Nickel–iron based materials are well-known catalysts for the oxygen evolution reaction (OER) and have been widely investigated. However, the synergy between these two components is still controversial. Herein, we report a facile immersion method for the synthesis of binder-free nickel–iron hydroxide loaded on Ni foam (NiFe-OH/NF) with superior hydrophilic property and high OER catalytic activity. The strong hydrophilic property of the binder-free NiFe-OH/NF electrode significantly enhances an effective contact between electrocatalyst and aqueous electrolyte and favors the bubble detachment from the electrode, facilitating the electron transfer and improving the OER activity. The hydrophilic NiFe-OH/NF can achieve a geometrical current density of 100 mA cm–1 at an extremely low overpotential (219 mV), along with a Tafel slope of 56 mV dec–1 and superior long-term stability at high current density in alkaline media, strongly indicating that the hydrophilicity plays an important role in improving the OER performance in the NiFe-OH/NF.

Despite their high theoretical energy density and low cost, lithium–sulfur batteries (LSBs) suffer from poor cycle life and low energy efficiency owing to the polysulfides shuttle and the electronic insulating nature of sulfur. Conductivity and polarity are two critical parameters for the search of optimal sulfur host materials. However, their role in immobilizing polysulfides and enhancing redox kinetics for long‐life LSBs are not fully understood. This work has conducted an evaluation on the role of polarity over conductivity by using a polar but nonconductive platelet ordered mesoporous silica (pOMS) and its replica platelet ordered mesoporous carbon (pOMC), which is conductive but nonpolar. It is found that the polar pOMS/S cathode with a sulfur mass fraction of 80 wt% demonstrates outstanding long‐term cycle stability for 2000 cycles even at a high current density of 2C. Furthermore, the pOMS/S cathode with a high sulfur loading of 6.5 mg cm−2 illustrates high areal and volumetric capacities with high capacity retention. Complementary physical and electrochemical probes clearly show that surface polarity and structure are more dominant factors for sulfur utilization efficiency and long‐life, while the conductivity can be compensated by the conductive agent involved as a required electrode material during electrode preparation. The present findings shed new light on the design principles of sulfur hosts towards long‐life and highly efficient LSBs.

Lithium-sulfur batteries have theoretical specific energy higher than state-of-the-art lithium-ion batteries. However, from a practical perspective, these batteries exhibit poor cycle life and low energy content owing to the polysulfides shuttling during cycling. To tackle these issues, researchers proposed the use of redox-inactive protective layers between the sulfur-containing cathode and lithium metal anode. However, these interlayers provide additional weight to the cell, thus, decreasing the practical specific energy. Here, we report the development and testing of redox-active interlayers consisting of sulfur-impregnated polar ordered mesoporous silica. Differently from redox-inactive interlayers, these redox-active interlayers enable the electrochemical reactivation of the soluble polysulfides, protect the lithium metal electrode from detrimental reactions via silica-polysulfide polar-polar interactions and increase the cell capacity. Indeed, when tested in a non-aqueous Li-S coin cell configuration, the use of the interlayer enables an initial discharge capacity of about 8.5 mAh cm−2 (for a total sulfur mass loading of 10 mg cm−2) and a discharge capacity retention of about 64 % after 700 cycles at 335 mA g−1 and 25 °C.

The amount of Fe and NH3 treatment significantly affect the structural and catalytic properties of resulting ZIF-derived Fe–N–C catalysts.