Integrated Electromicrobial Conversion of CO
            <sub>2</sub>
            to Higher Alcohols

Li, Han; Opgenorth, Paul H.; Wernick, David G.; Rogers, Sue; Wu, Tsai‐Fu; Higashide, Wendy; Malati, Peter; Huo, Yi-Xin; Cho, Kwang Myung; Liao, James C.

doi:10.1126/science.1217643

Cited by 654 publications

(468 citation statements)

References 23 publications

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“…Second, it should be possible to repurpose microbial microcompartments such as the carboxysome, which have evolved to harbor pathways with reactive one-to-twocarbon components, now that the targeting signals for directing enzymes to these compartments are becoming better understood (22)(23)(24). Once in vivo metabolic activity of the pathway is established, the formolase pathway could be further extended to use CO 2 as a sole carbon and energy source through the electrochemical reduction of CO 2 into formate (25).…”

Section: Discussionmentioning

confidence: 99%

Computational protein design enables a novel one-carbon assimilation pathway

Siegel¹,

Smith²,

Poust

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

325

255

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We describe a computationally designed enzyme, formolase (FLS), which catalyzes the carboligation of three one-carbon formaldehyde molecules into one three-carbon dihydroxyacetone molecule. The existence of FLS enables the design of a new carbon fixation pathway, the formolase pathway, consisting of a small number of thermodynamically favorable chemical transformations that convert formate into a three-carbon sugar in central metabolism. The formolase pathway is predicted to use carbon more efficiently and with less backward flux than any naturally occurring one-carbon assimilation pathway. When supplemented with enzymes carrying out the other steps in the pathway, FLS converts formate into dihydroxyacetone phosphate and other central metabolites in vitro. These results demonstrate how modern protein engineering and design tools can facilitate the construction of a completely new biosynthetic pathway.computational protein design | pathway engineering | carbon fixation N ovel strategies are needed to address current challenges in energy storage and carbon sequestration. One approach is to engineer biological systems to convert one-carbon compounds into multicarbon molecules such as fuels and other high value chemicals. Many synthetic pathways to produce value-added chemicals from common feedstocks, such as glucose, have been constructed in organisms that lack one-carbon anabolic pathways, such as Escherichia coli or Saccharomyces cerevisiae (1-3); however, despite considerable effort, it has been difficult to introduce heterologous one-carbon fixing pathways into these organisms (4). Likely problems include the inherent complexity, environmental sensitivity, inefficiency, or unfavorable chemical driving force of naturally occurring one-carbon metabolic pathways (5).An optimal pathway for one-carbon utilization in common synthetic biology platforms would be (i) composed of a minimal number of enzymes, (ii) linear and disconnected from other metabolic pathways, (iii) thermodynamically favorable with a significant driving force at most or all steps, and (iv) capable of functioning in a robust manner under both aerobic and anaerobic conditions (5). A pathway with these properties could enable the assimilation of one-carbon molecules as the sole carbon source for the production of fuels and chemicals. Although no such pathway is known in nature, the established electrochemical reduction of carbon dioxide to formate under ambient temperatures and pressures in neutral aqueous solutions provides an attractive starting point for a onecarbon fixation pathway (5-8).We describe the computational design of an enzyme that catalyzes the carboligation of three one-carbon molecules into a single three-carbon molecule. This enzyme enables the construction of a new pathway, the formolase pathway, in which formate is converted into the central metabolite dihydroxyacetone phosphate (DHAP; Fig. 1). The use of computational protein design to reengineer catalytic activities opens up the pathway design space beyond that available based o...

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Section: Discussionmentioning

confidence: 99%

Computational protein design enables a novel one-carbon assimilation pathway

Siegel¹,

Smith²,

Poust

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

325

255

View full text Add to dashboard Cite

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“…Furthermore, Li et al. presented the utilization of electromicrobial systems for CO 2 reduction and showed the conversion of CO 2 to higher alcohols by using genetically modified Ralstonia eutropha H16 38. Recently, Jiang et al.…”

Section: Introductionmentioning

confidence: 99%

Bio‐Electrocatalytic Application of Microorganisms for Carbon Dioxide Reduction to Methane

et al. 2016

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We present a study on a microbial electrolysis cell with methanogenic microorganisms adapted to reduce CO2 to CH4 with the direct injection of electrons and without the artificial addition of H2 or an additional carbon source except gaseous CO2. This is a new approach in comparison to previous work in which both bicarbonate and gaseous CO2 served as the carbon source. The methanogens used are known to perform well in anaerobic reactors and metabolize H2 and CO2 to CH4 and water. This study shows the biofilm formation of those microorganisms on a carbon felt electrode and the long‐term performance for CO2 reduction to CH4 using direct electrochemical reduction. CO2 reduction is performed simply by electron uptake with gaseous CO2 as the sole carbon source in a defined medium. This “electrometabolism” in such microbial electrolysis cells depends strongly on the potential applied as well as on the environmental conditions. We investigated the performance using different adaption mechanisms and a constant potential of −700 mV vs. Ag/AgCl for CH4 generation at 30–35 °C. The experiments were performed by using two‐compartment electrochemical cells. Production rates with Faradaic efficiencies of around 22 % were observed.

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“…The reduction of carbon dioxide in BESs may be a promising way to simultaneously reduce carbon dioxide emissions and generate fuels or other organic compounds [3,9,11,13,18,19,28], which is significant in terms of the environment, energy, and resources.…”

Section: Introductionmentioning

confidence: 99%

Production of Acetate from Carbon Dioxide in Bioelectrochemical Systems Based on Autotrophic Mixed Culture

Jiang²,

2013

J. Microbiol. Biotechnol.

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Integrated Electromicrobial Conversion of CO ₂ to Higher Alcohols

Abstract: An engineered microbe transforms carbon dioxide into a prospective liquid fuel in tandem with electrical power rather than light.

Cited by 654 publications

References 23 publications

Computational protein design enables a novel one-carbon assimilation pathway

Computational protein design enables a novel one-carbon assimilation pathway

Bio‐Electrocatalytic Application of Microorganisms for Carbon Dioxide Reduction to Methane

Production of Acetate from Carbon Dioxide in Bioelectrochemical Systems Based on Autotrophic Mixed Culture

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Integrated Electromicrobial Conversion of CO 2 to Higher Alcohols

Abstract: An engineered microbe transforms carbon dioxide into a prospective liquid fuel in tandem with electrical power rather than light.

Cited by 654 publications

References 23 publications

Computational protein design enables a novel one-carbon assimilation pathway

Computational protein design enables a novel one-carbon assimilation pathway

Bio‐Electrocatalytic Application of Microorganisms for Carbon Dioxide Reduction to Methane

Production of Acetate from Carbon Dioxide in Bioelectrochemical Systems Based on Autotrophic Mixed Culture

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Product

Resources

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Integrated Electromicrobial Conversion of CO ₂ to Higher Alcohols