Latest ArticlesChronic kidney disease (CKD) is a progressive disease characterized by high rates of morbidity and mortality, often leading to various complications. Early home diagnosis and point-of-care prognosis are therefore crucial for monitoring CKD progression and managing patient outcomes. β2-microglobulin (B2M) levels offer a valuable indicator of renal function changes, however, their quantitative detection typically relies on sophisticated and costly laboratory instrumentation. Here, we present a universal and adaptable strategy for efficiently conjugating rare-earth-based nanoparticles with antibodies via a carboxymethyl β-cyclodextrin-mediated "self-assembly-followed-by-conjugation" approach. Cyclodextrin modification enhances the rigidity, hydrophilicity, and electrostatic repulsion of nanoparticles, significantly improving their colloidal stability and upconversion luminescence in aqueous solution. Moreover, the ample carboxyl groups on cyclodextrin offer multiple sites for covalent conjugation, resulting in a substantial enhancement in antibody loading capacity and improved immunoaffinity for biomarkers. Employing this methodology, we developed an antibody-conjugated nanoprobe for B2M and fabricated a fluorescent lateral flow strip. Subsequently, image acquisition and data analysis using a smartphone enabled sensitive and quantitative detection of B2M in artificial urine, achieving a detection limit of 2.7 ng/mL. This study provides a versatile strategy for the development of nanoparticle-based colorimetric/luminescent immunoassay probes.
Traditional enzyme-nanozymes cascade assays for glucose detection are usually limited by pH incompatibility and operational complexity. Herein, we present a strategy based on hollow mesoporous Prussian blue (HMPB) nanozymes for one-step, dual-modal glucose sensing under neutral conditions. The rationally designed HMPB nanozymes exhibit intrinsic peroxidase-like activity at physiological pH (~7.4), inherent chromogenic properties and superior photothermal conversion efficiency. These features directly enable integration with glucose oxidase (GOx) for one-step glucose detection without intermediate pH adjustment. Additionally, the catalytic coupling of 4-aminoantipyrine/phenol oxidation products, enhanced by the intrinsic blue coloration of HMPB, generates vivid multicolorimetric responses for smartphone-based quantitative analysis. To enhance signal reliability, the photothermal properties of HMPB nanozymes are further ingeniously coupled with the thermal-responsive characteristics of oxidized 3,3′,5,5′-tetramethylbenzidine (oxTMB), establishing a dual-amplified thermal imaging platform through portable infrared thermal imager detection. HMPB nanozymes serve as both a catalytic activator and an intrinsic signal reporter, establish a new platform in dual-modal glucose monitoring. The platform demonstrates remarkable clinical adaptability through its smartphone-compatible colorimetric readout and portable thermal imaging capabilities, achieving a detection limit of 1.39 µmol/L (multicolorimetric modal) and 3.05 µmol/L (photothermometric modal) for glucose with robust reliability in human serum samples. This research overcomes the pH mismatch barrier in enzyme-nanozymes cascade system, and providing a cost-effective, instrument-flexible detection strategy that bridges laboratory research and point-of-care diagnostics.
Multi-substituted azetidines have been an under-utilized bioisosteres in modern drug entities, due to the scarcity of mild and stereo-controllable synthetic methods. The state-of-art aza-[2 + 2] cycloaddition suffers from two drawbacks, namely limited C=N scope and the dearth of stereochemical control. Herein, we extend a photocatalytic direct N-heteroarene dearomative aza-[2 + 2] cycloaddition under white light via energy transfer mechanism. A key protonic solvent triggered retro aza-[2 + 2] cycloaddition process was discovered and utilized as a stereochemical editing logic to address the challenge of diastereomeric control (controlling three contiguous stereocenters).
