Angew Chem Int Ed Engl
November 2024
Metal-organic hybrid catalysts with highly tunable single-sites are promising for oxygen-evolution reaction (OER), but molecular-scale understanding of underlying reaction mechanisms still remain elusive on these bulk materials. Herein, we report a direct construction of heterogenized molecular complexes stabilized on carbon substrates via coordinating Fe-Ni sites with four aromatic carboxylate ligands (FeNi-L). The ligands-tuning π-π stacking interaction between aromatic carboxylate ligands and carbon supports promote the oxidative charge accumulation on Fe-Ni sites via fast electron transferring, thus the optimized FeNi-L rendering a mass activity of 6680 A g at 0.
View Article and Find Full Text PDFPurpose: To explore the influence of gingival biotype and width of keratinized gingiva on peri-implant bone tissue, soft tissue health, and esthetic outcome of the papilla surrounding single posterior maxillary implants.
Methods: Seventy-eight patients who underwent single posterior maxillary implant surgery from May 2019 to September 2022 were selected, involving the placement of 78 implants. Based on periodontal probing outcomes one month post-restoration, the patients were divided into thin gingival biotype group(n=32) and thick gingival biotype group(n=46).
Autophagy is an intracellular degradation process that is important for the development and pathogenicity of phytopathogenic fungi and for the defence response of plants. However, the molecular mechanisms underlying autophagy in the pathogenicity of the plant pathogenic oomycete , the causal agent of litchi downy blight, have not been well characterized. In this study, the autophagy-related protein ATG2 homolog, PlATG2, was identified and characterized using a CRISPR/Cas9-mediated gene replacement strategy in .
View Article and Find Full Text PDFIn recent years, neuromorphic computing is recognized as a promising path to further improve the efficiency of integrated computing system in the post-Moore era, relying on its high parallelism. As a key fundamental element in hardware-implementing neuromorphic system, the synaptic device has made substantial research progress. Among these, SiO trapping-based memristive devices generally have systematically integrated merits, such as ease of fabrication and high CMOS process compatibility, but electrochemical activity to oxygen makes them unreliable for operating in air.
View Article and Find Full Text PDFis the pathogen of litchi downy blight, which is the most serious disease in litchi. Autophagy is an evolutionarily conserved catabolic process in eukaryotes. Atg8 is a core protein of the autophagic pathway, which modulates growth and pathogenicity in the oomycete .
View Article and Find Full Text PDFIn the post-Moore era, the gradually saturated computational capability of conventional digital computers showing the opposite trend as the exponentially increasing data volumes imperatively required a platform or technology to break this bottleneck. Brain-inspired neuromorphic computing promises to inherently improve the efficiency of information processing and computation by means of the highly parallel hardware architecture to reduce global data transmission. Here, we demonstrate a compact device technology based on the barrier asymmetry to achieve zero-consumption self-powered synaptic devices.
View Article and Find Full Text PDFAmong the platinum-group metals, ruthenium (Ru), with a low water dissociation energy, is considered a promising alternative to substitute Pt for catalyzing hydrogen evolution reaction (HER). However, optimizing the adsorption-desorption energies of H and OH intermediates on Ru catalytic sites is extremely desirable but remains challenging. Inspired by the natural catalytic characteristics of Mn-oxygen complex, this study reports to design Mn-oxygen compounds coordinated Ru sites (MOC-Ru) with deprotonated and low oxophilic microenvironments for modulating the adsorption-desorption of H and OH to promote HER kinetics.
View Article and Find Full Text PDFMetal alloys-structured electrocatalysts (MAECs) have made essential contributions to accelerating the practical applications of electrocatalytic devices in renewable energy systems. However, due to the complex atomic structures, varied electronic states, and abundant supports, precisely decoding the metal-metal interactions and structure-activity relationships of MAECs still confronts great challenges, which is critical to direct the future engineering and optimization of MAECs. Here, this timely review comprehensively summarizes the latest advances in creating the MAECs, including the metal-metal interactions, coordination microenvironments, and structure-activity relationships.
View Article and Find Full Text PDFThe lack of high efficiency and pH-universal bifunctional electrocatalysts for water splitting to hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) hinders the large-scale production of green hydrogen. Here, an IrPd electrocatalyst supported on ketjenblack that exhibits outstanding bifunctional performance for both HER and OER at wide pH conditions is presented. The optimized IrPd catalyst exhibits a specific activity of 4.
View Article and Find Full Text PDFRuthenium (Ru)-based catalysts have displayed compelling hydrogen evolution activities, which hold the promising potential to substitute platinum in alkaline H -evolution. In the challenging alkaline electrolytes, the water-dissociation process involves multistep reactions, while the profound origin and intrinsic factors of diverse Ru species on water-dissociation pathways and reaction principles remain ambiguous. Here the fundamental origin of water-dissociation pathways of Ru-based catalysts in alkaline media to be from their unique electronic structures in complex coordination environments are disclosed.
View Article and Find Full Text PDFCompared to platinum catalysts, ruthenium (Ru) is disclosed as a promising alternative for alkaline water electrolysis due to its similar hydrogen adsorption energy and relatively lower water dissociation barrier. However, in the challenging alkaline media, the dissatisfied Volmer step during water dissociation of Ru metal prohibits its practical applications. Here, a new pathway to modulate the electronic environment of Ru catalysts via a local charge transfer strategy for tuning the water dissociation kinetics and accelerating the alkaline water electrolysis is proposed.
