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New Near-Infrared Fluorescence Imaging Platform with Large Stokes Shift for Carboxylesterase 2 Detection in Thyroid Cancer and Inflammatory Diseases Diagnosis
No full textDevelopment of new near-infrared fluorophores is one of the eternal themes in the field of biosensing and biological imaging. In this work, we constructed a novel fluorophore platform MOR by replacing methylindole of hemicyanine fluorophore (CyR) with benzoxazole to acquire better fluorescence characteristics. Based on the platform, a near infrared (NIR) fluorescent probe MOR-CES2 was synthesized for the specific "off-on" response to carboxylesterase 2 (CES2). The probe exhibited excellent properties including near-infrared emission (735 nm), large Stokes shift (105 nm), high sensitivity (LOD, 0.3 ng/mL), and rapid response (15 min). The successful application of MOR-CES2 in biological imaging of CES2 in mice with thyroid cancer and inflammatory bowel disease demonstrated that the probe could identify cancer cells and tissues and sensitively respond to inflammation. The results proved the potency of MOR-CES2 as an efficient imaging tool to assist in the surgical resection of CES2-related tumors
Metal-Organic Framework-Based Composites for the Adsorption Removal of Per- and Polyfluoroalkyl Substances from Water
No full textThe increasing health risks posed by per- and polyfluoroalkyl substances (PFASs) in the environment highlight the importance of implementing effective removal techniques. Conventional wastewater treatment processes are inadequate for removing persistent organic pollutants. Recent studies have increasingly demonstrated that metal-organic frameworks (MOFs) are capable of removing PFASs from water through adsorption techniques. However, there is still constructive discussion on the potential of MOFs in adsorbing and removing PFASs for large-scale engineering applications. This review systematically investigates the use of MOFs as adsorbents for the removal of PFAS in water treatment. This primarily involved a comprehensive analysis of existing literature to understand the adsorption mechanisms of MOFs and to identify factors that enhance their efficiency in removing PFASs. We also explore the critical aspects of regeneration and stability of MOFs, assessing their reusability and long-term performance, which are essential for large-scale water treatment applications. Finally, our study highlights the challenges of removing PFASs using MOFs. Especially, the efficient removal of short-chain PFASs with hydrophilicity is a major challenge, while medium- to long-chain PFASs are frequently susceptible to being captured from water by MOFs through multiple synergistic effects. The ion-exchange force may be the key to solving this difficulty, but its susceptibility to ion interference in water needs to be addressed in practical applications. We hope that this review can provide valuable insights into the effective removal and adsorption mechanisms of PFASs as well as advance the sustainable utilization of MOFs in the field of water treatment, thereby presenting a novel perspective
Effect of Hydrophobic Chain Length in Amphiphilic Chitosan Conjugates on Intracellular Drug Delivery and Smart Drug Release of Redox-Responsive Micelle
No full textThree redox-sensitive nanocarriers were rationally designed based on amphiphilic low molecular weight chitosan-cystamine-octylamine/dodecylamin/cetylamine (LC-Cys-OA, LC-Cys-DA, LC-Cys-CA) conjugates containing disulfide linkage for maximizing therapeutic effect by regulating hydrophobic interaction. The resultant spherical micelles had the characteristics of low CMC, suitable size, excellent biosafety and desired stability. The drug-loaded micelles were fabricated by embedding doxorubicin (Dox) into the hydrophobic cores. The effect of hydrophobic chain lengths of amphiphilic conjugates on encapsulation capacity, redox sensitivity, trigger-release behavior, cellular uptake efficacy, antitumor effect and antimigratory activity of Dox-loaded micelles was systematically investigated. Studies found that Dox-loaded LC-Cys-CA micelle had superior loading capacity and enhanced redox sensitivity compared with the other two micelles. Release assay indicated that the three Dox-loaded micelles maintained sufficiently stability in normal blood circulation but rapidly disintegrated in tumor cells. More importantly, the LC-Cys-CA micelle with a longer hydrophobic chain length exhibited a higher accumulative Dox release percentage than the other two micelles. Additionally, an increase in hydrophobic chain lengths of amphiphilic conjugates improved cellular uptake efficiency, antitumor effect and antimigration activity of Dox-loaded micelles, which could be explained by enhanced loading ability and redox sensitivity. Our research was expected to provide a viable platform for achieving a desired therapeutic efficacy via the alteration of hydrophobic interaction
The Sources and Atmospheric Processes of Strong Light-Absorbing Components in Water Soluble Brown Carbon: Insights From a Multi-Proxy Study of PM<sub>2.5</sub> in 10 Chinese Cities
No full textHumic-like substances (HULIS) are significant contributor to the light absorption of water-soluble brown carbon (WSBrC), which contains certain strong light-absorbing chemical components that are not well understood, impeding the assessment of WSBrC's climate impact. China as the hotspot regions with high loading of WSBrC characterized by high light-absorbing capacity, here, we investigated the sources and atmospheric processes (delta C-13-Delta C-14), molecular composition (Fourier transform ion cyclotron resonance mass spectrometry), and light absorption properties (UV spectrophotometry) of HULIS in PM2.5 from 10 Chinese cities. HULIS-C was major contributor to the light absorption coefficient (70.5 +/- 6.6%) of WSBrC at 365 nm, which was more enriched with fossil sources (48.0 +/- 9.0% vs. 30.3 +/- 13.9%) but depleted in C-13 (delta C-13: -25.6 +/- 0.9 parts per thousand vs. -22.4 +/- 1.0 parts per thousand) relative to non-HULIS-C. This suggests that the fossil components in HULIS are more recalcitrant to oxidative aging and exhibit higher light-absorbing capacity, while the non-fossil organic carbon is more likely to be oxidatively bleached into small, colorless, and highly polar molecules (i.e., non-HULIS). Aromatic components are the major strong light-absorbing fossil components in HULIS, dominantly originating from coal combustion (>77%). Non-negative matrix factorization model showed that aromatic molecules from coal combustion have higher molecular weight and lower oxidation levels than biomass burning, potentially making them to be photo-recalcitrant compounds. Our finding that coal combustion-derived BrC maybe more persistent in the atmosphere and has greater long-term impact on climate than BrC derived from biomass burning is an important consideration in climate models and mitigation policies