Multiple myeloma (MM) is a highly aggressive hematologic malignancy characterized by abnormal proliferation of malignant plasma cells. CD38, a transmembrane glycoprotein, is highly expressed on the surface of plasma cells and serves as a critical diagnostic and therapeutic target for MM. However, the masking of CD38 epitopes caused by therapeutic interventions often leads to false-negative results in clinical detection of CD38, compromising diagnostic accuracy and underscoring the urgent need for novel specific molecular tools. Herein, we reported a novel aptamer, CD38jd4a, specifically targeting CD38 with potential clinical applications. A series of high-affinity aptamers specifically binding CD38 were selected and identified through a highly efficient aptamer selection method with CD38 as the target. Among them, aptamer CD38jd4a exhibited the best performance, with a dissociation constant (Kd) value as low as 5.4 ± 0.6 nmol/L. Through siRNA-mediated knockdown experiments, CD38jd4a was further validated to specifically recognize native CD38 expressed on surface of cells. Furthermore, binding epitopes of CD38jd4a were confirmed to be distinct from those recognized by any of current therapeutic antibodies. This unique characteristic enabled the simultaneous application of CD38jd4a with therapeutic antibodies for CD38 detection on CD38-positive Ramos cells by flow cytometry without cross-interference. Importantly, clinical blood sample analysis revealed that CD38jd4a was capable of effectively detecting CD38 despite epitope masking, thereby overcoming limitations of conventional antibody-based detection methods. Given the small molecular size and excellent performance, CD38jd4a is expected to be a robust diagnostic tool for CD38 detection, offering a promising alternative for clinical diagnostics of CD38.
According to the "New Coronavirus Pneumonia (COVID-19) Tenth Edition Diagnosis and Treatment Plan", residues from three prescriptions including Qingfei-Paidu Formula, Huashi-Baidu Formula, and Xuanfei-Zhixue Formula were selected as precursors for biochar preparation. The resulting Chinese medicine residue-derived biochars (CMR-BCs), prepared using different prescriptions and pyrolysis temperatures, were used to activate peracetic acid (PAA) for sulfamethoxazole (SMX) removal. Biochar (q800) produced from 800 ℃-treated Qingfei-Paidu Formula residue achieved ~60% SMX adsorption removal efficiency, outperforming other CMR-BCs. All prepared CMR-BC samples demonstrated oxidative degradation of SMX via activating PAA, with efficiencies ranging from ~20.8% to 45.5%, which might be ascribed to their abundant oxygen-containing functional groups and graphitic structures. Electro-chemical analysis and quenching tests indicated that the direct electron-transfer (DET) process was identified as the primary non-radical degradation mechanism. The formation of CMR-BCs-PAA* interfacial complexes enhanced the overall oxidation potential, facilitating the redox reaction between CMR-BCs-PAA* and SMX. In total, this study offers new insights into the non-radical mechanism of CMR-BC/PAA systems, presenting a potential solution for the resource utilization of Chinese medicine residue wastes.
To deal with the problem of NO3− enrichment in water environment, electrochemical catalysis of nitrate reduction reaction (NO3RR) provides a possibility. However, this catalytic process requires efficient and highly selective NO3RR electrocatalysts to catalyze NO3− conversion. Consequently, the objective of this work is to search highly active NO3RR electrocatalysts by employing an efficient screening strategy using density functional theory methods. The catalytic activity is assessed by calculating limiting potential UL(NO3RR) and UL(HER). The research results indicate that Os2_C19N3 not only has excellent catalytic activity (UL(NO3RR) = −0.15 V), but also can effectively avoid the occurrence of competitive hydrogen evolution reaction. The NO3RR process of Os2_C19N3 is * + NO3− → *NO3 → *NO3H → NO2 → *NO2H → *NO → *NOH → *N → *NH → *NH2 → *NH3 → * + NH3. When Os2_C19N3 is in the condition of DFT-Sol, DFT-D, and DFT-D-Sol, the NO3RR process is * + NO3− → *NO3 → *NO3H → NO2 → *NO2H → *NO → *NOH → *NHOH → *NH2OH → *NH2 → *NH3 → * + NH3, and the UL(NO3RR) values are −0.06, −0.15, and −0.06 V, respectively. This research may offer potential reference values for the development of innovative NO3RR catalysts and the synthesis of NH3.
