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The mechanism of enhanced photocatalytic indole cation-radical cyclization in confined space is examined by coupling a nanopipette reactor with in situ nano-electrospray mass spectrometry (nanoESI-MS).

Synergism of oxygen–iodine binary vacancies to interfacial electric field was developed by a cascade electrospray-annealing preparation, which enhanced CO2 photoreduction over VO–I-BiOCl/BiOI atomic-thin nanosheets.

DNA nanoframeworks, with great biological information and controlled framework structures, exhibit great potentials in biological applications. Their applications are normally limited by unstable structures susceptible to hydrolysis, depurination, depyrimidination, oxidation, alkylation, or nuclease degradations. Herein, to ensure the mechanical and chemical stabilities of DNA nanoframeworks for intracellular applications, biomineralization of multifunctional DNA nanoframeworks with a tetrahedral skeleton is employed. Via silicification, the S-S bond is simultaneously introduced to obtain the silica-armored DNA nanoframeworks (Si-DNA nanoframeworks), mechanically and chemically stabilized for efficient intracellular deliveries. This successfully prevents degradations and leakages of reagents loaded on Si-DNA nanoframeworks, including biomolecular siRNA and small DOX drugs. Furthermore, the nucleic acid strands of the nanoframeworks are labeled with FAM and the quencher, facilitating miRNA detection upon "turn-on" signals from hybridizations. Therefore, the nanoframeworks collapse via double responses of the silica coating (silica acidic dissolution and S-S reduction by GSH) in cancer cells, realizing on-demand reagent release for miRNA detection and synergistic treatments (by siRNA and DOX). Demonstrated by both in vivo and in vitro experiments, the biomineralization has stabilized DNA nanomaterials for biological applications.

Lung cancer is a heterogeneous disease with a severe disease burden. Because the prognosis of patients with lung cancer varies, it is critical to identify effective biomarkers for prognosis prediction.A total of 2325 lung cancer patients were integrated into four independent sets (training set, validation set I, II and III) after removing batch effects in our study. We applied the microarray data algorithm to screen the differentially expressed genes in the training set. The most robust markers for prognosis were identified using the LASSO-Cox regression model, which was then used to create a Cox model and nomogram.Through LASSO and multivariate Cox regression analysis, eight genes were identified as prognosis-associated hub genes, followed by the creation of prognosis-associated risk scores (PRS). The results of the Kaplan-Meier analysis in the three validation sets demonstrate the good predictive performance of PRS, with hazard ratios of 2.38 (95% confidence interval (CI), 1.61-3.53) in the validation set I, 1.35 (95% CI, 1.06-1.71) in the validation set II, and 2.71 (95% CI, 1.77-4.18) in the validation set III. Additionally, the PRS demonstrated superior survival prediction in subgroups by age, gender, p-stage, and histologic type (In this study, we developed a PRS signature to help predict the survival of lung cancer. By combining it with clinical risk factors, a nomogram was established to quantify the individual risk assessments.

Due to their special physicochemical properties, organic-inorganic hybrid perovskite quantum dots (OIP QDs) are ideal and potential catalysts for the nitrogen reduction reaction (NRR). However, the OIP QD-based NRR is limited by poor water resistance, competitive suppression by the hydrogen evolution reaction, and inefficient active sites on the catalyst surfaces. Herein, to ensure an efficient NRR in aqueous solution, a water-resistant polycarbonate-part-encapsulated heterojunction of Zn,Pt

Developments in framework nucleic acids (FNAs) are limited by complicated synthesis, by-product interference, and low framework utilization. Herein, simple core–shell spherical 3D FNAs (ST-SFNAs) preparation is presented based on siRNA-templated linear polymerization followed by hybridization chain reaction branched polymerization. Without by-products, all components exhibited their special functions to obtain high space utilization of ST-SFNAs. ST-SFNAs were covered by catalase and folic acid-functionalized liposome membranes. The catalase endowed ST-SFNAs with chemotactic activities in the H2O2 reaction catalyzed by catalase. Furthermore, combined with functionalized folic acids' targeting folate receptors, the synergistic chemotactic recognition of cancer cells was obtained. This dramatically promoted targeted cellular uptakes compared with traditional active or passive targeting pathways. Subsequently, the cascaded-logical programmable release of drugs was precisely controlled by targeting glutathione and ATP (via S–S bond and ATP aptamer on the inner g-DNA cover). This was visualized by “turn on” fluorescent signals generated by special hybridization of released hairpin DNAs with survivin mRNA biomarkers. Simultaneously, biocompatible synergistic therapy was achieved by simultaneously releasing doxorubicin and siRNA. With its high utilization for synergistic chemotactic recognition, programmable and visualized delivery, as well as synergistic therapy, an efficient platform for maximizing the therapeutic efficacy has been developed. This would initiate further FNA-based material development for a variety of biological applications., ST-SFNAs were developed by siRNA-templated linear-branched polymerizations with high space utilizations for loadings, which obtained synergistic cancer therapy via chemotactic recognition, visualized delivery, and cascaded-logical controlled release.

