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An efficient peroxymonosulfate activation by Nb2CTx-MXene mediated with CQDs composite catalyst for carbamazepine degradation: Kinetics and mechanistic insights
Nb2CTx-MXene with CQDs-modified catalyst was rationally designed and synthesized. • The composite exhibited highly efficient PMS activation for CBZ degradation. • Synergistic radical and non-radical oxidation pathways were experimentally validated. • Identifying key active sites and the degradation pathways improved understanding of Nb2CTx@CQDs catalytic performance. Persistent organic pollutants present long-term risks to aquatic ecosystems, calling for oxidation processes with well-defined activation mechanisms. In this work, an Nb 2 CTx- MXene composite decorated with ginger-derived carbon quantum dots (Nb 2 CTx@CQDs) was constructed to investigate interfacial peroxymonosulfate (PMS) activation for carbamazepine (CBZ) degradation in water. The surface chemistry, textural properties, and electronic features of the composite were systematically characterized. The Nb 2 CTx@CQDs(5 wt.%)/PMS system achieved 94.7 % CBZ removal within 50 min, corresponding to a pseudo-first-order rate constant k of 0.0598 min -1 under optimized conditions. Density functional theory calculations, together with Liquid chromatography-mass spectrometry (LC-MS) analysis, revealed the evolution of key intermediates and supported a stepwise CBZ degradation pathway. Mechanistic results indicate that PMS activation is governed by coupled radical and non-radical processes, promoted by CQDs-modified Nb 2 CTx surfaces playing a decisive role while, the evaluation of ecotoxicity analysis of CBZ intermediates suggested that they are much less harmful for ecosystem. This study highlights the importance of MXene surface modulation with CQDs for regulating PMS activation pathways and provides mechanistic insights relevant to advanced oxidation processes for the degradation of organic pollutants. Download: Download high-res image (291KB) Download: Download full-size image
One-pot synthesis of Ru/Nb2O5@Nb2C ternary photocatalysts for water splitting by harnessing hydrothermal redox reactions
MXenes, 2D transition metal carbides/nitrides, have been demonstrated as promising platform for fabricating novel composites with interesting photo-/electrochemical properties. It is desirable to gain insights into the reactivity of MXenes, enabling the controllable transformation of MXenes. Here, a one-pot hydrothermal synthesis method of MXene-based photocatalyst is validated by harnessing the reducibility of Nb 2 CT x MXene . The origin of reducibility of Nb 2 CT x during the hydrothermal oxidation process was demonstrated as the active hydrogen produced from the water splitting in the presence of Nb 2 CT x , which reduced Ru 3+ in situ to Ru nanoparticles on Nb 2 O 5 nanowires derived from Nb 2 CT x . Compared with the traditional photo-deposition method, the chemical valance of the noble metal Ru/Pt obtained by the one-pot synthesis method was closer to the metal state, which reduced the charge transfer resistance by 82.5%. It led to the photocatalytic hydrogen production of 10.11 mmol·h −1 ·g −1 with 41.25% apparent quantum yield at 313 nm.
