Enzymatic fuel cells via synthetic pathway biotransformation

dc.contributor.authorZhu, Zhiguangen
dc.contributor.committeechairZhang, Yi Heng Percivalen
dc.contributor.committeememberSenger, Ryan S.en
dc.contributor.committeememberLu, Changen
dc.contributor.committeememberNelson, Douglas J.en
dc.contributor.departmentBiological Systems Engineeringen
dc.date.accessioned2015-04-30T06:00:39Zen
dc.date.available2015-04-30T06:00:39Zen
dc.date.issued2013-06-11en
dc.description.abstractEnzyme-catalyzed biofuel cells would be a great alternative to current battery technology, as they are clean, safe, and capable of using diverse and abundant renewable biomass with high energy densities, at mild reaction conditions. However, currently, three largest technical challenges for emerging enzymatic fuel cell technologies are incomplete oxidation of most fuels, limited power output, and short lifetime of the cell. Synthetic pathway biotransformation is a technology of assembling a number of enzymes coenzymes for producing low-value biocommodities. In this work, it was applied to generate bioelectricity for the first time. Non-natural enzymatic pathways were developed to utilize maltodextrin and glucose in enzymatic fuel cells. Three immobilization approaches were compared for preparing enzyme electrodes. Thermostable enzymes from thermophiles were cloned and expressed for improving the lifetime and stability of the cell. To further increase the power output, non-immobilized enzyme system was demonstrated to have higher power densities compared to those using immobilized enzyme system, due to better mass transfer and retained native enzyme activities. With the progress on pathway development and power density/stability improvement in enzymatic fuel cells, a high energy density sugar-powered enzymatic fuel cell was demonstrated. The enzymatic pathway consisting of 13 thermostable enzymes enabled the complete oxidation of glucose units in maltodextrin to generate 24 electrons, suggesting a high energy density of such enzymatic fuel cell (300 Wh/kg), which was several folds higher than that of a lithium-ion battery. Maximum power density was 0.74 mW/cm2 at 50 deg C and 20 mM fuel concentration, which was sufficient to power a digital clock or a LED light. These results suggest that enzymatic fuel cells via synthetic pathway biotransformation could achieve high energy density, high power density and increased lifetime. Future efforts should be focused on further increasing power density and enzyme stability in order to make enzymatic fuel cells commercially applicable.en
dc.description.degreePh. D.en
dc.format.mediumETDen
dc.identifier.othervt_gsexam:984en
dc.identifier.urihttp://hdl.handle.net/10919/51948en
dc.publisherVirginia Techen
dc.rightsIn Copyrighten
dc.rights.urihttp://rightsstatements.org/vocab/InC/1.0/en
dc.subjectenzymatic fuel cellsen
dc.subjectbioelectricityen
dc.subjectsynthetic pathway biotransformationen
dc.subjectenzymatic pathwayen
dc.subjectenergy densityen
dc.subjectpower densityen
dc.titleEnzymatic fuel cells via synthetic pathway biotransformationen
dc.typeDissertationen
thesis.degree.disciplineBiological Systems Engineeringen
thesis.degree.grantorVirginia Polytechnic Institute and State Universityen
thesis.degree.leveldoctoralen
thesis.degree.namePh. D.en

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