The rapid degradation of organic pollutants, process monitoring and online controlling to obtain advanced products and decreased by-products are great and challenging tasks in environmental treatments. Herein, an accelerated plasma degradation in milliseconds was achieved by combining electrospray-based acceleration and plasma-based degradation. Taking the degradation of chloroaniline as an example, 97% of the degradation can be achieved in milliseconds. The velocity distribution of droplets was determined to be 40–50 m/s after being degraded for 0.30 ms, which exhibited different degradation behaviors in different milliseconds. Simultaneously, by virtue of the real-time and on-line detection ability of ambient mass spectrometry, intermediates, by-products and advanced products were monitored. Therefore, degradation mechanisms for different degradation times were proposed, which would provide theoretical guidance on obtaining efficient and green degradation. The fabrication, examining and understanding of accelerated plasma degradation not only enlarged application of accelerated reactions, but also promoted green and efficient degradation for environmental treatments.

Near-infrared (NIR) fluorescent probe has exhibited unique advantages for

Compared with traditional visible light-driven fluorescence visualization (FV), near-infrared (NIR)-induced FV is an interesting and promising method, while photoelectrochemical (PEC) immunoassay sensing possesses the advantages of high sensitivity, low cost, and simple instrumentation. We combined PEC sensing with NIR-induced FV together and developed a dual readout sensing platform. In this protocol, based on the antibody-analyte (i.e., antigen, DNA, and RNA) reaction and the sandwich-type structure, CuInS2 microflowers as the matrix provided the original background photocurrent; chlorin e6 (Ce6) was conjugated to antibody-modified upconversion nanoparticles and formed a signal label for the PEC sensing and naked-eye readout. Different from traditional PEC immunosensors, under NIR illumination, the developed dual mode sensing platform could achieve quick qualitative analysis and quantitative analysis. Preliminary application performance of the proposed biosensor in prostate-specific antigen analysis is acceptable, indicating its promising potential in clinical/biological studies.

Online mass spectrometry was applied to reveal multiple mechanisms of visible-light irradiated dye-sensitized photocatalysis for o-phenylenediamine oxidation. The reactants, products and short-lived intermediates were recorded and dynamically tracked. Dimer and unexpected trimer intermediates were observed to deduce the stepwise aerobic photooxidation mechanism with multiple routes, which was supported by theoretical calculations.

In this work, we constructed a target-triggered and controlled-release plasmon-enhanced fluorescent AIE probe to realize the purpose of conformational monitoring of insulin fibrillation. We synthesized a novel water-soluble anthracene derivative, 4,4',4'',4'''-(anthracene-9,10-diylbis(ethene-2,1,1-triyl))tetrakis(N,N,N-trimethylbenzenaminium) iodide (BDVAI), with AIE properties, high biocompatibility and good self-assembly effect. Gold nanocages (AuNCs) were selected as the substrate for PEF, and the inner space of hollow AuNCs was filled with BDVAI. Thiol-modified DNA chains were bonded to the surface of AuNCs by Au-S bonds, and an insulin aptamer was combined with the sulfhydryl chain to seal the AuNCs. This PEF-AIE sensor produces different fluorescence signals when interacting with native insulin and fibrillar insulin; thus, monitoring conformational changes in insulin can be realized by detecting fluorescence intensity changes during insulin fibrillation. Based on this design, this system realized sensitive detection of fibrillar insulin with a detection limit of 23.6 pM. This AIE molecular-based PEF fluorescence enhancement system improves the optical properties of fluorescent substances, which is of great significance in improving the detection sensitivity of amyloid fibrils conformational changes and providing a reliable basis for further understanding the pathogenesis of amyloidosis.

The TEMPO-electrocatalyzed acceptorless dehydrogenation of tetrahydroquinoline, a transformation in green synthesis and hydrogen storage, has been investigated by coupling of an electrocatalytic system with in situ extraction electrospray ionization mass spectrometry. Dynamic changes in important species and intermediates were monitored, which evoked an updated AD understanding.

The solvent content strongly affects viscoelastic properties and network structure of hydrogels. While due to the gels’ structural susceptibility and autofluorescence background, there is still no ...