High-entropy alloy (HEA)-based materials are expected to be promising oxygen electrocatalysts due to their exceptional properties. The electronic structure regulation of HEAs plays a pivotal role in enhancing their elctrocatalytic ability. Herein, PtFeCoNiMn nanoparticles (NPs) with subtle lattice distortions are constructed on metal-organic framework-derived nitrogen-doped carbon by an ultra-rapid Joule heating process. Thanks to the modulated electronic structure and the inherent cocktail effect of HEAs, the as-synthesized PtFeCoNiMn/NC exhibits superior bifunctional electrocatalytic performance with a positive half-wave potential of 0.863 V vs. reversible hydrogen electrode (RHE) for oxygen reduction reaction and a low overpotential of 357 mV at 10 mA·cm^–2 for oxygen evolution reaction. The assembled quasi-solid-state zinc-air battery using PtFeCoNiMn/NC as air electrode shows a high peak power density of 192.16 mW·cm^–2, low charge−discharge voltage gap, and excellent durability over 500 cycles at 5 mA·cm^–2. This work demonstrates an effective route for rational design of bifunctional nanostructured HEA electrocatalysts with favorable electronic structures, and opens up a fascinating directions for energy storage and conversion, and beyond.

Two-dimensional metal–organic frameworks (2D MOFs), as a new type of 2D materials, have been widely applied in various applications because of their unique structures and exposed active sites. Herein, we reported two low-cost 2D MOFs constructed by a raw chemical succinic acid (SA), M-SA (M = Ni or Co), which served as efficient photocatalysts for the reduction of CO₂ to CO. Taking advantage of the thinness and open metal sites, the ultrathin Ni-SA nanosheets (ca. 3.6 nm) exhibited excellent CO production of 6.96(7) mmol·g⁻¹·h⁻¹ and CO selectivity of 96.6%. Photoelectrochemical tests and theoretical calculations further confirmed the higher charge transfer efficiency and unsaturated metal sites for promoting photocatalytic performances. More importantly, Ni-SA can also be synthesized in large-scale by an energy-saving method under room temperature, strongly suggesting its promising future and potential for practical applications.

Cu-based materials are seldom reported as oxygen evolution reaction (OER) electrocatalysts due to their inherent electron orbital configuration, which makes them difficult to adsorb oxygen-intermediates during OER. Reasonably engineering the hierarchical architectures and the electronic structures can improve the performance of Cu-based OER catalysts, such as constructing multilevel morphology, inducing the porous materials, improving the Cu valence, building heterostructures, doping heteroatoms, etc. In this work, copper-1,3,5-benzenetricarboxylate (HKUST-1) octahedra in-situ grow on the Cu nanorod (NR)-supported N-doped carbon microplates, meanwhile an active layer of Cu(OH)₂ forms on the surface of the original conductive Cu NRs. The octahedral HKUST-1, serving as a spacer between the microplates, greatly improves the porosity and increases the available active sites, facilitating the mass transport and electron transfer, thus resulting in greatly enhanced OER performance.