Optimized 2D Nanostructures for Catalysis of Hydrogen Evolution Reactions

Hydrogen is one of the most promising energy carriers with energetic transport and storage advantages over fossil fuels. However, commercial H₂ production relies on Hydrocarbon reforming methods, emitting greenhouse gasses (GHG) such as CO2 [1]. H₂ can be produced without harmful emissions by water splitting in the electrochemical Hydrogen Evolution Reaction (HER). However, this mechanism is limited by the lack of cheap, abundant, and efficient catalysts. The search for new noble-metal-free catalysts has increasingly attracted researchers' interest in the last years, and several prospective materials have been proposed. The Transition Metal Dichalcogenides (TMD) emerged as prospect materials to catalyze HER. These materials exhibit interesting electronic and structural properties. Their catalytic activity can be optimized by increasing active site counting and tailoring electronic properties. Common strategies to optimize TMD catalytic activity comprehend phase engineering and doping [2]. TiSe₂ has emerged as a material with remarkable and extensively investigated properties. The stability of its 1T phase and sensibility of electronic properties to doping can be explored in catalysis. In this work, the catalytic activity of TiSe₂ in HERs is investigated via DFT calculations using the Quantum Espresso package. We employed the Computational Hydrogen Electrode model to conduct a thermodynamic study, evaluating the free energy variation of Hydrogen adsorption, which was reported as a good activity descriptor [3]. We found that the introduction of Pt dopants on the basal plane of the 1T-TiSe₂ enhances the activity of chalcogen sites.<br/><br/>References<br/>[1] P. J. Megía et al, Energy & Fuels <i>35</i> (20), 16403-16415 (2021);<br/>[2] Voiry D. et al., Adv. Mater., 28: 6197-6206 (2016).<br/>[3] J. K. Nørskov et al, J. Electrochem. Soc. 152 J23 (2005);