The atom arrangement in carbon electrocatalysts is crucial for enhancing the intrinsic activity toward oxygen reduction reactions (ORRs), a key process in multiple renewable energy systems. However, the challenge of designing electrocatalysts with improved performance by manipulating atomic arrangement has been limited by synthetic constraints and a lack of understanding of the catalytic phase formation. Herein, we gain atomic-level insight into the origin of a highly active site by creating a model catalyst with a heteroatom-decorated carbon matrix of a specific configuration.
View Article and Find Full Text PDFSingle-atom materials (SAMs) are a fascinating class of nanomaterials with exceptional catalytic properties, offering immense potential for energy storage and conversion. This work explores their advantages, challenges, and underlying mechanisms, providing valuable insights for rational design. By precisely controlling active sites, SAMs enable efficient charge and energy transfer, ultimately enhancing system performance.
View Article and Find Full Text PDFThe ability to control the morphology of supported alloy nanoparticles in an ultrasmall size range (≲5 nm) is challenging especially under reactive oxygen at elevated temperatures. The understanding of factors governing such nanoscale surface-dominated interfacial interactions and reactivities remains elusive since existing studies are mostly based on crystalline phases of larger-sized nanoparticles and the associated nanoparticle-support surface interactions. Here, we reveal a counterintuitive spreading and retraction phenomenon by in situ tracking of the spatiotemporal dynamics of alumina-supported ultrasmall ternary alloy nanoparticles under oxygen at different temperatures as a model system.
View Article and Find Full Text PDFThe ability to control phase structures and surface sites of ultrasmall alloy nanoparticles under reaction conditions is essential for preparing catalysts by design. This is, however, challenging due to limited understanding of the atomic-scale phases and their correlation with the ensemble-averaged structures and activities of catalysts during catalytic reactions. We reveal here a dynamic structural stability of alumina-supported ultrasmall and equiatomic copper-gold alloy nanoparticles under reaction conditions as a model system in the in situ/operando study.
View Article and Find Full Text PDFAchieving a synergistic, rapid, and concentrated energy release process of ammonium perchlorate (AP) is of vital significance for boosting the thrust of composite solid propellants. However, conventional catalytic promoters often exhibit suboptimal catalytic kinetics due to inefficient utilization of active sites. Herein, atomically dispersed Cu-coordinated covalent organic frameworks (COFs)-based catalytic promoters are reported, decorating with energetic anion groups.
View Article and Find Full Text PDFBackground: Patients with cirrhosis with hepatopulmonary syndrome (HPS) have a poorer prognosis. The disease has a subtle onset, symptoms are easily masked, clinical attention is insufficient, and misdiagnosis rates are high.
Aim: To compare the clinical characteristics of patients with cirrhosis, cirrhosis combined with intrapulmonary vascular dilatation (IPVD), and HPS, and to establish predictive models for IPVD and HPS.
Artificial photosynthesis offers a promising pathway to address environmental challenges and the global energy crisis by converting solar energy into storable chemical fuels such as hydrogen. Among various photocatalysts, transition metal-based materials have garnered significant attention due to their tunable crystal phase, morphology, surface active sites, and other key properties. This review provides a comprehensive overview of recent advances in transition metal-based photocatalysts for hydrogen production, with a particular focus on modification strategies and their underlying mechanisms.
View Article and Find Full Text PDFNon-noble metal-based heteroatom compounds demonstrate excellent electrocatalytic activity for the oxygen evolution reaction (OER). However, the origin of this activity, driven by structure evolution effects, remains unclear due to the lack of effective in situ/operando techniques. Herein, we employ the operando quick-scan x-ray absorption fine structure (Q-XAFS) technique coupled with in situ controlled electrochemical potential to establish a structure-activity correlation of the OER catalyst.
View Article and Find Full Text PDFExploration (Beijing)
February 2025
Proton exchange-membrane fuel cell (PEMFC) is a clean and efficient type of energy storage device. However, the sluggish reaction rate of the cathode oxygen reduction reaction (ORR) has been a significant problem in its development. This review reports the recent progress of advanced electrocatalysts focusing on the interface/surface electronic structure and exploring the synergistic relationship of precious-based and non-precious metal-based catalysts and support materials.
View Article and Find Full Text PDFJ Back Musculoskelet Rehabil
March 2025
Background: Existing evidence is insufficient to support that acupuncture is effective in treating ankylosing spondylitis (AS) due to the constraints of acupuncture site and manipulation, and relatively straightforward study treatments and indicators.
Objective: By incorporating high-quality original literature, this study aims to evaluate the effectiveness of acupuncture for AS and to demonstrate acupuncture as a non-drug supplementary and alternative means for treating AS.
Methods: We searched seven databases from their inception to March 31, 2023.
J Am Chem Soc
December 2024
Enhancing corrosion resistance is essential for developing efficient electrocatalysts for acidic oxygen evolution reaction (OER). Herein, we report the strategic manipulation of the local compressive strain to reinforce the anti-corrosion properties of the non-precious CoO support. The incorporation of Ru single atoms, larger in atomic size than Co, into the CoO lattice (Ru-CoO), triggers localized strain compression and lattice distortion on the Co-O lattice.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Chemical modification via functional dopants in carbon materials holds great promise for elevating catalytic activity and stability. To gain comprehensive insights into the pivotal mechanisms and establish structure-performance relationships, especially concerning the roles of dopants, remains a pressing need. Herein, we employ computational simulations to unravel the catalytic function of heteroatoms in the acidic oxygen evolution reaction (OER), focusing on a physical model of high-electronegative F and N co-doped carbon matrix.
