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

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• 作者：Glenn R. Hafenstine ; Ke Ma ; Alexander W. Harris ; Omer Yehezkeli ; Eunsol Park ; Dylan W. Domaille ; Jennifer N. Cha ; Andrew P. Goodwin
• 刊名：ACS Catalysis
• 出版年：2017
• 出版时间：January 6, 2017
• 年：2017
• 卷：7
• 期：1
• 页码：568-572
• 全文大小：318K
• ISSN：2155-5435

文摘

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.