Latest ArticlesChemodynamic therapy (CDT) based on nanozyme has received much attention for safe and effective cancer treatment. However, the catalytic ability of nanozyme and insufficient intracellular H2O2 levels severely limit their therapeutic effect. To overcome these limitations, we construct tumor microenvironment-responsive hybrid cascade systems, where single-atom Cu nanozymes (CuNC SANs) with high peroxidase (POD)-like activity were synthesized to immobilize glucose oxidase (GOx). To enhance their biological performance and stability, polyethylene glycol (DSPE-PEG-NH2) is further modified. After endocytosis into tumor cells, the immobilized GOx of cascade systems reacts with intracellular glucose to produce H2O2 in situ. The H2O2 with elevated concentration can be further catalyzed by CuNC SANs and increase ROS yield after cascade reaction, thus amplifying the effect of CDT. In addition, the consumption of glucose cuts off the energy supply of the tumor, realizing starvation therapy. Significantly, the photothermal properties of CuNC SANs not only accelerate the cascade reaction but also enable photothermal therapy (PTT) for cancer treatment. This study proposes a promising PTT/CDT/starvation triple therapy strategy for high-efficiency cancer therapy.
The melt-transesterification polycondensation method necessitates elevated reaction temperatures and protracted reaction times in the copolymerization of modified isosorbide-based polycarbonates. This results in a decline in molecular weight and color degradation of the copolymerized IS-PC. In this paper, the process of polyethylene glycol (PEG) modification was introduced in the synthesis of isosorbide-based copolycarbonate (PEXHDCYC) by means of a melt chain extension method. As demonstrated by experimental findings, this method has the capacity to reduce the reaction temperature and shorten the reaction time. Additionally, it has been observed to enhance the molecular weight and overall properties of the material. Through the optimization of reaction conditions, a series of PEXHDCYC with weight average molecular weight (Mw) ranging from 19,004 g/mol to 73,294 g/mol were synthesized. The results demonstrated that the glass transition temperature (Tg) of PEXHDCYC decreased in conjunction with an increase in the PEG1000 content. It is noteworthy that the PEXHDCYC synthesized by this method exhibits an exceptional elongation at break, reaching up to 135.45% ± 24%. Furthermore, PEXHDCYC demonstrates superior optical properties in comparison to bisphenol A polycarbonate (BPA-PC).
The electrocatalytic reduction of carbon dioxide (CO2) into fuels holds significant promise for addressing energy and environmental challenges, albeit hindered by constraints in conversion efficiency, production rates, and electrode stability. Metal diborides are considered as promising electrocatalysts that may demonstrate superior CO2 electroreduction performance due to their distinctive electronic properties. Herein, a series of novel bulk metal diborides, encompassing transition metals from group IVB to group VIIB elements, were fabricated using a high pressure-high temperature technique, which were directly utilized as self-supporting electrodes for electrocatalytic reduction of CO2. The zirconium diboride (ZrB2) electrode stood out in metal diborides with superior electrocatalytic activity in generating carbon monoxide (CO), achieving a Faradaic efficiency of 92.2% at −2.2 V vs. Ag/Ag+ in ionic liquid-based electrolytes. Impressively, the ZrB2 electrode demonstrated stable catalysis of CO2 reduction to CO over a nearly 60-h electrolysis period. Furthermore, the ZrB2 electrode and ionic liquid-based electrolytes could synergistically catalyze the reduction of CO2 to CO. Experimental results and density functional theory calculations support the notion that exposed metal sites on the ZrB2 (001) surface could enhance *CO desorption and restrain the hydrogen evolution reaction, thereby facilitating the conversion of CO2 into CO.
