Large Manipulation of Ferrimagnetic Curie Temperature by A-Site Chemical Substitution in ACuFeReO (A = Na, Ca, and La) Half Metals.

CaCuFeReO and LaCuFeReO quadruple perovskite oxides are well known for their high ferrimagnetic Curie temperatures and half-metallic electronic structures. By A-site chemical substitution with lower valence state Na, an isostructural compound NaCuFeReO with both A- and B-site ordered quadruple perovskite structures in -3 symmetry was prepared using high-pressure and high-temperature techniques. The X-ray absorption study demonstrates the valence states to be Cu, Fe, and Re.

Highly Efficient Photocatalytic HO Production under Ambient Conditions via Defective InS Nanosheets.

Oxygen and water generating hydrogen peroxide (HO) by optical drive is an extremely promising pathway, and the large amount of oxygen in air and natural sunlight illumination are excellent catalytic conditions. However, the separation efficiency of photogenerated electron-hole pairs greatly limits the photocatalytic efficiency, especially in the absence of sacrificial agents. Here, we report an InS nanosheet with an S vacancy (S-InS).

Optimized Adsorption of Had and OHad over Amorphous SrRuPtOxHy Nanobelts towards Efficient Alkaline Fuel Cell Catalysis.

PtRu-based catalysts toward hydrogen oxidation reaction (HOR) suffer from low efficiency, CO poisoning and over-oxidation at high potentials. In this work, an amorphization strategy is adopted for preparation of amorphous SrRuPtOxHy nanobelts (a-SrRuPtOxHy NBs). The a-SrRuPtOxHy NBs have optimized adsorption of intermediates (H and OH), increased number of active sites, highly weakened CO poisoning and enhanced anti-oxidation ability owing to the special amorphous structure.

Selective light-driven methane oxidation to ethanol.

Methane (CH) photocatalytic upgrading to value-added chemicals, especially C products, is significant yet challenging due to sluggish energy/mass transfer and insufficient chemical driven-force in single photochemical process. Herein, we realize solar-driven CH oxidation to ethanol (CHOH) on crystalline carbon nitride (CCN) modified with CuS and Cu single atoms (CuS/Cu-CCN). The integration of photothermal effect and photocatalysis overcomes CH-to-CHOH conversion bottlenecks, with CuS as a hotspot to convert solar-energy to heat.

Hollow Pt-Encrusted RuCu Nanocages Optimizing OH Adsorption for Efficient Hydrogen Oxidation Electrocatalysis.

As one of the best candidates for hydrogen oxidation reaction (HOR), ruthenium (Ru) has attracted significant attention for anion exchange membrane fuel cells (AEMFCs), although it suffers from sluggish kinetics under alkaline conditions due to its strong hydroxide affinity. In this work, we develop ternary hollow nanocages with Pt epitaxy on RuCu (Pt-RuCu NCs) as efficient HOR catalysts for application in AEMFCs. Experimental characterizations and theoretical calculations confirm that the synergy in optimized Pt-RuCu NCs significantly modifies the electronic structure and coordination environment of Ru, thereby balancing the binding strengths of H* and OH* species, which leads to a markedly enhanced HOR performance.

A Complex Oxide Containing Inherent Peroxide Ions for Catalyzing Oxygen Evolution Reactions in Acid.

Proton exchange membrane water electrolyzers powered by sustainable energy represent a cutting-edge technology for renewable hydrogen generation, while slow anodic oxygen evolution reaction (OER) kinetics still remains a formidable obstacle that necessitates basic comprehension for facilitating electrocatalysts' design. Here, we report a low-iridium complex oxide LaSrIrO with a unique hexagonal structure consisting of isolated Ir(V)O octahedra and true peroxide O groups as a highly active and stable OER electrocatalyst under acidic conditions. Remarkably, LaSrIrO, containing 59 wt % less iridium relative to the benchmark IrO, shows about an order of magnitude higher mass activity, 6-folds higher intrinsic activity than the latter, and also surpasses the state-of-the-art Ir-based oxides ever reported.

Unconventional Hexagonal Close-Packed High-Entropy Alloy Surfaces Synergistically Accelerate Alkaline Hydrogen Evolution.

Accelerating the alkaline hydrogen evolution reaction (HER), which involves the slow cleavage of HO-H bonds and the adsorption/desorption of hydrogen (H*) and hydroxyl (OH*) intermediates, requires developing catalysts with optimal binding strengths for these intermediates. Here, the unconventional hexagonal close-packed (HCP) high-entropy alloy (HEA) atomic layers are prepared composed of five platinum-group metals to enhance the alkaline HER synergistically. The breakthrough is made by layer-by-layer heteroepitaxial deposition of subnanometer RuRhPdPtIr HEA layers on the HCP Ru seeds, despite the thermodynamic stability of Rh, Pd, Pt, and Ir in a face-centered cubic (FCC) structure except for Ru.

Tailoring the d‑Band Center of High-Entropy Perovskite Oxide Nanotubes for Enhanced Nitrate Electroreduction.

