In Situ Reconstruction of High-Entropy Heterostructure Catalysts for Stable Oxygen Evolution Electrocatalysis under Industrial Conditions.

Despite of urgent needs for highly stable and efficient electrochemical water-splitting devices, it remains extremely challenging to acquire highly stable oxygen evolution reaction (OER) electrocatalysts under harsh industrial conditions. Here, a successful in situ synthesis of FeCoNiMnCr high-entropy alloy (HEA) and high-entropy oxide (HEO) heterocatalysts via a Cr-induced spontaneous reconstruction strategy is reported, and it is demonstrated that they deliver excellent ultrastable OER electrocatalytic performance with a low overpotential of 320 mV at 500 mA cm-2 and a negligible activity loss after maintaining at 100 mA cm-2 for 240 h. Remarkably, the heterocatalyst holds outstanding long-term stability under harsh industrial condition of 6 m KOH and 85 °C at a current density of as high as 500 mA cm-2 over 500 h. Density functional theory calculations reveal that the formation of the HEA-HEO heterostructure can provide electroactive sites possessing robust valence states to guarantee long-term stable OER process, leading to the enhancement of electroactivity. The findings of such highly stable OER heterocatalysts under industrial conditions offer a new perspective for designing and constructing efficient high-entropy electrocatalysts for practical industrial water splitting.

Fabricating carbon quantum dots of graphitic carbon nitride vis ultrasonic exfoliation for highly efficient H2O2 production.

A promising and sustainable approach for producing hydrogen peroxide is the two-electron oxygen reduction reaction (2e- ORR), which uses very stable graphitic carbon nitride (g-C3N4). However, the catalytic performance of pristine g-C3N4 is still far from satisfactory. Here, we demonstrate for the first time the controlled fabrication of carbon quantum dots (CQDs)-modified graphitic carbon nitride carbon (g-C3N4/CQDs-X) by ultrasonic stripping for efficient 2e- ORR electrocatalysis. HRTEM, UV-vis, EPR and EIS analyses are in good consistent which prove the in-situ generation of CQDs. The effect of sonication time on the physical properties and ORR activity of g-C3N4 is discussed for the first time. The g-C3N4/CQDs-12 catalyst shows a selectivity of up to 95% at a potential of 0.35 V vs. RHE, which is much higher than that of the original g-C3N4 catalyst (88%). Additionally, the H2O2 yield is up to 1466.6 mmol g-1 in 12 h, which is twice as high as the original g-C3N4 catalyst. It is discovered that the addition of CQDs through ultrasonic improves the g-C3N4 catalyst's electrical conductivity and electron transfer capability in addition to its high specific surface area and distinctive porous structure, speeding up the reaction rate. This research offers a green method for enhancing g-C3N4 activity.