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Multicatalytic, Light-Driven Upgrading of Butanol to 2-Ethylhexenal and Hydrogen under Mild Aqueous Conditions.


ABSTRACT: Microbes produce low-molecular-weight alcohols from sugar, but these metabolites are difficult to separate from water and possess relatively low heating values. A combination of photo-, organo-, and enzyme catalysis is shown here to convert C4 butanol (BuOH) to C8 2-ethylhexenal (2-EH) using only solar energy to drive the process. First, alcohol dehydrogenase (ADH) catalyzed the oxidation of BuOH to butyraldehyde (BA), using NAD+ as a cofactor. To prevent back reaction, NAD+ was regenerated using a platinum-seeded cadmium sulfide (Pt@CdS) photocatalyst. An amine-based organocatalyst then upgraded BA to 2-EH under mild aqueous conditions rather than harsh basic conditions in order to preserve enzyme and photocatalyst stability. The process also simultaneously increased total BuOH conversion. Thus, three disparate types of catalysts synergistically generated C8 products from C4 alcohols under green chemistry conditions of neutral pH, low temperature, and pressure.

SUBMITTER: Hafenstine GR 

PROVIDER: S-EPMC7597829 | biostudies-literature | 2017

REPOSITORIES: biostudies-literature

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Multicatalytic, Light-Driven Upgrading of Butanol to 2-Ethylhexenal and Hydrogen under Mild Aqueous Conditions.

Hafenstine Glenn R GR   Ma Ke K   Harris Alexander W AW   Yehezkeli Omer O   Park Eunsol E   Domaille Dylan W DW   Cha Jennifer N JN   Goodwin Andrew P AP  

ACS catalysis 20161219 1


Microbes produce low-molecular-weight alcohols from sugar, but these metabolites are difficult to separate from water and possess relatively low heating values. A combination of photo-, organo-, and enzyme catalysis is shown here to convert C<sub>4</sub> butanol (BuOH) to C<sub>8</sub> 2-ethylhexenal (2-EH) using only solar energy to drive the process. First, alcohol dehydrogenase (ADH) catalyzed the oxidation of BuOH to butyraldehyde (BA), using NAD<sup>+</sup> as a cofactor. To prevent back re  ...[more]

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