Compared to the raw NCP-0, which exhibits a hydrogen evolution rate of 64 mol g⁻¹h⁻¹, the hollow-structured NCP-60 particles display a significantly improved rate of 128 mol g⁻¹h⁻¹. Moreover, the H2 evolution rate of the resultant NiCoP nanoparticles achieved 166 mol g⁻¹h⁻¹, a remarkable 25-fold increase compared to the NCP-0 sample, entirely devoid of any co-catalysts.
Hierarchical structures arise from the complexation of nano-ions with polyelectrolytes, producing coacervates; yet, the rational design of functional coacervates is hampered by the lack of comprehensive understanding of their structure-property relationship, which arises from intricate interactions. In complexation with cationic polyelectrolytes, well-defined, monodisperse 1 nm anionic metal oxide clusters, namely PW12O403−, display a tunable coacervation system, the control of which stems from the alteration of counterions (H+ and Na+) within the PW12O403−. Isothermal titration calorimetry (ITC) and Fourier transform infrared spectroscopy (FT-IR) measurements suggest that the interaction between PW12O403- and cationic polyelectrolytes is potentially modulated by counterion bridging, with hydrogen bonding or ion-dipole interactions with polyelectrolyte carbonyl groups playing a role. Employing small-angle X-ray scattering and neutron scattering, the condensed and complex coacervate structures are investigated. ZM 447439 clinical trial The coacervate, with H+ counterions, exhibits both crystallized and discrete PW12O403- clusters, displaying a loose polymer-cluster network, in contrast to the Na+-based system, which showcases a densely packed structure with aggregated nano-ions filling the polyelectrolyte network meshes. ZM 447439 clinical trial The super-chaotropic effect in nano-ion systems is elucidated by the bridging action of counterions, suggesting pathways for designing functional metal oxide cluster-based coacervates.
The viability of large-scale metal-air battery production and implementation hinges on the availability of economical, abundant, and effective oxygen electrode materials. In situ, a molten salt-mediated strategy is implemented to embed transition metal-based active sites into porous carbon nanosheets. Subsequently, a nitrogen-doped porous chitosan nanosheet, featuring well-defined CoNx (CoNx/CPCN) embellishments, was reported. Structural characterization and electrocatalytic investigations both highlight a powerful synergistic interaction between CoNx and porous nitrogen-doped carbon nanosheets, which significantly enhances the rate of the sluggish oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Featuring CoNx/CPCN-900 as the air electrode, the Zn-air batteries (ZABs) exhibited noteworthy durability, withstanding 750 discharge/charge cycles, achieving a high power density of 1899 mW cm-2, and a notable gravimetric energy density of 10187 mWh g-1 at a current density of 10 mA cm-2. Importantly, the assembled all-solid cell demonstrates superb flexibility coupled with a high power density, specifically 1222 mW cm-2.
The electronics/ion transport and diffusion kinetics of sodium-ion battery (SIB) anode materials can be improved using a novel strategy involving molybdenum-based heterostructures. Hollow MoO2/MoS2 nanospheres were successfully designed through an in-situ ion exchange methodology employing the spherical Mo-glycerate (MoG) coordination compound. The research on the structural evolution of pure MoO2, MoO2/MoS2, and pure MoS2 compositions has shown the structural preservation of the nanosphere through the S-Mo-S bond. The exceptional electrochemical kinetic performance of the obtained MoO2/MoS2 hollow nanospheres for sodium-ion batteries arises from the high conductivity of MoO2, the layered structure of MoS2, and the synergistic effect between the materials. Hollow MoO2/MoS2 nanospheres achieve a rate performance, retaining 72% of their capacity at a 3200 mA g⁻¹ current, in marked contrast to their performance at 100 mA g⁻¹. Restoring the current to 100 mA g-1 allows for recovery of the initial capacity, with a maximum capacity fading of 24% observed in pure MoS2. The hollow MoO2/MoS2 nanospheres also showcase consistent cycling stability, with a maintained capacity of 4554 mAh g⁻¹ after undergoing 100 cycles at 100 mA g⁻¹. The design strategy for the hollow composite structure, explored in this work, reveals key information regarding the creation of energy storage materials.
