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CoS2 is considered to be a promising electrocatalyst for hydrogen evolution reaction (HER). However, its further widespread applications are hampered by the unsatisfactory activity due to relatively high chemisorption energy for hydrogen atom. Herein, theoretical predictions of first-principles calculations reveal that the introduction of a Cl-terminated MXenes-Ti3CNCl2 can significantly reduce the HER potential of CoS2-based materials and the Ti3CNCl2@CoS2 core–shell nanostructure has Gibbs free energy of hydrogen adsorption (|ΔGH|) close to zero, much lower than that of the pristine CoS2 and Ti3CNCl2. Inspired by the theoretical predictions, we have successfully fabricated a unique Ti3CNCl2@CoS2 core–shell nanostructure by ingeniously coupling CoS2 with a Cl-terminated MXenes-Ti3CNCl2. Interface-charge transfer between CoS2 and Ti3CNCl2 results in a higher degree of electronic localization and a formation of chemical bonding. Thus, the Ti3CNCl2@CoS2 core–shell nanostructure achieves a significant enhancement in HER activity compared to pristine CoS2 and Ti3CNCl2. Theoretical calculations further confirm that the partial density of states of CoS2 after hybridization becomes more non-localized, and easier to interact with hydrogen ions, thus boosting HER performance. In this work, the success of oriented experimental fabrication of high-efficiency Ti3CNCl2@CoS2 electrocatalysts guided by theoretical predictions provides a powerful lead for the further strategic design and fabrication of efficient HER electrocatalysts.
This work was supported by the National Natural Science Foundation of China (No. 62004143), the Central Government Guided Local Science and Technology Development Special Fund Project (No. 2020ZYYD033), the Natural Science Foundation of Hubei Province (No. 2021CFB133), the Opening Fund of Key Laboratory of Rare Mineral, Ministry of Natural Resources (No. KLRM-KF 202005), the Opening Fund of Key Laboratory for Green Chemical Process of Ministry of Education of Wuhan Institute of Technology (No. GCP202101), and the Innovation Project of Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education (No. LCX2021003). This work was dedicated to celebrating the 50th anniversary of Wuhan Institute of Technology.