Abstract

The development of a high-performance precious metal-free multifunctional electrocatalyst for overall water splitting is a promising sign for future energy research. Here, a new strategy has been followed for the synthesis of novel-structured binary metal chalcogenide electrocatalysts, such as nickel aluminum sulfide (NiAl2S4) or nickel aluminum selenide (NiAl2Se4) spinels. The new chalcogenides, NiAl2S4 or NiAl2Se4, were confirmed by different physicochemical characterizations. Using a 316 stainless steel (SSL) mesh electrode as a three-dimensional conducting substrate, the electrocatalytic overall water splitting reaction was studied. Here, NiAl2S4 spinel outperformed the other metal chalcogenide in terms of electrocatalytic activity and charge transport in the hydrogen evolution reaction (HER), the oxygen evolution reaction (OER), and overall water splitting in alkaline medium. Moreover, NiAl2S4 spinel provided the finest electrocatalytic efficiencies compared to other benchmark electrocatalysts with minimized overpotentials, such as 47 or 290 mV for HER or OER, respectively, to reach the current density of 20 mA cm–2. In overall water splitting studies, a two-electrode system was formulated to show a very low potential of 1.54 V at a current density of 20 mA cm–2. Further, the prepared NiAl2S4 electrocatalyst-loaded 316 SSL electrode demonstrated excellent durability in HER, OER, and overall water splitting reactions. The obtained Faradaic efficiency was 97%, which is due to the two-dimensional sheet-like morphology of NiAl2S4, enabling a high active surface area for efficient water electrolysis. Furthermore, NiAl2S4 spinel performed well as a counter electrode (CE) material in dye-sensitized solar cells, with an efficiency of 5.02% compared to Pt (5.38%) on the fluorine-doped indium tin oxide electrode.

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