Among 2D materials, transition-metal dichalcogenides (TMDCs) of group 5 metals recently have attracted substantial interest due to their superior electrocatalytic activity toward hydrogen evolution reaction (HER). However, a straightforward and efficient synthesis of the TMDCs which can be easily scaled up is missing. Herein, we report an innovative, simple, and scalable method for tantalum disulfide (TaS 2 ) synthesis, involving CS 2 as a sulfurizing agent and Ta 2 O 5 as a metal precursor. The structure of the created TaS 2 flakes was analyzed by Raman, XRD, XPS, SEM, and HRTEM techniques. It was demonstrated that a tuning between 1T (metallic) and 3R (semiconductor) TaS 2 phases can be accomplished by varying the reaction conditions. The created materials were tested for HER, and the electrocatalytic activity of both phases was significantly enhanced by electrochemical self-activation, up to that comparable with the Pt one. The final values of the Tafel slopes of activated TaS 2 were found to be 35 and 43 mV/dec for 3R-TaS 2 and 1T-TaS 2 , respectively, with the corresponding overpotentials of 63 and 109 mV required to reach a current density of 10 mA/cm 2 . We also investigated the mechanism of flake activation, which can be attributed to the changes in the flake morphology and surface chemistry. Our work provides a scalable and simple synthesis method to produce transition-metal sulfides which could replace the platinum catalyst in water splitting technology.
Environmental problems related to the economy based on fossil fuels are of paramount importance. However, transition to renewable energy sources is restrained by the availability of storage technologies. Electrochemistry is a widely recognized prominent tool to achieve this goal by converting renewable energy into the form of chemical bonds accessible further as fuels, such as hydrogen produced by water splitting. Crucial losses in such process are caused by the high overpotentials, required for water splitting as a hydrogen source. To achieve required efficiency of water splitting appropriate catalysts have to be found with the suitable combination of activity, stability and cost. Nano-structured, two-dimensional materials (2D) are attractive candidates due possessing many of the desired properties and highly tunable characteristics. Employing light allows additional degree of freedom to boost conventional photo-electrocatalysis, in particular plasmonmediated electrocatalysis. Enhancement of the catalytic activity can be increased even further if the catalytic system absorbs wide range of light spectrum. In this study, we combine plasmon-active Au grating with 2D flakes of TiB2, to perform plasmon-mediated water splitting half-reactionhydrogen evolution.
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