Biomimetic nucleotide-graphene hybrids for electrocatalytic oxygen conversion: Quantifying biomolecule mass loading
Metal-free electrocatalysts for the electrochemical conversion of gases constitute an important asset for a sustainable energy transition. Nucleotides act as redox mediators in the electron transport chain to reduce oxygen in cellular respiration. The biomimicry of such an efficient natural mechanism could be utilized to address the challenges associated with electrochemical gas conversion technologies, such as sluggish kinetics and high overpotentials. Multiple descriptors are generally reported to benchmark the activity of electrocatalysts where the turnover frequency (TOF) is claimed to be the most accurate criterion. Here, a library of graphene nanosheets-nucleotide hybrid materials was prepared, and the electrocatalytic performance towards ORR/OER reactions of a graphene-flavin mononucleotide hybrid was evaluated by rotating disc electrode experiments and TOF estimation. The determination of catalyst loading and dispersion is especially relevant when assessing the intrinsic activity of a catalyst and, therefore, the amount of nucleotide electrocatalyst loaded into the graphene support was thoroughly quantified by a combination of characterization techniques. Density functional theory calculations supported the observed experimental trends, both on the adsorption rate of a given nucleotide on graphene and the catalytic activity of a specific hybrid material. This work constitutes an avenue to predict nature-mimicking electrocatalysts for efficient energy storage.
| Main Authors: | , , , , , , |
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| Other Authors: | |
| Format: | artículo biblioteca |
| Language: | English |
| Published: |
Elsevier
2024-04-01
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| Subjects: | Nucleotides, Bioinspired graphene based electrocatalyts, Loading, ORR/OER reactions, Metal-free electrocatalyts, Gas conversion technologies, Ensure access to affordable, reliable, sustainable and modern energy for all, Build resilient infrastructure, promote inclusive and sustainable industrialization and foster innovation, |
| Online Access: | http://hdl.handle.net/10261/355431 http://dx.doi.org/10.13039/501100011033 http://dx.doi.org/10.13039/501100004837 https://api.elsevier.com/content/abstract/scopus_id/85185330302 |
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| Summary: | Metal-free electrocatalysts for the electrochemical conversion of gases constitute an important asset for a sustainable energy transition. Nucleotides act as redox mediators in the electron transport chain to reduce oxygen in cellular respiration. The biomimicry of such an efficient natural mechanism could be utilized to address the challenges associated with electrochemical gas conversion technologies, such as sluggish kinetics and high overpotentials. Multiple descriptors are generally reported to benchmark the activity of electrocatalysts where the turnover frequency (TOF) is claimed to be the most accurate criterion. Here, a library of graphene nanosheets-nucleotide hybrid materials was prepared, and the electrocatalytic performance towards ORR/OER reactions of a graphene-flavin mononucleotide hybrid was evaluated by rotating disc electrode experiments and TOF estimation. The determination of catalyst loading and dispersion is especially relevant when assessing the intrinsic activity of a catalyst and, therefore, the amount of nucleotide electrocatalyst loaded into the graphene support was thoroughly quantified by a combination of characterization techniques. Density functional theory calculations supported the observed experimental trends, both on the adsorption rate of a given nucleotide on graphene and the catalytic activity of a specific hybrid material. This work constitutes an avenue to predict nature-mimicking electrocatalysts for efficient energy storage. |
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