Superhydrophilic and Underwater Superaerophobic Dual-Function Peony-Shaped Selenide Micro-nano Array Self-Supported Electrodes for High-Efficiency Overall Water Splitting Driven by Renewable Energy.

With the intensification of global environmental pollution and resource scarcity, hydrogen has garnered significant attention as an ideal alternative to fossil fuels due to its high energy density and nonpolluting nature. Consequently, the urgent development of electrocatalytic water-splitting electrodes for hydrogen production is imperative. In this study, a superwetting selenide catalytic electrode with a peony-flower-shaped micronano array (MoS 2 /Co 0.8 Fe 0.2 Se 2 /Ni x Se y /nickel foam (NF)) was synthesized on NF via a two-step hydrothermal method. The optimal catalytic activity of cobalt-iron selenide was achieved by adjusting the Co/Fe ratio. The intrinsic catalytic activity of the electrodes was enhanced by incorporating transition metal selenides, which then served as a precursor for the subsequent loading of MoS 2 nanoflowers on the surface to fully expose the active sites. Furthermore, the superwetting properties of the electrode accelerated electrolyte penetration and electron/mass transfer, while also facilitating bubble detachment from the electrode surface, thereby preventing "bubble shielding effect". This resulted in superior oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) performance, as well as overall water splitting capabilities. In a 1.0 M KOH solution, the electrode required only 166 and 195 mV overpotential to achieve a current density of 10 mA cm -2 for OER and HER, respectively. When functioning as a bifunctional catalytic electrode, only 1.60 V of voltage was necessary to drive the electrolyzer to reach a current density of 10 mA cm -2 . Moreover, laboratory simulations of wind and solar energy-driven water splitting validated the feasibility of establishing a sustainable energy-to-hydrogen production chain. This work provides new insights into the preparation of low-overpotential, high-catalytic-activity superhydrophilic and underwater superaerophobic catalytic electrodes by rationally adjusting elemental ratios and exploring changes in electrode surface wettability.