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Preparation of hybrid multi-catalyst architecture containing enzyme, organic catalyst and carbon nanotubes modified for complete ethanol electrochemical oxidation

Grant number: 18/24180-1
Support Opportunities:Scholarships abroad - Research Internship - Post-doctor
Effective date (Start): March 01, 2019
Effective date (End): February 29, 2020
Field of knowledge:Physical Sciences and Mathematics - Chemistry - Physical-Chemistry
Principal Investigator:Adalgisa Rodrigues de Andrade
Grantee:Jefferson Honorio Franco
Supervisor: Shelley Dawn Minteer
Host Institution: Faculdade de Filosofia, Ciências e Letras de Ribeirão Preto (FFCLRP). Universidade de São Paulo (USP). Ribeirão Preto , SP, Brazil
Research place: University of Utah (U), United States  
Associated to the scholarship:17/20431-7 - Development of hybrid enzymatic cascade to produce an efficient ethanol/O2 biofuel cell, BP.PD


Biofuel cell provides a means to obtain clean, renewable energy and has potential for future use as an alternative energy source for low-power electronic devices. The characteristics of enzymatic biofuel cells are quite promising, however, they still present several challenges. Thus, some adjustments in these devices are important objects of research, such as: (1) increase in the generated energy, (2) increase of electronic conductivity into the biofilms. One way to enhance the electrocatalytic activity of the biosystem and also extend its service life is preparation of hybrid catalysts mixing enzymes with organic oxidation catalysts. In the first year of this post-doctorate project supported by FAPESP, we first report the preparation of dehydrogenase enzymatic system containing ADH and Aldh enzymes immobilized at the surface of a carbon support. Acetaldehyde (2 electrons transfer) and acetate (4 electron transfer) were the products generated during biooxidation of ethanol by HPLC. Another article published this years reports a tri-catalytic hybrid electrode system containing carbon canotubes (MWCNT-COOH), the two dehydrogenase enzymes (ADH and Aldh) and a organic catalyst (TEMPO-LPEI) for complete ethanol oxidation. We improve the harvest of electrons preparing bioelectrooxidation onto a carbon paper support comproving that the tri-catalytic hybrid electrode system is able to oxidize ethanol to CO2 by collecting 12 electrons from ethanol. Recently, we developed a biofuel cell in a hybrid system containing carbon nanotubes (MWCNT/COOH), the organic oxidation catalyst TEMPO-LPEI and the enzyme oxalate oxidase (OxOx) employing ethanol as substrate. Given the challenges associated with the acetate intermediate C-C bond cleavage, the design of a hybrid BFC proposed corroborates for complete ethanol oxidation to CO2. Now, after the publication of these articles of high impact, in addition to the promising results obtained recently (paper in preparation), we plan one year with BEPE project at University of Utah under supervision of Prof. Dr. Shelley Minteer, renowned expert in the field of biofuel cells. This BEPE Project aims to acquire the knowledge in preparation of organic oxidation catalyst, TEMPO-LPEI, learn how to isolate and purify the oxalate decarboxylase enzyme (OxDc) from Bacillus subtilis, which provides advantages in terms of cost and extends the possibilities for future enzymatic engineering and prepare a 3-D catalyst modifing nanotubes with pyrene derivatives (Pyrene / MWCNT) in order to obtain a diferent and sophisticated hybrid system (Pyrene / MWCNT, TEMPO-LPEI), more efficient than hybrid systems previously reported, capable to improve the BFC power density and generate a rapid and complete ethanol oxidation to CO2 achieving high electrochemical oxidation rates and energy production.

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Scientific publications (4)
(References retrieved automatically from Web of Science and SciELO through information on FAPESP grants and their corresponding numbers as mentioned in the publications by the authors)
FRANCO, JEFFERSON HONORIO; GRATTIERI, MATTEO; DE ANDRADE, ADALGISA R.; MINTEER, SHELLEY D.. Unveiling complete lactate oxidation through a hybrid catalytic cascade. Electrochimica Acta, v. 376, . (18/24180-1, 17/20431-7)
FRANCO, JEFFERSON HONORIO; KLUNDER, KEVIN J.; LEE, JACK; RUSSELL, VICTORIA; DE ANDRADE, ADALGISA R.; MINTEER, SHELLEY D.. Enhanced electrochemical oxidation of ethanol using a hybrid catalyst cascade architecture containing pyrene-TEMPO, oxalate decarboxylase and carboxylated multi-walled carbon nanotube. BIOSENSORS & BIOELECTRONICS, v. 154, . (17/20431-7, 18/24180-1)
FRANCO, JEFFERSON HONORIO; BONALDO, JOAO VICTOR; MINTEER, SHELLEY D.; DE ANDRADE, ADALGISA R.. Assembly of an improved hybrid cascade system for complete ethylene glycol oxidation: Enhanced catalytic performance for an enzymatic biofuel cell. BIOSENSORS & BIOELECTRONICS, v. 216, p. 9-pg., . (18/24180-1, 17/20431-7)
FRANCO, JEFFERSON HONORIO; MINTEER, SHELLEY D.; DE ANDRADE, ADALGISA R.. Ethanol Biofuel Cells: Hybrid Catalytic Cascades as a Tool for Biosensor Devices. BIOSENSORS-BASEL, v. 11, n. 2, . (17/20431-7, 18/24180-1)

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