Nitrogenated arbon electrodes as cathode materials for electrocatalytic transformations of organic compounds Christian Schröder 1 , Hugo Nolan 1,2 , MarcBrunet-Cabré 1 , Filippo Pota 1 , Niall McEvoy 1,2 , Kim McKelvey 1,3 , Tatiana S. Perova 4 , Paula E. Colavita 1,2 1 School of Chemistry, Trinity College Dublin, Dublin 2, Ireland, 2 CRANN and AMBER Research Centres, Trinity College Dublin, Dublin 2, Ireland, 3 MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Chemical and Physical Sciences, Victoria University of Wellington, Wellington, 6012, New Zealand, 4 School of Engineering, Trinity College Dublin, College Green, Dublin 2, Ireland Electrocatalytic transformations of biomass-derived molecules offer a way to convert renewable energy into fuels and value-added chemicals, thus lowering the carbon footprint of economic activities. The electrocatalytic hydrogenation (ECH) of oxygenated compounds, a cathodic process, is one of the conversions of interest. In this reaction adsorbed hydrogen is generated from the aqueous electrolyte and transferred to the organic unsaturated groups. The step of hydrogen activation is the so called Volmer step in the hydrogen evolution reaction (HER); therefore, catalyst materials which show HER activity are of interest for the ECH. Platinum and other noble metals show good activity in the ECH, but their scarcity and their cost make them less attractive for a scale up. Hence, to make this technology viable for large scale applications new electrocatalyst materials must be developed. Electrocatalysts based on carbon materials offer a variety of benefits: carbon is widely available, environmentally benign and can be chemically tailored. Herein, we report on the design of heteroatom-modified carbon-based electrodes towards hydrogen activation for the HER and the ECH of organics. Carbon thin-films with smooth topography and controlled composition were first synthesized and characterized. Composition was controlled via combinations of sputter deposition, reactive annealing and chemical vapour deposition. Structure and morphology were analysed with spectroscopic techniques and the electrochemical activity towards cathodic reactions was evaluated. Insights on the reaction mechanism were obtained by correlating electrochemical performance using benzaldehyde as a diagnostic substrate, reaction conditions and chemical composition. Our results suggest possible strategies for developing novel ECH electrocatalysts based on engineered functional carbons. References 1. Behan, J. A.; Stamatin, S. N.; Hoque, M. K.; Ciapetti, G.; Zen, F.; Esteban-Tejeda, L.; Colavita, P. E., Combined Optoelectronic and Electrochemical Study of Nitrogenated Carbon Electrodes. The Journal of Physical Chemistry C 2017, 121 (12), 6596-6604. 2. Nolan, H.; Schröder, C.; Brunet-Cabré, M.; Pota, F.; McEvoy, N.; McKelvey, K.; Perova, T. S.; Colavita, P. E., MoS2/carbon heterostructured catalysts for the hydrogen evolution reaction: N-doping modulation of substrate effects in acid and alkaline electrolytes. Carbon 2023 , 202, 70-80.
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