Hydroxyethyl starch 130/0.4 (HES130/0.4) is a macromolecular polysaccharide with polydispersity, which is widely used as a plasma expander. Full-profile bioanalysis of HES130/0.4 is required to characterize its plasma pharmacokinetics, yet current analytical technologies struggle with this task due to its complex structure and composition. To address this existing lacuna within the realm of analytical science, we propose a liquid chromatography-electrospray ionization mass spectrometry (LC-ESI-MS) methodology for the full-profile bioanalysis of HES130/0.4. Amide column separation with gradient optimization eluted polydisperse HES130/0.4 as a single symmetric peak. In-source collision-induced dissociation (IS-CID) converted the numerous precursor ions of HES130/0.4 into a limited number of characteristic fragment ions, from which m/z 597.4 was selected as the "pseudo-precursor ion" for MRM quantification. The ion transition m/z 597.4 → 435.3 was identified as the quantitative ion pair. The method demonstrated a linear calibration curve from 40 µg/mL to 4000 µg/mL, with accuracy and precision meeting acceptance criteria, confirming its reliability and reproducibility. Subsequently, the workflow was successfully applied to investigate the pharmacokinetics of HES130/0.4 in rat, revealing its large distribution volume and rapid elimination within 24 h. This work provides a straightforward approach for the full-profile quantification of HES130/0.4 in biological samples, overcoming the limitations of traditional methods in terms of poor specificity, low sensitivity and narrow linear range, and providing a reference for the in vivo full-profile bioanalysis of HES130/0.4 and other polysaccharides.
Foodborne bacterial infection is a serious threat to food safety, especially live pathogens causing outbreaks of most diseases. Thus developing live bacterial detection methods is important for public health. In this study, a microfluidic biosensor was developed for rapid detection of live Salmonella typhimurium, in which immune magnetic particle chains in microchannels were used to separate and enrich target bacteria, antibody-conjugated gold nanorods (GNRs) were applied for photothermal lysis of target live bacteria under near-infrared (NIR) irradiation, and a photon-counting detector was used for measuring adenosine triphosphate (ATP) bioluminescence in the presence of firefly luciferin/luciferase. This biosensor was proved to be able to quantitatively detect S. typhimurium from 5.0 × 102 CFU/mL to 5.0 × 106 CFU/mL in 60 min (magnetic separation 20 min; GNRs combination 20 min; NIR irradiation, 8 min) with limit of detection (LOD) of 495 CFU/mL. This biosensor showed an excellent specificity in the coexistence of other foodborne bacteria, and target bacteria were successfully measured even in the matrix interference of milk sample with mean recovery of 121.17%. This biosensor might be a promising tool for on-site assessment foodborne bacteria.
E. coli O157:H7 and Staphylococcus aureus have emerged as significant foodborne pathogens, characterized by considerable incidence rates and mortality. Despite advancements, current detection methods are hindered by challenges in enhancing specificity and sensitivity. Herein, we introduced a cutting-edge biosensor that employs a novel CHA-coupled CRISPR multi-stage signal amplification technique for the rapid and ultra-sensitive detection of these two pathogens. This microfluidic device consisted of an upstream serpentine mixing channel and a downstream boat-shaped microcavity equipped with a micro-column array, facilitating efficient reagent mixing, robust CHA amplification, and CRISPR reactions. Multiple signal amplification was achieved through bacterial competitive binding triggered by catalytic hairpin assembly (CHA) and crRNA-mediated CRISPR reactions. Based on this platform, the detection of target bacteria is transformed into nucleic acid detection, with a maximum detection range of 134 CFU/mL for E. coli O157:H7 and 181 CFU/mL for Staphylococcus aureus, which were better or comparable to previously reported biosensors. The entire assay was completed within approximately 1.5 h, with a minimal sample volume requirement of just 10 µL. The biosensor exhibited a high recovery rate, ranging from 95% to 115%, and demonstrated excellent specificity towards the target bacteria. In summary, this biosensor offers a rapid, accurate, and highly sensitive tool for food safety and clinical diagnostics.
Dielectric barrier discharge (DBD) plasma combined with Fe2+ for periodate (PI) activation was proposed for emerging contaminants treatment. The feasible, activation mechanism, degradation mechanism were comprehensively analyzed. Results showed that within 6 min treatment time, the degradation efficiency of sulfadiazine (SDZ) could reach 68.1%, 78.5% and 90.2% in DBD, DBD/PI and DBD/PI/Fe2+, respectively. The energy efficiency can also be improved from 47.24 mg/kWh (DBD) to 78.43 mg/kWh (DBD/PI/Fe2+). Compared with DBD system, the PI activation energy barrier in DBD/Fe2+ system is significantly decreased. Electron spin resonance (ESR) proved the existence of •OH, 1O2 and •O2− in DBD/PI/Fe2+ system, and the corresponding intensity are higher than that of DBD/PI system. The quenching experiments shown that •OH, 1O2, •O2− and electron play important role for SDZ degradation. Reactive species dominant to SDZ degradation was explored by LC–MS and density functional theory (DFT) analysis. Higher input power, acid condition and higher conductivity were favorable to SDZ degradation. DBD/PI/Fe2+ system has good effect in treating other emerging contaminants and obtains good environmental adaptability.
