ABSTRACT Platinum‐based electrocatalysts are fundamentally constrained by strong oxygen binding, which restricts the oxygen reduction reaction (ORR) kinetics, and by severe CO poisoning, which hinders the methanol oxidation reaction (MOR). To address these limitations, we synthesized PdPtRuIrRhNi high‐entropy alloy (HEA) mesoporous nanotubes that enable cooperative multicomponent electronic interactions and lattice‐strain‐induced modulation of surface electronic structures. The resulting HEA nanotubes exhibited exceptional bifunctional performance, achieving an ultrahigh ORR mass activity of 4.04 A mg Pt −1 (16.8 times that of Pt/C) and a superior MOR mass activity of 3.19 A mg Pt −1 , alongside impressive stability (exemplified by a 92% ORR activity retention after 50,000 cycles). Mechanistic investigations, supported by density functional theory calculations and in situ Fourier‐transform infrared spectroscopy, revealed the electronic origin of this enhancement: multicomponent electronic interactions and lattice strain collectively induce a substantial downshift of the Pt d‐band center. This specific electronic modulation fundamentally reshapes the reaction pathways, shifting the rate‐determining step of the ORR from *O hydrogenation to *OH desorption and suppressing *CO accumulation in the MOR for a poisoning‐tolerant mechanism. Overall, these high‐entropy electrocatalysts driven by lattice strain and electronic redistribution represent a robust design principle for optimizing adsorption energetics and overcoming conventional kinetic limitations.
ABSTRACT Surface reconstruction plays an important role in catalysts for the efficient oxygen evolution reaction (OER). In this work, we report the designed synthesis of the Ce‐ion‐doped Fe‐MOF (CFM) directly grown on nickel foam via a facile solvothermal route. Transmission electron microscopy indicates that the rich CeO 2 nanoparticles are uniformly decorated on the surface of the Fe‐MOF, significantly increasing the density of exposed active sites. The optimized CFM catalyst exhibits exceptional OER activity with an overpotential of 195 mV at 10 mA cm −2 and superior long‐term durability (> 100 h). Through a combination of spectroscopic characterization, electrochemical analysis, and density functional theory, we demonstrate that Ce‐ion doping plays a key role in regulating the local electronic environment of Fe sites, facilitating charge transfer, and promoting the formation of a highly active reconstructed surface. This work highlights rare‐earth‐element doping in MOFs as a promising strategy to fabricate a nonprecious and highly efficient OER electrocatalyst.
ABSTRACT α‐phase aluminum trihydride (α‐AlH 3 ) is a promising high‐capacity hydrogen storage material, but its practical application is limited by slow dehydrogenation kinetics and high reaction temperatures. This study demonstrates, for the first time, effective modulation of the hydrogen release kinetics of AlH 3 by employing a hollow nanostructured vanadium dioxide (VO 2 ) catalyst. The VO 2 hollow nanospheres were synthesized via a hydrothermal method and composited with AlH 3 using mild ball milling. Performance evaluation shows that with an optimal VO 2 addition of 2 wt%, the composite’s onset dehydrogenation temperature is markedly lowered to 44°C, with a peak temperature of only 107°C, while achieving a total hydrogen release capacity of 8.1 wt%. In isothermal dehydrogenation tests, the composite released 7.2 wt% of hydrogen within 60 min at 100°C. The apparent activation energy for dehydrogenation was significantly reduced from 88.5 kJ mol −1 for the milled AlH 3 to 60.4 kJ mol −1 for the composite. Integrated structural characterization and theoretical calculations elucidate the catalytic mechanism: the unique hollow structure of VO 2 provides efficient pathways for hydrogen diffusion, whereas significant electronic interactions between the surface V/O atoms and AlH 3 effectively weaken the Al‐H bonds and supply abundant active sites for aluminum nucleation. These effects collectively enhance the dehydrogenation kinetics. This work provides a novel perspective for designing nanostructured catalysts to optimize the hydrogen storage performance of metal hydrides.
ABSTRACT Achieving rapid and selective separation of anode and cathode materials remains a critical challenge in the recycling of spent lithium‐ion batteries. This study develops a microwave‐enhanced flotation strategy for the efficient recovery of cathode and anode materials. Thermogravimetric analysis identifies 450°C as the optimal temperature for binder decomposition. Notably, microwave treatment enables almost complete removal of organic binders and electrolytes in only 5 min, representing a substantial acceleration as compared with 15–60 min typically required by conventional thermal treatment. Surface analyses, including X‐ray photoelectron spectroscopy and contact angle measurements, confirm that microwave treatment effectively restores the surface hydrophobicity contrast between electrode particles. This enhanced thermal efficiency is attributed to microwave‐induced selective heating mechanism, in which conductive carbon black preferentially absorbs microwave energy, generating localized “hotspots” within the binder layer, thereby accelerating oxidative decomposition of organic components. As a result, flotation performance is significantly improved, increasing the recovery of cathode materials from 61.4% to 93.4% and the concentrate grade from 76.0% to 95.6%. Following a two‐stage flotation process, the purities of the recovered cathode and anode products reach 99.1% and 98.5%, respectively, indicating a strong potential for direct regeneration. Furthermore, comparative economic analysis demonstrates that this process provides a superior energy efficiency and reduced operating costs. Overall, this work elucidates the selective heating mechanism underlying microwave treatment and demonstrates its potential as a sustainable and efficient strategy for spent lithium‐ion battery recycling.
ABSTRACT In this study, aberration‐corrected transmission electron microscopy combined with first‐principles calculations was employed to systematically investigate the Cu‐involved crystal structures and evolution mechanisms of nanoprecipitates in a novel 7075B Al alloy. Firstly, an atomic model of the early‐stage GP‐η p structure together with specific atomic coordinates was determined. In addition, Cu solutes were found to preferentially substitute ZnI and ZnII sites in η 2 precipitates, ZnI sites in η p precipitates, and the central Al site in GP‐η p precipitates. Consequently, Cu solutes participate in the entire nanoprecipitation evolution process from GP‐η p to η 2 precipitates. Further first‐principles calculations reveal that Cu substitution at different Zn sites in η 2 modifies the local chemical bonding characteristics. Specifically, Cu–Mg bonding in Cu‐containing η 2 precipitates exhibits ionic character in addition to metallic bonding features due to charge redistribution, thereby influencing the electronic structure and stability of precipitates. These findings provide important insights into the nanophase transformation in multicomponent alloys and facilitate the development of high‐performance Al alloys.