Interlayer Engineering Construction of 2D Nb2CTx with Enlarged Interlayer Spacing Towards High Capacity and Rate Capability for Lithium-Ion Storage
The Li + storage rate capability and diffusion dynamics in two-dimensional (2D) materials are mainly determined by the interlayer spacing of materials. Investigating the effects of interlayer spacing on Li + diffusion rate in 2D materials can provide a theoretical guidance for developing the high rate 2D materials for Li + storage. Herein, a novel approach that P-phenylenediamine (PPDA) electrostatically intercalated into Nb 2 CT x layers is employed to facilitate fast Li + diffusion dynamics and improve diffusion rate for Li + storage. The PPDA molecules existed between Nb 2 CT x layers have “support and dragline” effects on layers structure during Li + insertion/exaction. The PPDA-Nb 2 CT x not only enlarges interlayer spacing ( d =1.27 nm) to accelerate the Li + diffusion rate, but also enhances the layered structure stability due to the “support and dragline” effects of PPDA molecules. The PPDA-Nb 2 CT x exhibits the excellent capacity of 400 mAh g −1 at a current density of 0.1 A g −1 and displays a superior capacity retention as 70.2 % at 5.0 A g −1 compared with that of 0.5 A g −1 . The PPDA-Nb 2 CT x //AC lithium ions hybrid capacitor (LIHC) delivers an excellent power density of 2754.8 W kg −1 at an energy density of 58.3 Wh kg −1 and a capacity retention with 80.0 % at 1.0 A g −1 after 1000 cycles. The interlayer engineering based on electrostatic intercalation provides a novel perspective to expand interlayer spacing, possessing a theoretical guidance for developing the Li + storage materials with high-rate capability. Graphical Make room for the ions : The approach that the interlayer engineering of electrostatic intercalation PPDA between Nb 2 CT x layers can enlarge interlayer spacing and facilitate fast Li + diffusion dynamics. The PPDA-Nb 2 CT x with 1.27 nm interlayer spacing not only offers the abundant transport highways to accelerate Li + diffusion, but also maintains the stability of layered structure due to the “support and dragline” effects of PPDA molecules. The method provides a novel perspective to design 2D materials with the high-rate capability for Li + storage.
Topological confinement and built-in electric field at F‑Nb2CTx/Nb2O5 heterointerfaces enable fast electron/ion kinetics for lithium-ion batteries
A topological confinement strategy is developed to construct atomically matched F-Nb 2 CT x /Nb 2 O 5 heterointerfaces. • The strongly coupled heterointerface enables 0.16068 |e| charge transfer and generates a built-in electric field. • The built-in electric field synergistically accelerates electron migration and Li + diffusion kinetics. • Excellent rate capability (257.7 mAh g −1 at 5.0 A g −1 ) and cycling stability (125.2% after 550 cycles) are achieved. • This work establishes a new heterointerface engineering paradigm for high-power, long-life lithium-ion battery anodes. Niobium pentoxide (Nb 2 O 5 ) is regarded as a promising anode material for lithium-ion batteries owing to its open-framework structure, competitive theoretical capacity, and intrinsic operational safety. However, its practical application is impeded by intrinsically low electronic conductivity and sluggish lithium-ion diffusion, leading to unsatisfactory rate capability and cycling stability. Herein, we propose a novel topological confinement strategy to construct atomically matched few-layer Nb 2 CT x /Nb 2 O 5 (F‑Nb 2 CT x /Nb 2 O 5 ) heterointerfaces for enhanced electron/ion kinetics. By leveraging the unique two-dimensional geometry of F‑Nb 2 CT x , a natural topological confinement space is established, inducing the in-situ derivation of well-ordered ultrafine Nb 2 O 5 nanocones with atomic-level lattice matching through the shared niobium element. This strongly coupled heterointerface enables electron transfer of 0.16068 |e| from F‑Nb 2 CT x to Nb 2 O 5 and establishes a built-in electric field, synergistically optimizing electron/ion transport kinetics. Benefiting from the strong interfacial coupling, the resulting electrode delivers a high reversible capacity of 430.0mAh g −1 at 0.2 A g −1 and maintains a remarkable rate capability of 257.7mAh g −1 even at 5.0 A g −1 . Moreover, it exhibits exceptional cycling stability with a capacity retention of 125.2% after 550 cycles at 1.0 A g −1 . This work establishes a new paradigm for overcoming the kinetic bottlenecks of oxide anodes through rational