Latest ArticlesPalladium-based alloy catalysts have been employed as one of the potential candidates for oxygen reduction reaction (ORR), but the dissolution of transition metal hinders their application. Herein, structure ordered PdTe intermetallic with Pd shell (o-PdTe@Pd) are synthesized via an electrochemical etching driven surface reconstruction strategy. The surface reconstruction could tune the electronic structure, weaken the adsorption energy of reaction intermediates on o-PdTe@Pd, resulting in enhanced electrocatalytic activity for ORR. The mass activity of o-PdTe@Pd is about 3.3 and 2.7 times higher than that of Pd/C in acid and alkaline, respectively. Besides, the half-potentials for ORR decay only about 44 mV and 12 mV after 30 k cycles accelerated durability test in acid and alkaline media, respectively. The enhanced durability originates from the resistance of Te atoms dissolve in the ordered PdTe intermetallic core and the core-shell structure. When assembled in a Zn-air battery, o-PdTe@Pd electrode delivers a higher specific capacity (794 mAh/g) and better cycling stability than Pt/C.
Radiotherapy (RT) is a crucial treatment for cancer; however, its effectiveness is limited by adverse effects on normal tissues, radioresistance, and tumor recurrence. To overcome these challenges, hydrogels have been employed for delivery of radiosensitizers and other therapeutic agents. This review summarizes recent advancements in the application of hydrogel-based local drug delivery systems for improving the therapeutic efficacy of RT in cancer treatment. Firstly, we introduce the classification and properties of hydrogels. Next, we detail hydrogel-based platforms designed to enhance both external beam radiation therapy and brachytherapy. We also discuss hydrogels used in combination therapy involving RT and immunotherapy. Lastly, we highlight the challenges that hydrogels face in RT. By surveying the latest developments in hydrogel applications for RT, this review aims to provide insights into the development of more effective and targeted cancer therapies.
Herein, a modified metal-free acetylene black (MMF-AB) catalyst was synthesized by a simple solvothermal-calcination method and designed successfully to activate peroxodisulfate (PDS) for the degradation of sulfisoxazole (SIZ). Due to the doping of N, S and O metal-free elements, the modified catalyst showed excellent catalytic performance with 100% SIZ removal within 30 min. Pseudo first-order reaction rate constants (evaluating catalytic efficiencies and activity) of MMF-AB (kobs = 0.105 min−1) was 3 times higher than pure-AB (kobs = 0.029 min−1). Interestingly, it was demonstrated that the reaction system is based on the transfer of electrons from SIZ to PDS to realize an electron-transfer-based mechanism by the evidence of premixing, electron paramagnetic resonance (EPR) spectroscopy, salt-bridge experiments and electrochemical analyses. The introduction of recyclable filtration device solved the secondary pollution caused by the dispersion of the powdered catalyst in the treated water, which further proved the practicality and superiority of the MMF-AB catalyst.
Facile and efficient method for constructing carbon dots (CDs) with narrow full width at half maximum (FWHM) is a major challenge in the field, and researches on regulating the FWHM of CDs are also rare and scarce. In this work, we delved into the synthesis of CDs with narrow fluorescence emission FWHM (NFEF-CDs) in the m-phenylenediamine (m-PD)/ethanol system, utilizing solid superacid resin as catalyst with solvothermal method. The resulting NFEF-CDs exhibit a photoluminescent (PL) emission peak at 521 nm with a narrow FWHM of 41 nm, an absolute PL quantum yield (QY) of 80%, and display excitation-independent PL behavior. Through comprehensive characterization, we identified the protonation of edge amino on NFEF-CDs as the key factor in achieving the narrow FWHM. Subsequently, we validated the broad applicability of solid superacid resins as catalysts for synthesizing CDs with narrow FWHM in the m-PD/ethanol system. Finally, we utilized a self-leveling method to prepare NFEF-CDs film on the surface of poly(methyl methacrylate) (PMMA) substrate and investigated the solid-state fluorescence properties of NFEF-CDs as well as their performance as luminescence solar concentrator (LSC) for photovoltaic conversion. The results revealed that the as-prepared LSC exhibit an internal quantum efficiency (ηint) of 42.39% and an optical efficiency (ηopt) of 0.68%. These findings demonstrate the promising prospects of NFEF-CDs in the field of LSCs and provide a theoretical basis for their application in photovoltaic conversion.
Organic thermoelectric (OTE) materials and devices have garnered significant attention in the past decade for flexible and wearable electronics. Due to the numerous combinations of different backbones, side chains, and functional groups for polymer molecules, further efficient developments of high performance OTEs rely on reverse and rational molecular design as well as fundamental understanding to the structure-property relationship, which both require precise theoretical input. Recently, many theoretical efforts and progresses have been made to predict TE properties and develop high performance OTE materials. Here, we present first the general methods and principles for OTE theoretical calculations. Subsequently, the latest theoretical advances regarding the effects of molecular design, chemical doping, ambipolar charge transport etc., to TE conversion are carefully reviewed. These theoretical advances not only significantly deepen the fundamental understanding of OTEs, but also provide precise guidance to the molecular design of OTE materials. Finally, we propose several perspectives for future theoretical investigations of OTEs.
