group.
ASSOCIATED CONTENT Supporting Information The detailed information for additional experiments and theory section is available free of charge on the ACS Publications website, which includes the preparation of cascade enzymes modified electrode, the optimization of experimental condition, the collect efficiency of enzyme modified electrode and FEM simulation. Supporting information (PDF)
AUTHOR INFORMATION Corresponding Author * E-mail:
[email protected] (X.H. Xia)
Author Contributions ‡These authors contributed equally.
ACKNOWLEDGMENT This work was supported by grants from the National Natural Science Foundation of China (21775066, 21327902, 21635004, 21627806). We also gratefully acknowledge the HPCC (High-Performance Computing Center) of Nanjing University.
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Figure 3. Simulated concentration profiles of H2O2 (a) of the βGal/GOx cascade reaction at rotating speeds of 200, 600 and 1600 rpm. (b) Simulated ring electrode current of H2O2 generated from the cascade reaction with 30 mM lactose versus rotating speed.
CONCLUSION In summary, we propose a novel strategy to explore the mass transport effect on the kinetics of β-Gal/GOx cascade reaction
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