Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 112, Issue 16, Pages 4964-4969Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1417719112
Keywords
hydrogen; biomass; in vitro metabolic engineering; metabolic network modeling; global sensitivity analysis
Categories
Funding
- Virginia Tech Biological Systems Engineering Department
- Shell GameChanger Program
- Virginia Tech CALS Biodesign and Bioprocessing Research Center
- National Science Foundation (NSF) [STTR I (IIP-1321528), SBIR II (IIP-1353266)]
- Department of Energy [STTR I (IIP-1321528)]
- Department of Defense through the National Defense Science and Engineering Graduate Fellowship Program
- Institute for Critical Technology and Applied Science Scholar Program
- NSF's Research Experience for Undergraduates program
- Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences of the US Department of Energy [DE-FG05-95ER20175]
- Virginia Agricultural Experiment Station
- Hatch Program of the National Institute of Food and Agriculture, US Department of Agriculture
- Div Of Engineering Education and Centers
- Directorate For Engineering [1156645] Funding Source: National Science Foundation
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The use of hydrogen (H-2) as a fuel offers enhanced energy conversion efficiency and tremendous potential to decrease greenhouse gas emissions, but producing it in a distributed, carbon-neutral, low-cost manner requires new technologies. Herein we demonstrate the complete conversion of glucose and xylose from plant biomass to H-2 and CO2 based on an in vitro synthetic enzymatic pathway. Glucose and xylose were simultaneously converted to H-2 with a yield of two H-2 per carbon, the maximum possible yield. Parameters of a nonlinear kinetic model were fitted with experimental data using a genetic algorithm, and a global sensitivity analysis was used to identify the enzymes that have the greatest impact on reaction rate and yield. After optimizing enzyme loadings using this model, volumetric H-2 productivity was increased 3-fold to 32 mmol H-2.L-1.h(-1). The productivity was further enhanced to 54 mmol H-2.L-1.h(-1) by increasing reaction temperature, substrate, and enzyme concentrations-an increase of 67-fold compared with the initial studies using this method. The production of hydrogen from locally produced biomass is a promising means to achieve global green energy production.
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