(308g) Ration Design of Efficient TaS2 Catalyst Towards Promising Electrochemical Hydrogen Production

Electrochemical hydrogen evolution reaction (HER) has drawn significant attention as a promising process to produce hydrogen for clean and renewable energy. Although platinum has been considered the most active catalyst towards HER, its application at a large scale is limited by its high cost and earth scarcity. Various transition metal dichalcogenides (TMDs) catalysts have been developed for HER to substitute Pt, such as MoS₂- and TaS₂-based catalysts [1, 2]. TaS₂, and MoS₂, have two main phases: the 2H phase with trigonal prism and the 1T phase with octahedral coordination. Unlike MoS₂, which has semiconductive properties for the 2H phase, TaS₂ is not only conductive in the 1T phase, but also metallic when in 2H phase [3]. Considering the potential of TaS₂ based HER catalyst, here we utilize computational methods to study and engineer the nanostructures of TaS₂ and predict the theoretical activities for hydrogen production to discover new catalysts. Through density functional theory (DFT) calculations, we unravel the influence of (Co-, Fe-, and Ru-) intercalations on the HER activity and the stability of TaS₂, including both edges and basal planes as active sites. We note that Fe-intercalation can largely reduce the absolute value of DG_H (Gibbs free energy of hydrogen adsorption), thereby highly boosting the HER activity of TaS₂ catalyst. Thus, we propose design principles for more efficient catalysts, which could largely speed up the development process of HER improvement.

[1] Ge. Ye, et al. Nano Lett. 2016, 16, 1097.

[2] L. Najafi, et al. ACS Catal. 2020, 10, 3313.

[3] C. Tsai, et al. Surf. Sci. 2015, 640, 133.