Biological conversion of carbon dioxide and hydrogen into liquid fuels and industrial chemicals

Hawkins, Aaron S.; McTernan, Patrick M.; Lian, Hong; Kelly, Robert M.; Adams, Michael W. W.

doi:10.1016/j.copbio.2013.02.017

Cited by 89 publications

(52 citation statements)

References 71 publications

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“…Here, the recombinant expression and characterization of two enzymes in the final steps of the 3HP/4HB pathway are reported and in vitro production of acetate from 4HB is confirmed. The level of biochemical detail of the 3HP/4HB pathway in relationship to the central metabolism continues to develop, which will inform future metabolic engineering prospects for microbial biosynthesis of fuels and organic chemicals (33).…”

Section: Figmentioning

confidence: 99%

Conversion of 4-Hydroxybutyrate to Acetyl Coenzyme A and Its Anapleurosis in the Metallosphaera sedula 3-Hydroxypropionate/4-Hydroxybutyrate Carbon Fixation Pathway

Hawkins

Adams

Kelly

2014

Appl Environ Microbiol

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The extremely thermoacidophilic archaeon Metallosphaera sedula (optimum growth temperature, 73°C, pH 2.0) grows chemolithoautotrophically on metal sulfides or molecular hydrogen by employing the 3-hydroxypropionate/4-hydroxybutyrate (3HP/ 4HB) carbon fixation cycle. This cycle adds two CO 2 molecules to acetyl coenzyme A (acetyl-CoA) to generate 4HB, which is then rearranged and cleaved to form two acetyl-CoA molecules. Previous metabolic flux analysis showed that two-thirds of central carbon precursor molecules are derived from succinyl-CoA, which is oxidized to malate and oxaloacetate. The remaining onethird is apparently derived from acetyl-CoA. As such, the steps beyond succinyl-CoA are essential for completing the carbon fixation cycle and for anapleurosis of acetyl-CoA. Here, the final four enzymes of the 3HP/4HB cycle, 4-hydroxybutyrate-CoA ligase (AMP forming) (Msed_0406), 4-hydroxybutyryl-CoA dehydratase (Msed_1321), crotonyl-CoA hydratase/(S)-3-hydroxybutyrylCoA dehydrogenase (Msed_0399), and acetoacetyl-CoA ␤-ketothiolase (Msed_0656), were produced recombinantly in Escherichia coli, combined in vitro, and shown to convert 4HB to acetyl-CoA. Metabolic pathways connecting CO 2 fixation and central metabolism were examined using a gas-intensive bioreactor system in which M. sedula was grown under autotrophic (CO 2 -limited) and heterotrophic conditions. Transcriptomic analysis revealed the importance of the 3HP/4HB pathway in supplying acetyl-CoA to anabolic pathways generating intermediates in M. sedula metabolism. The results indicated that flux between the succinate and acetyl-CoA branches in the 3HP/4HB pathway is governed by 4-hydroxybutyrate-CoA ligase, possibly regulated posttranslationally by the protein acetyltransferase (Pat)/Sir2-dependent system. Taken together, this work confirms the final four steps of the 3HP/4HB pathway, thereby providing the framework for examining connections between CO 2 fixation and central metabolism in M. sedula. Metallosphaera sedula is an extremely thermoacidophilic archaeon (optimum growth temperature, 73°C, and optimum pH, 2.0) that grows heterotrophically on peptides and chemolithoautotrophically on metal sulfides or hydrogen gas (1). For chemolithotrophic growth, it uses a unique carbon fixation pathway known as the 3-hydroxypropionate/4-hydroxybutyrate (3HP/4HB) cycle (2), so far found only in members of the order Sulfolobales. This cycle is one of two such cycles found exclusively in thermophilic archaea, the other being the dicarboxylate/4-hydroxybutyrate (DC/4HB) cycle present in the orders Desulfurococcales and Thermoproteales (3-5). In the first part of the 3HP/4HB cycle, acetyl coenzyme A (CoA) (C 2 ) is converted into succinylCoA (C 4 ) by two successive carboxylation steps (5-7). In the second half of this cycle, succinyl-CoA is then converted to 4HB, which is rearranged and cleaved to produce two molecules of acetyl-CoA. Both the 3HP/4HB and DC/4HB cycles use the same set of enzymes to convert succinyl-CoA to acetyl-CoA. However, the enzymes used in ...

