Enhanced hydrogen evolution reaction activity of hydrogen-annealed vertical MoS₂ nanosheets

Molybdenum disulfide (MoS₂) is a promising electrocatalyst for hydrogen evolution reaction (HER), but only edges and S-vacancies are catalytic active sites for the HER. Therefore, it is crucial to increase edge sites and S-vacancies for enhancing the HER activity of MoS₂. Here, we report an enhanced HER activity of MoS₂ by combing vertical nanosheets and H₂ annealing. Compared to horizontal MoS₂ nanosheets, pristine vertical MoS₂ nanosheets showed better HER activity due to a larger amount of edges. H₂ annealing further enhanced the HER activity of vertical MoS₂ nanosheets remarkably. Scanning electron microscopy (SEM), X-ray photoelectron spectra (XPS) and electrochemical impedance spectroscopy (EIS) were used to elucidate the enhanced HER activity by H₂ annealing. SEM images showed that H₂ annealing roughened the MoS₂ edges, leading to more edge sites. XPS data revealed the smaller S : Mo ratio after H₂ annealing, meaning more S-vacancies. Meanwhile, EIS measurements showed that charge transfer was accelerated by H₂ annealing. These findings elaborated the H₂ annealing induced enhancement of the HER activity, which were further confirmed by the subsequent re-sulfurization experiment.