New Bioanodes: Truncated Hydride Carrier Coenzymes and Electrochemistry.

摘要

The long-term goal of this project was to develop novel biofuel cells suitable for energy harvesting and low-level power generation. The original objectives, in collaboration with Cass (Imperial College, UK), Ellington (Texas) , and Bugg (Warwick University, UK), were to develop synthetic, cost-effective and more stable analogs of NADH which could be used in conjunction with a protein-engineered dehydrogenase enzyme to provide the electrochemical basis of a novel bioanode for use in a biofuel cell. The plan was to synthesize a series of NADH analogs of increasing complexity (Bugg) and then use this series of analogs in conjunction with protein evolution studies to develop engineered dehydrogenase enzymes that are capable of utilizing these molecules in place of NADH (Cass and Ellington). The mechanism of the electrochemical oxidation of these NADH analogs at chemically modified electrodes was studied and efficient electrodes developed for use in conjunction with the modified enzymes as the anode of a biofuel cell. Methods for the immobilization of the NADH analogs onto electrode surfaces and the resulting electrochemistry of the immobilized molecules also were studied. (4 tables, 51 figures, 41 refs.).