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

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논문

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

학술지

ACS catalysis

저자명

Hafenstine, Glenn R.; Ma, Ke; Harris, Alexander W.; Yehezkeli, Omer; Park, Eunsol; Domaille, Dylan W.; Cha, Jennifer N.; Goodwin, Andrew P.

초록

<P>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 reaction, NAD<SUP>+</SUP> 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 C<SUB>8</SUB> products from C<SUB>4</SUB> alcohols under green chemistry conditions of neutral pH, low temperature, and pressure.</P><P><B>Graphic Abstract</B><BR><IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/accacs/2017/accacs.2017.7.issue-1/acscatal.6b03213/production/images/medium/cs-2016-03213f_0006.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/cs6b03213'>ACS Electronic Supporting Info</A></P>

발행연도

2017

발행기관

American Chemical Society

ISSN

2155-5435

7

1

페이지

pp.568-572

주제어

enzyme catalysis; photocatalysis; organocatalysis; green chemistry; nonequilibrium processes

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