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Letona-Elizburu, A.; Enterría, M.; Aziz, A.; Villar-Rodil, S.; Paredes, J.I.; Carrasco, J.; Ortiz-Vitoriano, N.
Sustainable Materials and Technologies, April 2024, 2024-04-00, Letnik: 39Journal Article
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. Sustainable metal-free nucleotide/graphene hybrids are prepared as promising electrocatalysts for gas conversion reactions. Non-covalent π-π interactions are facilitated through liquid adsorption and the amount of adsorbed nucleotide in graphene is assessed using various techniques. The trend observed experimentally aligns consistently with the adsorption energies computed through DFT calculations. The riboflavin-containing hybrid shows a better ability to catalyze OER than graphene. Display omitted
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JCR | SNIP | JCR | SNIP | JCR | SNIP | JCR | SNIP |
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in: SICRIS
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