High-entropy perovskite oxides exhibit promising application prospects in the field of electrocatalysis, owing to their flexible elemental composition, plentiful active sites, and superior structural stability. Herein, high-entropy perovskite oxide nanotubes are prepared with La, Nd, Pr, Er, Eu at A-site by electrospinning as efficient electrocatalysts for nitrate reduction reaction (NORR). Electrochemical tests demonstrate that LaNdPrErEuCuO nanotubes (LNPEEC NTs) display outstanding NORR performance, achieving a NH Faraday efficiency (FE) of 100% at -0.

Selective and durable HO electrosynthesis catalyst in acid by selenization induced straining and phasing.

Developing efficient electrocatalysts for acidic electrosynthesis of hydrogen peroxide (HO) holds considerable significance, while the selectivity and stability of most materials are compromised under acidic conditions. Herein, we demonstrate that constructing amorphous platinum-selenium (Pt-Se) shells on crystalline Pt cores can manipulate the oxygen reduction reaction (ORR) pathway to efficiently catalyze the electrosynthesis of HO in acids. The Se‒Pt nanoparticles, with optimized shell thickness, exhibit over 95% selectivity for HO production, while suppressing its decomposition.

Solvation Effect-Determined Mechanisms of Cation Exchange Reactions for Efficient Multicomponent Nanocatalysts.

Cation exchange (CE) reaction is a classical synthesis method for creating complex structures. A lock of study on intrinsic mechanism limits its understanding and practical application. Using X-ray absorption spectroscopy, we observed that the evolution from Ru-Cl to Ru-O/OH occurs during the CE between KRuCl and CoSn(OH) in aqueous solution, while CE between KPtCl and CoSn(OH) is inhibited due to the failure of structural evolution from Pt-Cl to Pt-O/OH.

Atom-glue stabilized Pt-based intermetallic nanoparticles.

Pt-based nanoparticles (NPs) have been widely used in catalysis. However, this suffers from aggregation and/or sintering at working conditions. We demonstrate a robust strategy for stabilizing PtCo NPs under high temperature with strong interaction between M-N-C and PtCo NPs with Pt-M-N coordination, namely, "atom glue.

Highly Efficient Manganese Bromides with Reversible Luminescence Switching through Amorphous-Crystalline Transition.

While luminescent stimuli-responsive materials (LSRMs) have become one of the most sought-after materials owing to their potential in optoelectronic applications, the use of earth-scarce lanthanides remains a crucial problem to be solved for further development. In this work, two manganese-based LSRMs, ()-(+)-1-phenylethylammonium manganese bromide, (R-PEA)MnBr, and ()-(-)-1-phenylethylammonium manganese bromide, (S-PEA)MnBr, are successfully demonstrated. Both (R-PEA)MnBr and (S-PEA)MnBr show a kinetically stable red-emissive amorphous state and a thermodynamically stable green-emissive crystalline state at room temperature, where the fully reversible transition can be done through melt-quenching and annealing processes.

Enhanced oxygen evolution and power density of Co/Zn@NC@MWCNTs for the application of zinc-air batteries.

Rechargeable zinc-air batteries (ZABs) are viewed as a promising solution for electric vehicles due to their potential to provide a clean, cost-effective, and sustainable energy storage system for the next generation. Nevertheless, sluggish kinetics of the oxygen evolution reaction (OER), the oxygen reduction reaction (ORR) at the air electrode, and low power density are significant challenges that hinder the practical application of ZABs. The key to resolving the development of ZABs is developing an affordable, efficient, and stable catalyst with bifunctional catalytic.

Alkali Metals Activated High Entropy Double Perovskites for Boosted Hydrogen Evolution Reaction.

An efficient and facile water dissociation process plays a crucial role in enhancing the activity of alkaline hydrogen evolution reaction (HER). Considering the intricate influence between interfacial water and intermediates in typical catalytic systems, meticulously engineered catalysts should be developed by modulating electron configurations and optimizing surface chemical bonds. Here, a high-entropy double perovskite (HEDP) electrocatalyst La(CoNiMgZnNaLi)RuO, achieving a reduced overpotential of 40.

Bimetallic nanoalloys planted on super-hydrophilic carbon nanocages featuring tip-intensified hydrogen evolution electrocatalysis.

The insufficient availability and activity of interfacial water remain a major challenge for alkaline hydrogen evolution reaction (HER). Here, we propose an "on-site disruption and near-site compensation" strategy to reform the interfacial water hydrogen bonding network via deliberate cation penetration and catalyst support engineering. This concept is validated using tip-like bimetallic RuNi nanoalloys planted on super-hydrophilic and high-curvature carbon nanocages (RuNi/NC).

Ruthenium Single-Atom Modulated Protonated Iridium Oxide for Acidic Water Oxidation in Proton Exchange Membrane Electrolysers.

