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Published on: October 25, 2018
Control of bioelectrocatalytic transformations on DNA scaffolds
Gilad Piperberg1, Ofer I Wilner, Omer Yehezkeli
1Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
Journal of the American Chemical Society
|June 10, 2009
Summary
Programmed biocatalytic transformations are achieved by organizing biomolecules on DNA scaffolds. Precise positioning of glucose oxidase and electron mediators on DNA enables controlled glucose oxidation and hydrogen peroxide reduction, demonstrating spatial control in bioelectrocatalysis.
Area of Science:
- Bioelectrochemistry
- Nanobiotechnology
- Enzyme catalysis
Background:
- DNA scaffolds enable precise spatial arrangement of biomolecules.
- Controlled positioning of enzymes and mediators is crucial for bioelectrocatalytic efficiency.
- Electrode-linked systems offer platforms for studying and utilizing biocatalytic processes.
Purpose of the Study:
- To demonstrate programmed biocatalytic transformations using spatially organized biomolecules on a DNA scaffold.
- To investigate the effect of molecular arrangement on enzyme activity and electron transfer.
- To establish a controllable bioelectrocatalytic system for glucose oxidation and hydrogen peroxide reduction.
Main Methods:
- Immobilization of glucose oxidase (GOx) and ferrocene-based electron mediators on a DNA scaffold linked to an electrode.
- Hybridization of nucleic acid-functionalized biomolecules to specific sites on the DNA scaffold.
- Electrochemical measurements to monitor biocatalytic activity and electron transfer.
- Systematic exchange of biomolecule positions to assess spatial dependency.
Main Results:
- Ferrocene-mediated oxidation of GOx and subsequent glucose oxidation were activated when GOx was positioned remotely from the electrode and the mediator adjacent.
- Reversing the positions of GOx and the mediator abolished glucose bioelectrocatalytic oxidation.
- In a coupled system, glucose oxidase-catalyzed glucose oxidation producing H(2)O(2) was effectively coupled with microperoxidase-11 (MP-11) catalyzed H(2)O(2) reduction when MP-11 was adjacent to the electrode.
- The bioelectrocatalytic cathodic currents were tunable by glucose concentration, and reversing MP-11 and GOx positions eliminated H(2)O(2) reduction.
Conclusions:
- The spatial organization of biomolecules on DNA scaffolds is critical for programmed biocatalytic transformations.
- Precise positioning of enzymes and electron mediators dictates the efficiency and occurrence of bioelectrocatalytic reactions.
- This study establishes a versatile platform for designing sophisticated bioelectrocatalytic systems with spatial control.
