Modulation of chalcogen‐functionalized MXenes Ti 2 CT 2 (T = O, S, Se, and Te) as catalysts for hydrogen evolution reaction

• Published in: Journal of the American Ceramic Society 2024-01, Vol.107 (1), p.430-438
• Main Authors: Li, Yiran, Lai, Mengling, Zhao, Juanli, Li, Jiancheng, Li, Wenxian, Liu, Bin
• Format: Article
• Language: English
• ISSN: 0002-7820; 1551-2916
• DOI: 10.1111/jace.19452

Exploration and exploitation of efficient and nonprecious catalysts for hydrogen evolution reaction (HER) is one of the key solutions to energy problems. Two‐dimensional (2D) MXenes have attracted extensive attention as potential catalysts and supports due to their unique structure and customizable properties. In this work, we have systematically investigated the structural stability and electronic properties of chalcogen‐functionalized MXenes Ti 2 CT 2 (T = O, S, Se, and Te) and Pt‐anchored Ti 2 CT 2 MXenes (Pt‐Ti 2 CT 2 ). Density functional theory calculations have discovered that all Ti 2 CT 2 exhibit metallic electronic structures except Ti 2 CO 2 with an indirect bandgap. Additionally, the electronic densities of states at Fermi level for Pt‐Ti 2 CT 2 are greatly enhanced after anchoring Pt atoms. The reduction of chalcogen electronegativity is recognized to mainly contribute to weaker bond strength but greater electronic activity. Moreover, Pt‐Ti 2 CTe 2 is predicted to exhibit near‐zero Gibbs free energy of hydrogen adsorption especially at high hydrogen coverage, indicating its significant potential as HER catalysts. It is also revealed that Ti 2 CT 2 and Pt‐Ti 2 CT 2 MXenes are not only ideal candidates of catalyst materials but also could serve as good catalyst substrates. This work provides insights into the structural and chemical complexity of MXenes for catalyst applications but also demonstrates a new strategy to modulate high‐efficiency and low‐cost catalyst and support materials.