Lithium-ion batteries (LIBs) benefit from the high conductivity (approximately 5 × 10⁴ S m⁻¹) and substantial capacity (around 372 mAh g⁻¹) of iron oxides when employed as anode materials, making them a frequent subject of research. A gravimetric capacity value of 926 mAh g-1 (milliampere-hours per gram) was obtained. Practical application is constrained by the substantial volume shifts and high susceptibility to dissolution or aggregation that accompany charge-discharge cycles. We report a design strategy for the fabrication of yolk-shell porous Fe3O4@C anchored onto graphene nanosheets, yielding the material Y-S-P-Fe3O4/GNs@C. Not only does this particular structure create the necessary internal void space for Fe3O4's fluctuating volume, but it also provides a carbon shell to limit Fe3O4's expansion, thereby dramatically improving the capacity retention properties. The pores in Fe3O4 facilitate ion transport, and the graphene nanosheet-supported carbon shell enhances the overall conductivity. Consequently, the Y-S-P-Fe3O4/GNs@C composite shows a high reversible capacity (1143 mAh g⁻¹), excellent rate capability (358 mAh g⁻¹ at 100 A g⁻¹), and a significant cycle life with consistent cycling stability (579 mAh g⁻¹ remaining after 1800 cycles at 20 A g⁻¹), when used in LIBs. The full-cell, comprised of Y-S-P-Fe3O4/GNs@C//LiFePO4, demonstrates a high energy density of 3410 Wh kg-1 when assembled, coupled with a power density of 379 W kg-1. An Fe3O4-based anode material, Y-S-P-Fe3O4/GNs@C, is shown to be efficient for lithium-ion battery applications.
To mitigate the mounting environmental problems stemming from the dramatic increase in carbon dioxide (CO2) concentrations, a worldwide reduction in CO2 emissions is urgently required. Geological carbon sequestration using gas hydrates within marine sediments stands as a promising and attractive means to reduce CO2 emissions, given its considerable storage capacity and inherent safety measures. Despite the potential, the slow kinetics and unclear enhancement mechanisms associated with CO2 hydrate formation restrict the practical implementation of hydrate-based CO2 storage techniques. In this study, vermiculite nanoflakes (VMNs) and methionine (Met) were used to probe the synergistic effect of natural clay surfaces and organic matter on the rate of CO2 hydrate formation. VMNs dispersed in Met exhibited significantly reduced induction times and t90 values, differing by one to two orders of magnitude from Met solutions and VMN dispersions. Beyond this, the rate at which CO2 hydrates formed was significantly contingent upon the concentration of both Met and VMNs. The effect of Met side chains on CO2 hydrate formation arises from their ability to stimulate water molecules to form a structure akin to a clathrate. Whereas Met concentrations remained below 30 mg/mL, water molecules maintained their ordered structure, permitting CO2 hydrate formation; however, surpassing this threshold led to the disruption of this ordered structure by ammonium ions emanating from dissociated Met, inhibiting the formation of CO2 hydrate. Negatively charged VMNs in dispersion can diminish the inhibition through the adsorption of ammonium ions. This research explores the formation pathway of CO2 hydrate in the presence of clay and organic matter, vital components of marine sediments, and furthermore, contributes to the practical application of CO2 storage using hydrate technology.
Through the supramolecular assembly of phenyl-pyridyl-acrylonitrile derivative (PBT), WPP5, and organic pigment Eosin Y (ESY), a novel water-soluble phosphate-pillar[5]arene (WPP5)-based artificial light-harvesting system (LHS) was successfully created. WPP5, after interacting with the guest PBT, initially bound effectively to form WPP5-PBT complexes in water, which subsequently self-assembled into WPP5-PBT nanoparticles. Due to the presence of J-aggregates of PBT, WPP5 PBT nanoparticles displayed exceptional aggregation-induced emission (AIE) properties. These J-aggregates proved suitable as fluorescence resonance energy transfer (FRET) donors for artificial light-harvesting. Subsequently, the emission area of WPP5 PBT corresponded strongly to the UV-Vis absorption range of ESY, facilitating substantial energy transfer from WPP5 PBT (donor) to ESY (acceptor) by Förster resonance energy transfer (FRET) within the WPP5 PBT-ESY nanoparticles. ZM 447439 clinical trial A pronounced antenna effect (AEWPP5PBT-ESY) of 303 was determined for the WPP5 PBT-ESY LHS, surpassing the values obtained from recently developed artificial LHSs for photocatalytic cross-coupling dehydrogenation (CCD) reactions, implying a potential for use in photocatalytic reactions. Furthermore, the energy transfer from PBT to ESY drastically improved the absolute fluorescence quantum yields, escalating from a value of 144% (for WPP5 PBT) to an impressive 357% (for WPP5 PBT-ESY), thereby substantiating FRET mechanisms in the WPP5 PBT-ESY LHS. WPP5 PBT-ESY LHSs were utilized as photosensitizers to drive the catalytic CCD reaction of benzothiazole and diphenylphosphine oxide, subsequently releasing the captured energy. In contrast to the free ESY group (21%), the WPP5 PBT-ESY LHS exhibited a substantial cross-coupling yield of 75%, attributable to the transfer of PBT's UV energy to ESY for the CCD reaction. This suggests the potential for enhancing the catalytic activity of organic pigment photosensitizers in aqueous solutions.
To advance the practical utility of catalytic oxidation technology, it is paramount to illustrate the concurrent conversion patterns of a range of volatile organic compounds (VOCs) across various catalysts. Concerning the mutual influence of benzene, toluene, and xylene (BTX), a study on their synchronous conversion was performed on manganese dioxide nanowire surfaces.
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