heterointerface engineering. A topological confinement strategy is developed to construct atomically matched few-layer Nb 2 CT x /Nb 2 O 5 (F-Nb 2 CT x /Nb 2 O 5 ) heterointerfaces. The unique two-dimensional geometry of F‑Nb 2 CT x provides a natural topological confinement space, directing the in-situ derivation of well-defined ultrafine Nb 2 O 5 nanocones with atomic-level lattice matching through the shared niobium element. This strongly coupled heterointerface enables electron transfer of 0.16068 |e| from F‑Nb 2 CT x to Nb 2 O 5 and establishes a built-in electric field, synergistically optimizing electron/ion transport kinetics. The resulting F‑Nb 2 CT x /Nb 2 O 5 heterostructured anode achieves an exceptional high-rate capacity of 257.7 mAh g −1 at 5.0 A g −1 and remarkable cycling stability, retaining 125.2% of its capacity after 550 cycles at 1.0 A g −1 . This work provides a new paradigm of heterointerface engineering to overcome the kinetic bottlenecks of oxide anodes for high-power, long-life lithium-ion batteries. Download: Download high-res image (207KB) Download: Download full-size image
Nb2CTx MXene boosting PEO polymer electrolyte for all-solid-state Li-S batteries: two birds with one stone strategy to enhance Li+ conductivity and polysulfide adsorptivity
All-solid-state lithium-sulfur (Li-S) battery is regarded as next-generation high energy density and safety battery system. The key challenge is to develop a compatible high-performance solid-state electrolyte. Herein, a two birds with one stone strategy is proposed to simultaneously enhance Li + conductivity and polysulfide adsorptivity of poly(ethylene oxide) (PEO)-based polymer electrolyte via the integration of Nb 2 CT x MXene. Moreover, the sheet size of Nb 2 CT x MXene is crucial for the enhancement of Li + conductivity and polysulfide adsorptivity, attributing to the difference in a specific surface area related to the percolation effect. By tuning the sheet size of Nb 2 CT x MXene from 500–300 nm to below 100 nm, the ionic conductivity of the PEO electrolyte is increased to 2.62 × 10 −4 S·cm −1 with improved Li + transference number of 0.37 at 60 °C. Furthermore, theoretical calculation and X-ray photoelectron spectroscopy (XPS) conjointly prove that polysulfides could be effectively adsorbed by Nb 2 CT x nanosheets via forming Nb−S bonding to inhibit their shuttle in the PEO framework. As a result, the all-solid-state Li-S cell exhibits an initial capacity of 1149 mAh·g −1 at 0.5C and good cycling stability with 491 mAh·g −1 after 200 cycles. The results demonstrate the necessity of polysulfide inhibition and the application of Nb 2 CT x MXene in PEO-based electrolytes for all-solid-state Li-S batteries. Graphic
Plasmonic sensor based on offset-splicing and waist-expanded taper using multicore fiber for detection of Aflatoxins B1 in critical sectors
In this work, authors have developed a portable, sensitive, and quick-response fiber optic sensor that is capable of detection of Aflatoxins B1 (AFB1) quantitatively and qualitatively. Using multi-mode fiber (MMF) and multi-core fiber (MCF), the MMF-MCF-MCF-MMF fiber structure based on symmetric transverse offset splicing and waist-expanded taper is fabricated. The evanescent waves are enhanced to form a strong evanescent field by etching the fiber surface with hydrofluoric acid. To successfully excite the localized surface plasmon resonance phenomenon, gold nanoparticles are deposited on the optical fiber probe's surface. Further, to modify the fiber optic probes, Niobium carbide (Nb2CTx) MXene and AFB1 antibodies are functionalized. Nb2CTx MXene is employed to strengthen the biocompatibility of the sensor and increase the specific surface area of the fiber probe, while AFB1 antibody is used to identify AFB1 micro-biomolecules in a specific manner. The reproducibility, reusability, stability, and selectivity of the proposed fiber probe are tested and validated using various concentration of AFB1 solutions. Finally, the linear range, sensitivity, and limit of detection of the sensing probe are determined as 0 - 1000 nM, 11.7 nm/µM, and 26.41 nM, respectively. The sensor offers an indispensable technique, low-cost solution and portability for AFB1-specific detection in agricultural products and their byproducts with its novel optical fiber structure and superior detecting capability. It is also useful for marine species like fish and consequently affecting health of human body.
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