Proton exchange membrane water electrolysers promise to usher in a new era of clean energy, but they remain a formidable obstacle in designing active and durable electrocatalysts for the acidic oxygen evolution reaction (OER). In this study, a protonated iridium oxide embedded with single-atom dispersed ruthenium atoms (HIr RuO) that demonstrates exceptional activity and stability in acidic water oxidation is introduced. The single Ru dopants favorably induce localized oxygen vacancies in the Ir─O lattice, synergistically strengthening the adsorption of OOH* intermediates and enhancing the intrinsic OER activity.

Synergistic ROS Generation via Core-Shell Nanostructures with Increased Lattice Microstrain Combined with Single-Atom Catalysis for Enhanced Tumor Suppression.

This study emphasizes the innovative application of FePt and Cu core-shell nanostructures with increased lattice microstrain, coupled with Au single-atom catalysis, in significantly enhancing OH generation for catalytic tumor therapy. The combination of core-shell with increased lattice microstrain and single-atom structures introduces an unexpected boost in hydroxyl radical (OH) production, representing a pivotal advancement in strategies for enhancing reactive oxygen species. The creation of a core-shell structure, FePt@Cu, showcases a synergistic effect in OH generation that surpasses the combined effects of FePt and Cu individually.

Charge Redistribution in High-Entropy Perovskite Oxide Porous Nanotubes Boosts Nitrate Electroreduction to Ammonia.

High-entropy perovskite oxides are promising materials in the field of electrocatalysis due to their advantages such as large spatial composition regulation, entropy effects, and tunable material properties. However, the preparation of high-entropy perovskite oxides with stable and controllable structures still remains challenging. Herein, we fabricated a series of high-entropy perovskite oxide porous nanotubes (PNTs) by electrospinning as efficient electrocatalysts for the nitrate reduction reaction (NORR).

A catalyst family of high-entropy alloy atomic layers with square atomic arrangements comprising iron- and platinum-group metals.

We report a catalyst family of high-entropy alloy (HEA) atomic layers having three elements from iron-group metals (IGMs) and two elements from platinum-group metals (PGMs). Ten distinct quinary compositions of IGM-PGM-HEA with precisely controlled square atomic arrangements are used to explore their impact on hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR). The PtRuFeCoNi atomic layers perform enhanced catalytic activity and durability toward HER and HOR when benchmarked against the other IGM-PGM-HEA and commercial Pt/C catalysts.

Strain-Triggered Distinct Oxygen Evolution Reaction Pathway in Two-Dimensional Metastable Phase IrO via CeO Loading.

A strain engineering strategy is crucial for designing a high-performance catalyst. However, how to control the strain in metastable phase two-dimensional (2D) materials is technically challenging due to their nanoscale sizes. Here, we report that cerium dioxide (CeO) is an ideal loading material for tuning the in-plane strain in 2D metastable 1T-phase IrO (1T-IrO) via an in situ growth method.

Site-Selective Zn-Metalation in Poly-Triphenyl Amine-based Porous Organic Polymer for Solid-Gas Phase CO Photoreduction.

Harvesting solar energy to produce value-added chemicals from carbon dioxide (CO) presents a promising route for addressing the complexities of sustainable energy systems and environmental issues. In this context, the development of metal-coordinated porous organic polymers (POPs) offers a vital avenue for improving the photocatalytic performance of organic motifs. The current study presents a metal-integrated photocatalytic system (namely, ) developed via a one-pot Friedel-Crafts (F.

Interrogation of 3d Transition Bimetallic Nanocrystal Nucleation and Growth Using Electron Microscope and Synchrotron X-ray Techniques.

Understanding the nucleation and growth mechanism of 3d transition bimetallic nanocrystals (NCs) is crucial to developing NCs with tailored nanostructures and properties. However, it remains a significant challenge due to the complexity of 3d bimetallic NCs formation and their sensitivity to oxygen. Here, by combining electron microscopy and synchrotron X-ray techniques, we elucidate the nucleation and growth pathways of Fe-Ni NCs.

Close Intimacy between PtIn Clusters and Zeolite Channels for Ultrastability toward Propane Dehydrogenation.

Propane dehydrogenation (PDH) serves as a pivotal intentional technique to produce propylene. The stability of PDH catalysts is generally restricted by the readsorption of propylene which can subsequently undergo side reactions for coke formation. Herein, we demonstrate an ultrastable PDH catalyst by encapsulating PtIn clusters within silicalite-1 which serves as an efficient promoter for olefin desorption.

Augmented Electrochemical Oxygen Evolution by d-p Orbital Electron Coupling.

While high-entropy alloys, high-entropy oxides, and high-entropy hydroxides, are advanced as a novel frontier in electrocatalytic oxygen evolution, their inherent activity deficiency poses a major challenge. To achieve the unlimited goal to tailor the structure-activity relationship in multicomponent systems, entropy-driven composition engineering presents substantial potential, by fabricating high-entropy anion-regulated transition metal compounds as sophisticated oxygen evolution reaction electrocatalysts. Herein, a versatile 2D high-entropy metal phosphorus trisulfide is developed as a promising and adjustable platform.