View Article and Find Full Text PDF, a perennial herb belonging to the Asteraceae family, is a vital ingredient in traditional Chinese medicine. Increased demands for the herb have led to its widespread cultivation in China, but the corresponding increase in pesticide use has raised concerns about pesticide residues. Such residues would affect the safety and global market potential of .
View Article and Find Full Text PDFBackground: Sarcoidosis is a multisystem disease characterized by granuloma formation in various organs. Sarcoidosis-related flexor tendon contractures are uncommon in clinical settings. This contracture is similar to stenosing tenosynovitis and potentially leads to misdiagnosis and mistreatment.
View Article and Find Full Text PDFBackground: In this study, we compared the clinical efficacy of endoscope-assisted anterior cervical discectomy and fusion (ACDF) with open ACDF in the treatment of single-segment cervical spondylotic myelopathy.
Methods: A retrospective analysis was performed on 52 patients with single-segment cervical spondylotic myelopathy between June 2021 and February 2022, including 33 males and 19 females, with a mean age of 58.42 ± 9.
Angew Chem Int Ed Engl
February 2024
Understanding the correlation between the structural evolution of electrocatalysts and their catalytic activity is both essential and challenging. In this study, we investigate this correlation in the context of the oxygen evolution reaction (OER) by examining the influence of structural disorder during and after dynamic structural evolution on the OER activity of Fe-Ni (oxy)hydroxide catalysts using operando X-ray absorption spectroscopy, alongside other experiments and theoretical calculations. The Debye-Waller factors obtained from extended X-ray absorption fine structure analyses reflect the degree of structural disorder and exhibit a robust correlation with the intrinsic OER activities of the electrocatalysts.
View Article and Find Full Text PDFHuan Jing Ke Xue
August 2023
The effects of coconut fiber biochar (CFB) and nitrate-modified coconut fiber biochar (NCFB) on the passivation of exogenous lead (Pb) in paddy soils and their underlying mechanisms were investigated using soil incubation experiments combined with spectroscopic techniques such as scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), synchrotron radiation X-ray fluorescence (SRXRF), and Fourier transform infrared absorption spectroscopy (FTIR). The effects of NCFB and CFB on the passivation of exogenous lead (Pb) in paddy soils and its underlying mechanisms were investigated. Compared with that of CFB, the inner wall of NCFB honeycomb pores was rougher, and the amount of alcohol-phenol-ether functional groups containing the C-O structure and the amount of carboxyl groups containing the C[FY=,1]O/O[FY=,1]C-O structure on the surface of CFB was significantly decreased after nitric acid modification.
View Article and Find Full Text PDFManipulating the intrinsic activity of heterogeneous catalysts at the atomic level is an effective strategy to improve the electrocatalytic performances but remains challenging. Here, atomically dispersed Ni anchored on CeO particles entrenched on peanut-shaped hollow nitrogen-doped carbon structures (-Ni/CeO@NC) is rationally designed and synthesized. The as-prepared -Ni/CeO@NC catalyst exhibits substantially boosted intrinsic activity and greatly reduced overpotential for the electrocatalytic oxygen evolution reaction.
View Article and Find Full Text PDFHere, an ultra-highly active Ni-MOF-5 catalyst with high Ni loading for ethylene dimerization is reported. The Ni-MOF-5 catalysts are synthesized by a facile one-pot co-precipitation method at room temperature, where Ni replaces Zn in MOF-5. Unlike Zn with tetrahedral coordination in MOF-5, Ni is coordinated with extra solvent molecules except for four-oxygen from the framework.
View Article and Find Full Text PDFHybrid materials, integrating the merits of individual components, are ideal structures for efficient oxygen evolution reaction (OER). However, the rational construction of hybrid structures with decent physical/electrochemical properties is yet challenging. Herein, a promising OER electrocatalyst composed of trimetallic metal-organic frameworks supported over S/N-doped carbon macroporous fibers (S/N-CMF@Fe Co Ni -MOF) via a cation-exchange strategy is delicately fabricated.
View Article and Find Full Text PDFActivity, cost, and durability are the trinity of catalysis research for the electrochemical oxygen reduction reaction (ORR). While studies towards increasing activity and reducing cost of ORR catalysts have been carried out extensively, much effort is needed in durability investigation of highly active ORR catalysts. In this work, we examined the stability of a trimetallic PtPdCu catalyst that has demonstrated high activity and incredible durability during ORR using density functional theory (DFT) based computations.
View Article and Find Full Text PDFCopper (Cu)-based catalysts generally exhibit high C selectivity during the electrochemical CO reduction reaction (CORR). However, the origin of this selectivity and the influence of catalyst precursors on it are not fully understood. We combine operando X-ray diffraction and operando Raman spectroscopy to monitor the structural and compositional evolution of three Cu precursors during the CORR.
View Article and Find Full Text PDF2D materials show many particular properties, such as high surface-to-volume ratio, high anisotropic degree, and adjustable chemical functionality. These unique properties in 2D materials have sparked immense interest due to their applications in photocatalytic systems, resulting in significantly enhanced light capture, charge-transfer kinetics, and surface reaction. Herein, the research progress in 2D photocatalysts based on varied compositions and functions, followed by specific surface modification strategies, is introduced.
View Article and Find Full Text PDFACS Appl Mater Interfaces
March 2022
The ability to harness the catalytic oxidation of hydrocarbons is critical for both clean energy production and air pollutant elimination, which requires a detailed understanding of the dynamic role of the nanophase structure and surface reactivity under the reaction conditions. We report here findings of an in situ/operando study of such details of a ternary nanoalloy under the propane oxidation condition using high-energy synchrotron X-ray diffraction coupled to atomic pair distribution function (HE-XRD/PDF) analysis and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The catalysts are derived by alloying Pt with different combinations of second (Pd) and third (Ni) transition metals, showing a strong dependence of the catalytic activity on the Ni content.
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