Bioelectrocatalytic Oxidation of Alkanes in a JP-8 Enzymatic Biofuel Cell

Ulyanova, Yevgenia; Arugula, Mary A.; Rasmussen, Michelle; Pinchon, Erica; Lindström, Ulf; Singhal, Sameer

doi:10.1021/cs500802d

Cited by 15 publications

(14 citation statements)

References 32 publications

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“…As a comparison to using the promiscuous AOx enzyme in the PEC, a more substrate-specific enzyme, ADH (alcohol dehydrogenase), was also studied. 33 While ADH is also known to perform alcohol oxidation, it is dependent on the diffusional cofactor NAD + /NADH rather than a bound FAD. 30 In the case of NAD + -dependent ADH, the reaction thermodynamics heavily favor the alcohol, requiring continuous regeneration of NAD + via NADH oxidation for increased BA production.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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

Harris

Yehezkeli

Hafenstine

et al. 2017

ACS Sustainable Chem. Eng.

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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 2ethylhexenal (2-EH). In this work, BuOH was first oxidized to n-butyraldehyde (BA) by the alcohol oxidase enzyme (AOx), concurrently generating hydrogen peroxide (H 2 O 2 ). To preserve enzyme activity and increase kinetics nearly 2-fold, the H 2 O 2 was removed by oxidation at a bismuth vanadate (BiVO 4 ) 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 lightdriven, unbiased PEC showed 3.1 ± 0.1% BuOH conversion, or ~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.

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Section: ■ Results and Discussionmentioning

confidence: 99%

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

Harris

Yehezkeli

Hafenstine

et al. 2017

ACS Sustainable Chem. Eng.

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“…The use of FAD-GDH, which is oxygen insensitive (unlike glucose oxidase) and can now be obtained commercially, has only very recently reported in combination with quinone-modified buckypapers, and promisingly, gave high catalytic currents up to 1.97 mAcm - Enzymatic biofuel cells have also been explored as portable, low-temperature and sulfurinsensitive alternatives to solid oxide fuels cells that run on JP-8 jet fuel, for example, for military applications. Minteer and coworkers exploited an enzyme cascade of alkane monooxygenase (AMO) and alcohol oxidase (AOx) at a MWCT buckypaper (Buckeye Composites) anode for mediated bioelectrocatalytic oxidation of hexane, octane, and jet fuel 67 . This study demonstrated the possibility to exploit alkanes as fuels for biofuel cells for the first time, and additionally, showed the possibility to produce power densities up to 3 mW cm -2 without pre-processing of alkane-based fuels.…”

Section: Portable Enzymatic Biofuel Cellsmentioning

confidence: 99%

1. Buckypapers for bioelectrochemical applications

Gross¹,

Holzinger²,

Cosnier³

2019

Bioelectrochemistry

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Buckypapers are self-supporting nanostructured thin films of entangled carbon nanotubes (CNTs), resembling an electronic paper, which are held together by pi-pi stacking and interweaving interactions. Richard Smalley's group first reported the formation of carbon nanotube sheets in 1998 (coining the term "bucky paper") as a method for characterizing the production quality of CNTs. 1 Carbon nanotube buckypapers and their composites have excellent prospects for a wide range of applications from aerospace materials 2 to sensors 3,4 and fuel cells 5,6 , and are thus of interest to a vast research and industrial community. Over the last 5-7 years, buckypaper materials have emerged for the construction of implantable, wearable and portable bioelectronic devices owing to their properties including high conductivity and porosity, flexibility, lightweight, biocompatibility, and the ability for electron transfer with enzymes and microbes 7 . In addition to being used for enzymatic and microbial biofuel cell construction [7][8][9] , buckypapers are also emerging for hybrid supercapacitors 10 , photoelectric biofuel cells 11 , and other bioelectronic systems including biosensors 4,12 , bioreactors 13 and biologic devices 14 .Buckypaper is the accepted term for carbon nanotube sheets, disordered or aligned, formed by vacuum filtration of aqueous (e.g. in the presence of a non-ionic surfactant such as Triton X-100) and non-aqueous dispersions (e.g. in N,N-dimethylformamide, DMF) of single-walled, double-walled and multi-walled carbon nanotubes (SWCNTs, DWCNTs, and MWCNTs) 1,6,15 . Sonication, centrifugation and additional filtration steps are also commonly used to improve the quality and purity of the CNT dispersion prior to filtration through a porous membrane 6,15 . Free-standing "lab-made" buckypaper sheets are finally obtained after washing, drying, and peeling from the underlying membrane."Commercial" buckypaper prepared by continuous manufacturing is a popular type of buckypaper.The MWCNT buckypaper from Buckeye Composites (a division of NanoTechLabs, USA) is the most widely reported commercialized buckypaper for bioelectrochemical applications [16][17][18][19] . In addition to vacuum filtration, lab-made buckypaper can also be prepared via methods including dominopushing 20 , CNT winding 21 and by using a lab-scale hand sheet former 22 . The most common type of buckypapers used in bioelectrochemistry are illustrated in Figure 1.1.Buckypaper fabrication is conceptually straightforward but factors such as dispersion homogeneity, CNT type and chemical functionality, membrane porosity, and the presence of

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“…These less traditional techniques include extraction using ionic liquids [34][35][36][37][38] and biodesulfurization using bacteria [39][40][41][42] or enzymes. 43 These techniques, while effective, are not as portable as adsorptive desulfurization, which would be ideal for eld applications.…”

Section: Current Research Directions and Adsorptive Desulfurization Fmentioning

confidence: 99%