Rational hybridization of two-dimensional (2D) nanomaterials with extrinsic species has shown great promise for boosting electrocatalytic oxygen evolution reaction (OER). To date, the rational design and engineering of heterojunctions based...

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The introduction of high-entropy and high specific surface area into Prussian blue analogues (PBAs) has yet to create interest in the field of electrocatalytic small-molecule oxidation reactions. Herein, we synthesize a novel class of high-entropy (HE) PBAs with a high specific surface area via a simple NH 3 •H 2 Oetching strategy and systematically investigate the electrocatalytic performance of HE-PBA toward electrocatalytic water, ethanol, and urea oxidation reactions. Importantly, the NH 3 •H 2 O-etched HE-PBA (denoted as HE-PBA-e) demonstrated enhanced electrocatalytic performance toward small-molecule oxidation compared to the pristine HE-PBA, reaching 10 mA cm −2 with potentials of 1.56, 1.41, and 1.37 V for the oxygen evolution reaction (OER), ethanol oxidation reaction (EOR), and urea oxidation reaction (UOR), respectively. Deep characterizations suggest that the NH 3 • H 2 O etching treatment not only creates rich nanopores to enlarge the surface area and boosts the mass transport and electron transfer but also facilitates the formation of high-valence metal oxides to improve the intrinsic activity. This demonstration of how systematically increasing the high oxidation state of metals will serve as a governing principle for the rational design of more advanced HE-PBAs toward the electrooxidation of small molecules.

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Electrocatalytic water splitting holds great research prospects in the production of green hydrogen energy, and electrocatalysts are the prerequisite. Widely employed as efficient electrocatalysts, hollow nanostructures have attracted a lot...