Carbon Dots for the Enhancement of Hydrogne Evolution Reacion (HER) Activity

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Carbon dots (CDs) constitute an exciting class of spherical nanometer-sized objects with sizes typically below 10 nm. Due to their strong photoluminescence, ease of synthesis and processing properties from the liquid phase, they are of great interest to for the formation of novel hybrid materials [1,2] with tailored functionalities for electrooptical/(photo-)electrochemical and electrocatalytic applications [2, 3]. In this work we show that green emitting CDs, produced in a hydrothermal bottom-up approach through reaction of m-phenylene diamine (m-PDA) precursor with ethylenediaminetetraacetic acid (EDTA), can be successfully interfaced with 1T-MoSe2, a 2D layered transition metal dichalcogenide, via a non-covalent functionalization approach. The interaction is predominantly of electrostatic nature, driven by the attraction between negatively charged MoSe2 surface and positively charged ammonium groups of the CDs. While 1T phase of MoSe2 is known as catalytic active phase enabling HER reactions, we reveal that non-covalently attached CDs can efficiently boost its activity, as evidenced by a significantly reduced overpotential and increase in current densities. Weak electrostatic interactions, however, lead to leaching effects upon electrochemical cycling test over prolonged times, underlining the need for developing stabilization strategies in future works. Overall, this work underlines the potential of 1T-MoSe2-CD hybrids as efficient and tunable HER catalysts. References: [1] L. Vallan, R. Canton-Vitoria, H.B. Gobeze, Y. Jan, R. Arenal, A.M. Benito, W.K. Maser, F. D’Souza, N. Tagmatarchis, J. Amer. Chem. Soc. 2018, 140, 13488. [2] A. Kagkoura, R. Canton-Vitoria, L. Vallan, J. Hernández-Ferrer, A.M. Benito, W.K. Maser, R. Arenal, N. Tagmatarchis, Chem. Eur.J. 2020, 26, 1. [3] A. Ansón-Casaos, J. Hernández-Ferrer, L. Vallan, H. Xie, M. Lira-Cantú, A.M. Benito, W.K. Maser, Int. J. Hydrogen Ener. 2021, 46, 12180.

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