NH4V4O10 has attracted significant attention as a cathode material for aqueous zinc-ion batteries (AZIBs) due to its adjustable interlayer spacing (~9.5 Å) and high theoretical specific capacity (~400 mAh/g). However, its development is hindered by sluggish Zn2+ kinetics and structural instability. In this work, a glycine (Gly) intercalation strategy is demonstrated, which establishes three stabilization mechanisms in the Gly-NVO cathode: (1) Gly pillars are shown to expand the interlayer spacing to 1.21 nm; (2) Hydrogen-bonding networks are formed between layers; (3) Reversible NH4+ (de)intercalation behavior is observed. The Gly-NVO cathode delivers a capacity of 520 mAh/g at 0.2 A/g (393 Wh/kg energy density), along with outstanding rate capability (400 and 150 mAh/g at 10 and 50 A/g, corresponding to power densities of 5688 and 24.3 kW/kg, respectively). A capacity retention of 88.2% is maintained after 10,000 cycles at 50 A/g. DFT calculations confirm that the introduction of Gly significantly enhances the electrical conductivity of NVO while effectively weakening electrostatic interactions, and energy barrier for Zn2+ intercalation and vanadium dissolution are reduced by Gly. Additionally, due to the reversible NH4+ (de)intercalation behavior in Gly-NVO, the assembled aqueous ammonium-ion batteries (AAIBs) exhibit stable cycling ability. This work highlights organic molecule pre-intercalation as a viable strategy for optimizing the durability of ammonium vanadate cathodes.
Materials with blue-shifted and enhanced emission exhibit extensive applications in information encryption, solar ultraviolet sensing and ink-free printing, however, preparing blue-shifted and enhanced emission from photo-responsive material remains a significant challenge. Herein, we designed and synthesized successfully the photo-responsive ionic-bonded organic crystals (IOC) using tetraphenylethylene (TPE)-based multidentate imidazolium salt and sulfonic acid. Impressively, the discernible response of IOC to UV light is evidenced by a blue shift and an enhancement in dilute solution. Specifically, this has resulted in a significant increase in the absolute quantum yield, from 7.0% to 41.3%. This remarkable efficiency can be attributed to the cooperative effect that reduces non-radiative processes, the restriction of intermolecular motions (RIM) and the modulation of charge transfer (CT) behavior. This work first reports blue-shifted and enhanced emission from ionic crystal, providing a new strategy to achieve photochromic materials.
Iron-based metal oxide catalysts are widely used for selective catalytic reduction (SCR) of NOx with NH3 due to their excellent catalytic performance at medium and high temperatures, high nitrogen selectivity, robust resistance to sulfur dioxide poisoning, environmental sustainability and cost effectiveness. However, several challenges including sub-optimal low-temperature catalytic activity, narrow operating temperature range, poor resistance to alkali/alkaline earth metal poisoning, as well as insufficient thermal stability and H2O/SO2 resistance always hinder the further application of iron-based metal oxide catalysts, which is in urgent need of further improvement in practical applications. This review provides a comprehensive overview of the development, applications and challenges associated with different types of iron-based metal oxide catalysts and suggests corresponding modification strategies to address the as-mentioned issues. Iron oxide catalysts can promote low-temperature catalytic performance by adjusting crystal structures and exposing specific crystal faces; however, their thermal stability and resistance to SO2/H2O and alkali metals still have substantial room for improvement. Iron-based composite metal oxide catalysts can effectively increase the resistance to SO2/H2O by coupling multiple metals and modulating adjacent electronic sites. Iron-based acidic salt catalysts greatly enhance the resistance to alkali metal poisoning by enriching the surface acid sites and providing sacrificial sites. Supported iron-based metal oxide catalysts can significantly improve both catalytic performance and resistance by modulating reaction pathways and constructing core-shell structures. This review clarifies the important direction of further research on iron-based metal oxide catalysts, and provides scientific basis and design ideas for the development and application of high-efficiency low-temperature NOx reduction catalysts.
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