Quenching experiments play an essential role in the probing of reactive oxygen species (ROS) in advanced oxidation processes (AOPs). However, inappropriate choice of quencher type and concentration will affect the judgement of the contribution of ROS. Herein, we systematically explored the direct reaction of quenchers with oxidants commonly used in AOPs (e.g., hydrogen peroxide (H2O2), peroxymonosulfate (PMS), and peroxydisulfate (PDS)). The experimental results showed that PMS had a noticeable reaction with methyl phenyl sulfoxide, dimethyl sulfoxide and furfuryl alcohol, and the second-order reaction rate constants between them were measured. Meanwhile, PDS and H2O2 were hardly consumed in the presence of various quenchers. Moreover, high-performance liquid chromatography measurements demonstrated that L-histidine, benzoquinone, and phenol would have the artifact of rapid PMS depletion due to the limitations of the test method. Furthermore, in response to the problems with the quenching experiments, some suggestions for the selection of quencher type and concentration were presented. This work is of great reference value in guiding the appropriate selection of quenchers in AOPs, which in turn facilitates the accurate investigation of ROS and reaction mechanisms.
Antibiotic contamination in aquatic environments poses serious risks to ecosystems and public health, necessitating the development of effective removal technologies. In this study, a novel biochar-supported ferric oxyhydroxide (FeOOH/BC) composite catalyst was developed for the activation of peracetic acid (PAA) to degrade cefapirin (CFP), a widely used and persistent cephalosporin antibiotic. The catalyst featured highly dispersed FeOOH nanoparticles and enhanced interfacial electron transfer, enabling efficient activation of PAA through dual pathways involving both radical and non-radical species. FeOOH/BC-1 exhibited the highest catalytic activity, where high-valent iron, singlet oxygen, and surface-bound reactive species played the primary roles in CFP degradation. Fe(Ⅲ) active sites generate high-valent iron oxo, while N active sites in biochar accounted for the direct electron transfer. This work provides a new approach for activating PAA in the degradation of emerging contaminants and offers a feasible method for catalyst regeneration in wastewater treatment applications.
Microplastics (MPs), which originate from plastic degradation, are becoming a significant environmental pollutant, and their prevalence is increasing rapidly. Humans can ingest MPs through various pathways and their presence has been detected in multiple human organs, raising concerns about the potential toxic effects associated with plastic consumption. Epigenetic modifications of nucleic acids play crucial roles in various biological processes, including gene expression and tumorigenesis. Previous studies have demonstrated that exposure to certain environmental pollutants can influence disease pathogenesis by affecting epigenetic factors, including modifications of nucleic acids. However, the impact of MPs on epigenetic modifications of nucleic acids remains largely unexplored. In this study, we systematically investigated the alterations in epigenetic modifications of DNA and RNA following exposure to polystyrene microplastics (PS-MPs). We utilized liquid chromatography-tandem mass spectrometry (LC-MS/MS) to simultaneously analyze two DNA epigenetic modifications of 5-methylcytosine (5mC) and 5-hydroxymethylcytosine (5hmC), along with twenty RNA epigenetic modifications from small RNA and nine epigenetic modifications from mRNA. We measured changes in the levels of DNA and RNA modifications across six tissues (heart, liver, spleen, lung, kidney, and intestine) in mice after PS-MPs exposure. The results indicated that exposure to PS-MPs significantly altered the landscape of epigenetic modifications in nucleic acids. Furthermore, we observed tissue-specific effects, suggesting that different organs respond uniquely to PS-MPs exposure. Additionally, the correlation patterns between DNA and RNA modifications changed following PS-MPs exposure. These findings provide valuable insights suggesting that PS-MPs exposure may alter the patterns of epigenetic modifications in nucleic acids, potentially leading to adverse health effects.
Nanomedicine preparation is a promising approach for the effective utilization of natural bioactive products. However, the successful fortification of natural products into nanocarriers in a host-guest manner remains a great challenge. Here, a 96-WP TFH/TM strategy integrating 96-well plate mediated thin-film hydration, turbidity measurement, stability evaluation, and relative quantification, was proposed to screen host-guest complexes. As a proof-of-concept, biomimetic bile acid-lecithin nanomicelles (BA-L NMs) were used as nanocarriers and 51 natural products were assayed for guest molecules. Muscone came out as the fit-for-purpose candidate to produce stable NMs, namely M-NMs. Following spectroscopic characterization and molecular dynamics calculation, hydrophobic interactions, hydrogen bonding, and salt bridges were demonstrated as the primary correlations amongst taurocholic acid, lecithin, and muscone. M-NMs exhibited significant in vitro and in vivo anti-inflammation features. Together, we developed a 96-WP TFH/TM strategy to achieve high-throughput host-guest complex screening, facilitating the development of natural product nanomicelles.
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