Compared with acidic environments, promoting the water dissociation process is crucial for speeding up hydrogen evolution reaction (HER) kinetics in alkaline electrolyte. Although the construction of heterostructured electrocatalysts by hybridizing noble metals with metal (hydr)oxides has been reported as a feasible approach to achieve high performance, the high cost, complicated fabrication process, and unsatisfactory mass activity limit their large-scale applications. Herein, we report a single-phase HER electrocatalyst composed of single-atom ruthenium (Ru) incorporated into a cobalt oxide spine structure (denoted as Ru SA/CoO), which possesses exceptional HER performance in alkaline media via unusual atomic-scale Ru-Co pair sites.
View Article and Find Full Text PDFColossal magnetoresistance (CMR) effects have been extensively studied in ABO perovskite manganites where the Mn-O-Mn double-exchange mechanism plays a pivotal role. However, A-site-ordered AA'BO-type quadruple perovskite oxides exhibit significantly suppressed double exchange due to their extremely small B-O-B bond angles (≈140°), hindering the realization of intrinsic CMR effects. Here, we report the design and synthesis of a novel quadruple perovskite oxide Pb(PbHg)MnO (PPHMO) characterized by an unusually increased Mn-O-Mn bond angle of up to 153°.
View Article and Find Full Text PDFPlatinum (Pt) has been documented as the top-tier fuel cell catalyst, yet it faces a notable challenge regarding its poor CO tolerance and sluggish oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs), particularly when using CO-contaminated blue and gray H. Here, we present an interfacial metal coordination strategy to design a bifunctional platinum-cobalt (PtCo) intermetallic catalyst integrated with a tin-nitrogen-carbon (Sn-N-C) support, which forms Pt-Sn-N bonds that substantially boost both ORR activity and CO tolerance. The PtCo/Sn-N-C-made fuel cell achieves a topmost peak power density of 2.
View Article and Find Full Text PDFReversible protonic ceramic cells (R-PCCs) hold significant promise for energy storage and conversion. However, achieving high-performance, large-scale cells remains challenging, primarily due to issues with compatibility and adhesion at the electrode-electrolyte interface. Here, a scalable strategy is presented for regulating an active interface structure (AIS) via tape casting to develop high-performance, durable R-PCCs.
View Article and Find Full Text PDFObjectives: Family and other carers of people with dementia can potentially benefit from training and support to reduce the negative impacts of caregiving and prevent harm to care recipients. While interventions for carers in low- and middle-income countries (LMICs) are emerging, their effectiveness is not well understood. Through a systematic review and meta-analysis, the objective was to evaluate the effectiveness of interventions to support carers of people with dementia in improving the well-being of carers and their care recipients in LMICs.
View Article and Find Full Text PDFHydrogen (H) manipulation plays a significantly important role in many important applications, in which the occurrence of hydrogen spillover generally shows substrate-dependent behavior. It therefore remains an open question about how to trigger the hydrogen spillover on the substrates that are generally hydrogen spillover forbidden. Here a new metastable-phase 2D edge-sharing oxide: six-hexagonal phase-hafnium oxide (Hex-HfO, space group: P6mc (186)) with the coordination number of six is demonstrated, which serves as an ideal platform for activating efficient hydrogen spillover after loading Ru nanoclusters (Ru/Hex-HfO).
View Article and Find Full Text PDFLung cancer remains the leading cause of cancer-related mortality worldwide, characterized by its complexity and heterogeneity [...
View Article and Find Full Text PDFDue to the intricate nature of cancer development and progression, various types of cancer are increasingly prevalent worldwide [...
View Article and Find Full Text PDFCuO octahedra usually show elongated distortion, leading to active orbitals and planar exchange interactions, while compressed CuO octahedra with active orbitals and unidirectional exchange interactions are exceptionally rare. Here, we design and synthesize a new frustrated antiferromagnet CaCuFeO through a high-pressure and high-temperature approach, in which robust compressed CuO octahedra are realized, separating the FeO sheets that comprise zigzag spin ladders. Magnetic susceptibility and specific heat measurements exhibit a long-range antiferromagnetic order below the Néel temperature of 165 K, which is further confirmed by neutron diffraction.
View Article and Find Full Text PDFReducing green hydrogen production cost is critical for its widespread application. Proton-exchange-membrane water electrolyzers are among the most promising technologies, and significant research has been focused on developing more active, durable, and cost-effective catalysts to replace expensive iridium in the anode. Ruthenium oxide is a leading alternative while its stability is inadequate.
View Article and Find Full Text PDFAnodic oxygen evolution reaction (OER) exhibits a sluggish four-electron transfer process, necessitating catalysts with exceptional catalytic activity to enhance its kinetic rate. Van der Waals layered oxides are ideal materials for catalyst design, yet its stability for acidic OER remains large obstacle. Doping provides a crucial way to improve the activity and stability simultaneously.
View Article and Find Full Text PDFCaCuFeReO 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.
View Article and Find Full Text PDFOxygen 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).
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Ruthenium dioxide (RuO) is one of the promising catalysts for the acidic oxygen evolution reaction (OER). However, designing RuO catalysts with good activity and stability remains a significant challenge. In this work, we propose the manganese (Mn)-doped RuO assembly as a catalyst for the OER with improved activity and stability.
View Article and Find Full Text PDFPtRu-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 SrRuPtOH nanobelts (a-SrRuPtOH NBs). The a-SrRuPtOH NBs has 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.
View Article and Find Full Text PDFThe high overpotential and unsatisfactory stability of RuO-based catalysts seriously hinder their application in acidic oxygen evolution reaction (OER). Herein, a Ru@RuO core/shell catalyst doped with atomically dispersed Mn species, denoted as Ru@Mn-RuO, is reported, which is prepared by a facile one-pot method. Detailed structural characterizations confirm that Mn is homogeneously and atomically distributed in RuO shell, which causes lattice contraction of RuO.
View Article and Find Full Text PDFMethane (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.
View Article and Find Full Text PDFNickel-based electrocatalysts are promising for industrial water electrolysis, but the dense hydroxyl oxide layer formed during the oxygen evolution reaction (OER) limits active sites accessibility and presents challenges in balancing structural stability with effective charge transfer. Based on this, an efficient in situ leaching strategy is proposed to construct grain boundary-rich catalyst structure with high charge transfer ability and a deep catalytic active layer reached >200-nm. Under OER conditions, stable sub-nano NiAl particles are embedded in Ni(Fe)OOH, originating from leaching out the unstable NiAl phase of the initial NiAl/NiAl alloy doped with Fe.
View Article and Find Full Text PDFAs 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.
View Article and Find Full Text PDFProton 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.
View Article and Find Full Text PDFDeveloping 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.
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