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Section: Figmentioning

confidence: 99%

Conversion of 4-Hydroxybutyrate to Acetyl Coenzyme A and Its Anapleurosis in the Metallosphaera sedula 3-Hydroxypropionate/4-Hydroxybutyrate Carbon Fixation Pathway

Hawkins

Adams

Kelly

2014

Appl Environ Microbiol

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“…CO 2 is an attractive building block for C 1 -chemistry; however, the conversion of CO 2 is quite challenging due to its inert and stable nature. Several methods for the activation and conversion of CO 2 have been proposed, such as chemical [5], biological [6], photochemical [7,8], and electrochemical methods [9][10][11][12]. Among these technologies, the electrochemical method is the most promising and benign, owing to its convenient operation and ability to control the yield and selectivity of the produced chemicals.…”

Section: Introductionmentioning

confidence: 99%

Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO₂ Conversion and H₂ Production

Choi

Jung

Yoo

et al. 2017

Journal of Electrochemical Science and Technology

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Electrochemical conversion of CO 2 and production of H 2 were attempted on a three-dimensionally ordered, porous metal organic framework (MOF-74) in which transition metals (Co, Ni, and Zn) were impregnated. A lab-scale proton exchange membrane-based electrolyzer was fabricated and used for the reduction of CO 2 . Real-time gas chromatography enabled the instantaneous measurement of the amount of carbon monoxide and hydrogen produced. Comprehensive calculations, based on electrochemical measurements and gaseous product analysis, presented a time-dependent selectivity of the produced gases. M-MOF-74 samples with different central metals were successfully obtained because of the simple synthetic process. It was revealed that Co-and Ni-MOF-74 selectively produce hydrogen gas, while Zn-MOF-74 successfully generates a mixture of carbon monoxide and hydrogen. The results indicated that M-MOF-74 can be used as an electrocatalyst to selectively convert CO 2 into useful chemicals.

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“…lants capture photons from sunlight to fix carbon dioxide into sugars via the Calvin cycle, and they deposit most of the carbohydrates onto plant cell walls (1). Plant cell walls are major constituents of what is commonly defined as biomass, a huge component of all terrestrial habitats that is mostly represented by the cell walls of dead plants, trees, grasses, and leftovers of actively managed croplands.…”

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confidence: 99%

Genomics Review of Holocellulose Deconstruction by Aspergilli

Segato

Damásio

Lucas

et al. 2014

Microbiol Mol Biol Rev

115

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SUMMARY Biomass is constructed of dense recalcitrant polymeric materials: proteins, lignin, and holocellulose, a fraction constituting fibrous cellulose wrapped in hemicellulose-pectin. Bacteria and fungi are abundant in soil and forest floors, actively recycling biomass mainly by extracting sugars from holocellulose degradation. Here we review the genome-wide contents of seven Aspergillus species and unravel hundreds of gene models encoding holocellulose-degrading enzymes. Numerous apparent gene duplications followed functional evolution, grouping similar genes into smaller coherent functional families according to specialized structural features, domain organization, biochemical activity, and genus genome distribution. Aspergilli contain about 37 cellulase gene models, clustered in two mechanistic categories: 27 hydrolyze and 10 oxidize glycosidic bonds. Within the oxidative enzymes, we found two cellobiose dehydrogenases that produce oxygen radicals utilized by eight lytic polysaccharide monooxygenases that oxidize glycosidic linkages, breaking crystalline cellulose chains and making them accessible to hydrolytic enzymes. Among the hydrolases, six cellobiohydrolases with a tunnel-like structural fold embrace single crystalline cellulose chains and cooperate at nonreducing or reducing end termini, splitting off cellobiose. Five endoglucanases group into four structural families and interact randomly and internally with cellulose through an open cleft catalytic domain, and finally, seven extracellular β-glucosidases cleave cellobiose and related oligomers into glucose. Aspergilli contain, on average, 30 hemicellulase and 7 accessory gene models, distributed among 9 distinct functional categories: the backbone-attacking enzymes xylanase, mannosidase, arabinase, and xyloglucanase, the short-side-chain-removing enzymes xylan α-1,2-glucuronidase, arabinofuranosidase, and xylosidase, and the accessory enzymes acetyl xylan and feruloyl esterases.

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Biological conversion of carbon dioxide and hydrogen into liquid fuels and industrial chemicals

Cited by 89 publications

References 71 publications

Conversion of 4-Hydroxybutyrate to Acetyl Coenzyme A and Its Anapleurosis in the Metallosphaera sedula 3-Hydroxypropionate/4-Hydroxybutyrate Carbon Fixation Pathway

Conversion of 4-Hydroxybutyrate to Acetyl Coenzyme A and Its Anapleurosis in the Metallosphaera sedula 3-Hydroxypropionate/4-Hydroxybutyrate Carbon Fixation Pathway

Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO₂ Conversion and H₂ Production

Genomics Review of Holocellulose Deconstruction by Aspergilli

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Biological conversion of carbon dioxide and hydrogen into liquid fuels and industrial chemicals

Cited by 89 publications

References 71 publications

Conversion of 4-Hydroxybutyrate to Acetyl Coenzyme A and Its Anapleurosis in the Metallosphaera sedula 3-Hydroxypropionate/4-Hydroxybutyrate Carbon Fixation Pathway

Conversion of 4-Hydroxybutyrate to Acetyl Coenzyme A and Its Anapleurosis in the Metallosphaera sedula 3-Hydroxypropionate/4-Hydroxybutyrate Carbon Fixation Pathway

Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO2 Conversion and H2 Production

Genomics Review of Holocellulose Deconstruction by Aspergilli

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Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO₂ Conversion and H₂ Production