View Article and Find Full Text PDFPlatinum-based catalysts occupy a pivotal position in diverse catalytic applications in hydrogen chemistry and electrochemistry, for instance, the hydrogen evolution reactions (HER). While adsorbed Pt atoms on supports often cause severe mismatching on electronic structures and HER behaviors from metallic Pt due to the different energy level distribution of electron orbitals. Here, the design of crystalline lattice-confined atomic Pt in metal carbides using the Pt-centered polyoxometalate frameworks with strong PtO-metal covalent bonds is reported.
View Article and Find Full Text PDFThe antiparasitic drug nitazoxanide (NTZ) has received considerable attention for its potential in cancer therapy. In this study, we demonstrate that tizoxanide (TIZ), an active metabolite of NTZ, exhibits antiglioma activity and by inducing G2/M cell cycle arrest and apoptosis. , TIZ dose-dependently inhibited the proliferation of U87, U118, and A172 human glioblastoma (GBM) cells at 48 h with IC values of 1.
View Article and Find Full Text PDFis an important plant pathogenic oomycete with multiple hosts. The P4-ATPases, aminophospholipid translocases (APTs), play essential roles in the growth and pathogenesis of fungal pathogens. However, the function of P4-ATPase in remains unclear.
View Article and Find Full Text PDFMetalN-coordinated centers supported by carbonaceous substrates have emerged as promising artificial metalloenzymes (AMEs) to mimic the biocatalytic effects of their natural counterparts. However, the synthesis of well-defined AMEs that contain different atomic metalN centers but present similar physicochemical and coordination structures remains a substantial challenge. Here, 20 different types of AMEs with similar geometries and well-defined atomic metalN-coordinated centers are synthesized to compare and disclose the catalytic activities, substrate selectivities, kinetics, and reactive oxygen species (ROS) products.
View Article and Find Full Text PDFRab GTPases are key regulators of membrane and intracellular vesicle transports. However, the biological functions of FgRab1 are still unclear in the devastating wheat pathogen . In this study, we generated constitutively active (CA) and dominant-negative (DN) forms of from the wild-type PH-1 background for functional analyses.
View Article and Find Full Text PDFDeveloping efficient, durable, and low-cost earth-abundant elements-based oxygen evolution reaction (OER) catalysts by rapid and scalable strategies is of great importance for future sustainable electrochemical hydrogen production. The earth-abundant high-valency metals, especially vanadium, can modulate the electronic structure of 3d metal oxides and oxyhydroxides and offer the active sites near-optimal adsorption energies for OER intermediates. Here, the authors propose a facile assembling and regulating strategy to controllably synthesize a serial of transition metal (CoFe, NiFe, and NiCo)-based vanadates for efficient OER catalysis.
View Article and Find Full Text PDFCoherent frequency conversion of vector beams (VBs) without distorting their intensity profile or spatial polarization distribution is important for novel applications in quantum and classical regimes. Here, we experimentally and theoretically investigate VB transfer from near-infrared to blue light using a Sagnac interferometer, combining the parametric four-wave mixing process in atomic vapor. The vector probe beam is converted into a completely different wavelength, and the vector mode of the generated blue beam is highly similar to the incident probe beam.
View Article and Find Full Text PDFTrehalose biosynthesis pathway is a potential target for antifungal drug development, and trehalose 6-phosphate (T6P) accumulation is widely known to have toxic effects on cells. However, how organisms maintain a safe T6P level and cope with its cytotoxicity effects when accumulated have not been reported. Herein, we unveil the mechanism by which the rice blast fungus Magnaporthe oryzae avoids T6P accumulation and the genetic and physiological adjustments it undergoes to self-adjust the metabolite level when it is unavoidably accumulated.
View Article and Find Full Text PDFEngineering efficient zinc-air batteries have attracted tremendous attention because of their essential role in the field of renewable energy systems. However, the sluggish reaction kinetics of the oxygen reduction reaction (ORR) at the air cathode impair the battery performance significantly. Recently, metal-N-C-based porous carbon nanoarchitectures have emerged as promising ORR electrocatalysts in zinc-air batteries.
View Article and Find Full Text PDFElectrochemical water splitting has attracted significant attention as a key pathway for the development of renewable energy systems. Fabricating efficient electrocatalysts for these processes is intensely desired to reduce their overpotentials and facilitate practical applications. Recently, metal-organic framework (MOF) nanoarchitectures featuring ultrahigh surface areas, tunable nanostructures, and excellent porosities have emerged as promising materials for the development of highly active catalysts for electrochemical water splitting.
View Article and Find Full Text PDFMol Plant Microbe Interact
July 2021
The causal agent of stem and root rot of cowpea, , is a widely distributed species of the genus. Here, we generate a high-quality complete genome assembly of PSY2020 (89.39 Mb, N 2.
View Article and Find Full Text PDFTo deal with the ever-growing toxic benzene-derived compounds in the water system, extensive efforts have been dedicated for catalytic degradation of pollutants. However, the activities and efficiencies of the transition metal-based nanoparticles or single-atom sites are still ambiguous in Fenton-like reactions. Herein, to compare the Fenton-like catalytic efficiencies of the nanoparticles and single atoms, the free-standing nanofibrous catalyst comprising Co nanocrystals and Co-N codoped carbon nanotubes (CNTs) or bare Co-N doped CNTs is fabricated.
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