Light-Driven Catalytic Upgrading of Butanol in a Biohybrid Photoelectrochemical System

被引:15
|
作者
Harris, Alexander W. [1 ]
Yehezkeli, Omer [1 ]
Hafenstine, Glenn R. [1 ]
Goodwin, Andrew P. [1 ,2 ]
Cha, Jennifer N. [1 ,2 ]
机构
[1] Univ Colorado, Dept Chem & Biol Engn, 3415 Colorado Ave, Boulder, CO 80303 USA
[2] Univ Colorado, Mat Sci & Engn Program, 3415 Colorado Ave, Boulder, CO 80303 USA
来源
ACS SUSTAINABLE CHEMISTRY & ENGINEERING | 2017年 / 5卷 / 09期
关键词
Bismuth vanadate; Alcohol oxidase; Aldol condensation; Green chemistry; HYDROGEN-PRODUCTION; ALCOHOL OXIDASE; PHOTOCATALYTIC REDUCTION; PICHIA-PASTORIS; BIVO4; WATER; OXIDATION; YEAST; CO2; MECHANISM;
D O I
10.1021/acssuschemeng.7b01849
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
This paper reports the design and preparation of a biohybrid photoelectrochemical cell (PEC) that can drive the tandem enzymatic oxidation and aldol condensation of n-butanol (BuOH) to C-8 2-ethylhexenal (2-EH). In this work, BuOH was first oxidized to n-butyraldehyde (BA) by the alcohol oxidase enzyme (AOx), concurrently generating hydrogen peroxide (H2O2). To preserve enzyme activity and increase kinetics nearly 2-fold, the H2O2 was removed by oxidation at a bismuth vanadate (BiVO4) photoanode. Organocatalyzed aldol condensation of C-4 BA to C-8 2-EH improved the overall BuOH conversion to 6.2 +/- 0.1% in a biased PEC after 16 h. A purely light-driven, unbiased PEC showed 3.1 +/- 0.1% BuOH conversion, or similar to 50% of that obtained from the biased system. Replacing AOx with the enzyme alcohol dehydrogenase (ADH), which requires the diffusional nicotinamide adenine dinucleotide cofactor (NAD(+)/NADH), resulted in only 0.2% BuOH conversion due to NAD(+) dimerization at the photoanode. Lastly, the application of more positive biases with the biohybrid AOx PEC led to measurable production of H-2 at the cathode, but at the cost of lower BA and 2-EH yields due to both product overoxidation and decreased enzyme activity.
引用
收藏
页码:8199 / 8204
页数:6
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