In Fenton-like oxidation, the catalyst directly influences the reaction mechanism for the degradation of pollutants from water. Here, a α-MnO2 catalyst (OAm-1) was synthesized via a self-assembly method with the assistance of a surfactant. OAm-1 possessed a large specific surface area of 221 m2/g, abundant mesoporous structures and a large proportion of Mn(Ⅲ). Further characterization exhibited that OAm-1 had abundant oxygen vacancies and excellent reducibility and conductivity. The adsorption and catalytic ability of OAm-1 were studied in the degradation of oxytetracycline (OTC) via the activation of hydrogen peroxide (H2O2). Through the radical quenching experiments, electron resonance spectroscopy (EPR), X-ray photoelectron spectroscopy (XPS) and Fourier-transform infrared spectroscopy (FT-IR) analysis, Mn(Ⅲ) of OAm-1 was proved to be the active sites for the chemisorption of OTC. Systematic electrochemical experiments and analysis have shown that a process of electron transfer mediated by OAm-1 occurred between the pollutant and H2O2 during a Fenton-like reaction. This work experimentally verifies the electron transfer process dominated nonradical mechanism over α-MnO2, which is helpful for understanding the catalytic mechanism of the Fenton-like oxidation.
Flow-electrode capacitive deionization (FCDI) represents a promising approach for ion separation from aqueous solutions. However, the optimization of spacer, particularly for nitrate-contaminated groundwater systems, has often been overlooked. This research comprehensively investigates the influence of using a conductive (carbon cloth, CC) spacer on nitrate removal performance within FCDI system, comparing it to a non-conductive (nylon net, NN) spacer. In both CC and NN FCDI systems, it is unsurprisingly that nitrate removal efficiency improved notably with the increasing current density and hydraulic retention time (HRT). Interestingly, the specific energy consumption (SEC) for nitrate removal did not show obvious fluctuations when the current density and HRT varied in both systems. Under the auspiciously optimized process parameters, CC-FCDI attained a 20% superior nitrate removal efficiency relative to NN-FCDI, accompanied by a notably diminished SEC for CC-FCDI, registering at a mere 28% of NN-FCDI. This great improvement can be primarily attributed to the decrement in FCDI internal resistance after using conductive spacer, which further confirmed by electrochemical tests such as linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS). Upon prolonged continuous nitrate removal at the optimized conditions, the CC-FCDI system achieved a consistent 90% nitrate removal efficiency with a low SEC of 2.7–7.8 kWh/kg NO3-N, underscoring its steady performance. Overall, this study highlights the pivotal importance of careful spacer design and optimization in realizing energy-efficient groundwater treatment via FCDI.
The dynamic kinetic asymmetric transformation of racemic propargylic ammonium salts with prochiral aldimine esters through a stereodivergent propargylation is catalyzed by dual nickel and copper catalysis. Thus, a diverse range of optically active α-quaternary amino esters were produced via CN bond cleavage with high reaction efficiency and stereoselectivity (up to > 99% ee). By selection of the appropriate pairwise combination of catalyst configurational isomers, all four possible stereoisomers of the corresponding propargylation products are obtained in high yields with excellent regio-, diastereo-, and enantioselectivities.
Owing to the serious potential side-effects on the environment and human health, the rapid detection and removal of antibiotics have become an important research focus. In this work, four zinc-based metal-organic frameworks (MOFs) with different functional groups, i.e., Zn-MOF, Zn-MOF-CH3, Zn-MOF-NO2, Zn-MOF-COOH, were utilized for the construction of LDO/MOF composite materials with a nickel-iron-cobalt-based layered double oxide, NiFeCo-LDO. The results showed that the LDO/MOF composites not only had high sensitivity in detecting sulfonamide and quinolone antibiotics, but also had an appreciable ability to adsorb them from wastewater. The maximum adsorption capacities of all the four types of LDO@Zn-MOFs to all antibiotics can at least reach 150 mg/g, and the limits of detection in relation to all four antibiotics were at least as low as 100 µg/L. Our work suggested the dual-function extraction performance can be attributed to the synergistic effects between the LDO and the MOFs. Moreover, the strong ferromagnetism derived from the LDO provided great convenience for the separation and regeneration of the LDO/MOF composites.
Heterocycle-braced cyclic peptides have demonstrated enhanced metabolic stability, increased potency and selectivity. Here, we present a rapid synthesis method for constructing Trp(C7)-alkene(E)-crosslinked cyclic peptides with potent anti-proliferative activities against cancer cells, through C-H alkenylation and macrolactamization. This report addresses critical challenges associated with the installation and removal of the directing group N-Piv, configuration selectivity of the olefin, and intramolecular cyclization. Notably, this method exhibits mild reaction conditions, traceless removal of the directing group, and high configuration selectivity.
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