Assembly of an improved hybrid cascade system for complete ethylene glycol oxidation: Enhanced catalytic performance for an enzymatic biofuel cell

Jefferson Honorio Franco; João Victor Bonaldo; Shelley D Minteer; Adalgisa R De Andrade

doi:10.1016/j.bios.2022.114649

Assembly of an improved hybrid cascade system for complete ethylene glycol oxidation: Enhanced catalytic performance for an enzymatic biofuel cell

Biosens Bioelectron. 2022 Nov 15:216:114649. doi: 10.1016/j.bios.2022.114649. Epub 2022 Aug 27.

Authors

Jefferson Honorio Franco¹, João Victor Bonaldo², Shelley D Minteer³, Adalgisa R De Andrade⁴

Affiliations

¹ Department of Chemistry, Faculty of Philosophy Sciences and Letters at Ribeirão Preto, University of São Paulo, 14040-901, Ribeirão Preto, SP, Brazil; UNESP, National Institute for Alternative Technologies of Detection, Toxicological Evaluation and Removal of Micropollutants and Radioactives (INCT-DATREM), Institute of Chemistry, P.O. Box 355, 14800-900, Araraquara, SP, Brazil.
² Department of Chemistry, Faculty of Philosophy Sciences and Letters at Ribeirão Preto, University of São Paulo, 14040-901, Ribeirão Preto, SP, Brazil.
³ Department of Chemistry, University of Utah, Salt Lake City, UT, 84112, United States.
⁴ Department of Chemistry, Faculty of Philosophy Sciences and Letters at Ribeirão Preto, University of São Paulo, 14040-901, Ribeirão Preto, SP, Brazil; UNESP, National Institute for Alternative Technologies of Detection, Toxicological Evaluation and Removal of Micropollutants and Radioactives (INCT-DATREM), Institute of Chemistry, P.O. Box 355, 14800-900, Araraquara, SP, Brazil. Electronic address: ardandra@usp.br.

PMID: 36055133
DOI: 10.1016/j.bios.2022.114649

Abstract

We report an Enzymatic Fuel Cell (EFC) combining an enzyme that can cleave carbon-carbon bonds (oxalate oxidase (OxOx)) with an organic catalyst (Pyrene-TEMPO (TEMPO = 2,2,6,6-tetramethyl piperidinyl-N-oxyl)) immobilized on the surface of modified carboxylated multi-walled carbon nanotubes (MWCNT-COOH). This combination gave a hybrid bi-catalyst electrode for complete ethylene glycol (EG) oxidation. The hybrid electrode provided ninefold enhanced catalytic activity (0.17 ± 6 × 10^-3 mA cm^-2) in the presence of EG as compared to the electrode in the absence of EG (0.018 ± 3 × 10^-5 mA cm^-2), indicating that the enzyme combined with the organic catalyst improved energy generation through deep EG electrooxidation. Electrochemical impedance spectroscopy reveals that the addition of the enzyme in the electrode containing MWCNT-COOH-Pyrene-TEMPO increased the charge transfer resistance (R_ct) and the capacitance of the double layer. Long-term electrolysis for 15 h showed that the hybrid electrode presented outstanding current density and stability. The EG oxidation products were identified and quantified by high-performance liquid chromatography (HPLC-UV/RID). The results confirmed complete EG oxidation in the presence of CO₂ in the solution, allowing 10 electrons to be collected from the fuel. Overall, this study illustrates the development of a simple and improved hybrid bi-catalyst electrode for promising applications in small electronic devices.

Keywords: Enzymatic biofuel cell; Ethylene glycol; Hybrid electrode; Organic catalyst; Oxalate oxidase.

MeSH terms

Bioelectric Energy Sources*
Biosensing Techniques*
Carbon Dioxide / chemistry
Electrodes
Ethylene Glycol
Nanotubes, Carbon* / chemistry
Pyrenes / chemistry

Substances

Nanotubes, Carbon
Pyrenes
Carbon Dioxide
pyrene
Ethylene Glycol