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Communication Dans Un Congrès Année : 2017

Development of novel cathode materials for the bioelectrocatalysis of oxygen reduction reaction by laccase from Trametes versicolor

Résumé

Biocatalysts such as enzymes or bacteria constitute an attractive alternative to transition metal catalysts. They have several advantages as they often possess a better selectivity and higher catalytic performances and they can be used in different types of electrochemical devices such as fuel cells or batteries [1].We are focusing here on the cathode of a fuel cell working with enzymes acting as biocatalysts. This type of device is called a biofuel cell. In the cathodic compartment, the oxygen reduction reaction (ORR) occurs. Most of the enzymes used to catalyse this reaction belong to the multi-copper oxidase family. Among multi-copper enzymes, laccase, an extra-cellular blue copper enzyme, is the most widely used biocatalyst. This enzyme contains four copper atoms shared in two different areas of the protein. The T1 site is responsible for the oxidation of phenolic substrates while T2/T3 is responsible for the ORR [2, 3, 4]. The particularity of the cathode developed in this work is first that the enzymes are directly grafted on the electrode material and no redox mediator is therefore required to shuttle the electrons between the support and the enzyme. We have used several strategies to immobilize the enzyme on the electrode surface by playing on the grafting procedure, on the structure of the laccase or on the electrode material. The goal of all these strategies was to optimize the oxygen reduction reaction. In the first one, we have used amorphous carbon nitride film (a-CNx) thin film deposited on rough graphite as an electrode. a-CNx thin films contain in their pristine form surface amine groups [5] suitable for enzyme grafting and also by an electrochemical treatment carboxylic functional groups. Moreover, they can be easily deposited on various substrates by cathodic reactive magnetron sputtering. The second strategy was to increase considerably the surface area of the graphite by depositing carbon nanowalls (CNW) by plasma-enhanced chemical vapour in a CO/H2 microwave discharge. The carbon nanowalls were then functionalized by atmospheric plasma to ensure enzyme grafting. It is well to know that amorphous carbon nitride and carbon nanowalls have not been studied yet as biofuel cell electrode materials in the literature. The resulting electrodes a-CNx@graphite and CNW@gtraphite has been characterized by electrochemical measurements (cyclic voltammetry and chronoamperometry), UV-visible, XPS techniques to characterize the enzyme catalytic activity and to quantify it amount. For a better understanding of the electron transfer between the electrode and dioxygen was further developed by using the electrochemical impedance spectroscopy (EIS) technique. 1. M. Rasmussen, S. Abdellaoui, S.D. Minteer, Biosensors ans bioelectronics (2016), 76, 91-102. 2. E.I. Solomon, Inorg. Chem (2016), 55, 6364-6375. 3. A. Le Goff, M. Holzinger, S. Cosnier, Cellular and Molecular Life Sciences (2015), 72, 941-952. 4. S. Cosnier, A. Le Goff, M. Holzinger, Electrochemistry Communications (2014), 38, 19 5. S. Jribi, S.I. Cordoba de Torresi, T. Augusto, H. Cachet, C. Debiemme-Chouvy, C. Deslouis, A. Pailleret, Electrochimica Acta (2014), 136, 473-482.

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Chimie
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Dates et versions

hal-03978145 , version 1 (08-02-2023)

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  • HAL Id : hal-03978145 , version 1

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Achraf Blout, Alain Pailleret, Claude Jolivalt. Development of novel cathode materials for the bioelectrocatalysis of oxygen reduction reaction by laccase from Trametes versicolor. 68th ISE annual Meeting, ISE, Aug 2017, Providence, United States. ⟨hal-03978145⟩
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