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Building carbon-carbon bonds using a biocatalytic methanol condensation cycle.


ABSTRACT: Methanol is an important intermediate in the utilization of natural gas for synthesizing other feedstock chemicals. Typically, chemical approaches for building C-C bonds from methanol require high temperature and pressure. Biological conversion of methanol to longer carbon chain compounds is feasible; however, the natural biological pathways for methanol utilization involve carbon dioxide loss or ATP expenditure. Here we demonstrated a biocatalytic pathway, termed the methanol condensation cycle (MCC), by combining the nonoxidative glycolysis with the ribulose monophosphate pathway to convert methanol to higher-chain alcohols or other acetyl-CoA derivatives using enzymatic reactions in a carbon-conserved and ATP-independent system. We investigated the robustness of MCC and identified operational regions. We confirmed that the pathway forms a catalytic cycle through (13)C-carbon labeling. With a cell-free system, we demonstrated the conversion of methanol to ethanol or n-butanol. The high carbon efficiency and low operating temperature are attractive for transforming natural gas-derived methanol to longer-chain liquid fuels and other chemical derivatives.

SUBMITTER: Bogorad IW 

PROVIDER: S-EPMC4234558 | biostudies-literature | 2014 Nov

REPOSITORIES: biostudies-literature

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Building carbon-carbon bonds using a biocatalytic methanol condensation cycle.

Bogorad Igor W IW   Chen Chang-Ting CT   Theisen Matthew K MK   Wu Tung-Yun TY   Schlenz Alicia R AR   Lam Albert T AT   Liao James C JC  

Proceedings of the National Academy of Sciences of the United States of America 20141029 45


Methanol is an important intermediate in the utilization of natural gas for synthesizing other feedstock chemicals. Typically, chemical approaches for building C-C bonds from methanol require high temperature and pressure. Biological conversion of methanol to longer carbon chain compounds is feasible; however, the natural biological pathways for methanol utilization involve carbon dioxide loss or ATP expenditure. Here we demonstrated a biocatalytic pathway, termed the methanol condensation cycle  ...[more]

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