NIR-activatable nitric oxide generator based on nanoparticles loaded small-molecule photosensitizers for synergetic photodynamic/gas therapy
No full textBackgroundTherapeutic approaches that combine conventional photodynamic therapy (PDT) with gas therapy (GT) to sensitize PDT are an attractive strategy, but the molecular structure design of the complex lacks effective guiding strategies.ResultsHerein, we have developed a nanoplatforms Cy-NMNO@SiO2 based on mesoporous silica materials loaded NIR-activatable small-molecule fluorescent probe Cy-NMNO for the synergistic treatment of photodynamic therapy/gas therapy (PDT/GT) in antibacterial and skin cancer. The theoretical calculation results showed that the low dissociation of N-NO in Cy-NMNO enabled it to dissociate effectively under NIR light irradiation, which is conducive to produce Cy and NO. Cy showed better 1O2 generation performance than Cy-NMNO. The cytotoxicity of Cy-NMNO obtained via the synergistic effect of GT and PDT synergistically enhances the effect of photodynamic therapy, thus achieving more effective tumor treatment and sterilization than conventional PDT. Moreover, the nanoplatforms Cy-NMNO@SiO2 realized efficient drug loading and drug delivery.ConclusionsThis work not only offers a promising approach for PDT-GT synergistic drug delivery system, but also provides a valuable reference for the design of its drug molecules
Structural framework for the understanding spectroscopic and functional signatures of the cyanobacterial Orange Carotenoid Protein families
No full textThe Orange Carotenoid Protein (OCP) is a unique photoreceptor crucial for cyanobacterial photoprotection. Best studied Synechocystis sp. PCC 6803 OCP belongs to the large OCP1 family. Downregulated by the Fluorescence Recovery Protein (FRP) in low-light, high-light-activated OCP1 binds to the phycobilisomes and performs non -photochemical quenching. Recently discovered families OCP2 and OCP3 remain structurally and functionally underexplored, and no systematic comparative studies have ever been conducted. Here we present two first crystal structures of OCP2 from morphoecophysiologically different cyanobacteria and provide their comprehensive structural, spectroscopic and functional comparison with OCP1, the recently described OCP3 and all-OCP ancestor. Structures enable correlation of spectroscopic signatures with the effective number of hydrogen and discovered here chalcogen bonds anchoring the ketocarotenoid in OCP, as well as with the rotation of the echinenone's beta-ionone ring in the CTD. Structural data also helped rationalize the observed differences in OCP/ FRP and OCP/phycobilisome functional interactions. These data are expected to foster OCP research and applications in optogenetics, targeted carotenoid delivery and cyanobacterial biomass engineering
Aging in soil increases the disturbance of microplastics to the gut microbiota of soil fauna
No full textMicroplastics (MPs) in the soil environment inevitably experience aging processes. However, how aging in soil affects MP toxicity to soil fauna remains poorly understood. In this study, two types of widely distributed MPs (polypropylene and tire wear particles) were aged in different soils, and their surface properties, morphology, leaching features of additives, biofilm colonization and toxicity to the typical soil fauna Enchytraeus crypticus were investigated. Results showed that aging in soil slightly changed the surface properties and morphology for both types of MPs, but significantly affected the release of additives, especially for those MPs aged in soil amended with manure. Moreover, a distinct and less diverse microbial community than the surrounding soils was formed on the surface of MPs, and MP type was a determinant of the biofilm microbial community. Exposure experiments indicated that aged MPs, especially those aged in soil with manure significantly affected the reproduction of soil worms with a more obvious disturbance to their gut microbiota, and biofilm features and changes in the leaching properties of MPs during aging were the main factors for these shifts. This study is the first attempt to reveal the role of aging in soil in MP toxicity to soil fauna
Comparative investigations on the metabolomic responses to cadmium in clams<i> Ruditapes</i><i> philippinarum</i> from the Bohai Sea and South China Sea
No full textCadmium (Cd) is a typical heavy metal contaminant along China coasts. Clams Ruditapes philippinarum are widely distributed in multiple climatic zones. However, few research has been conducted on the different responses to Cd in clams from different climatic zones. In this study, the temperate zone Bohai Sea (BS) and tropical zone South China Sea (SCS) clams exhibited distinct background metabolome profiles, characterized by different strategies of osmotic regulation, energy metabolism, and anaerobiosis tendencies, suggesting different tolerance and enrichment capacities to Cd. After Cd treatments, the BS clams demonstrated quicker and higher accumulations of Cd than the SCS clams. Despite differences in their background metabolomes, both BS and SCS clams displayed similar metabolomic responses to Cd, such as anaerobiosis inhibition and increased energy demands. Overall, these findings suggested that the inconsistency of biological responses induced by geographic conditions should be considered in ecotoxicological studies. Capsule abstract: This study elucidated the biological differences in clams Ruditapes philippinarum from the Bohai Sea and South China Sea, and the metabolomic responses in these two clam populations after Cd (200 mu g/L) treatments
Preparation and Properties of Crosslinked Quaternized Chitosan-Based Hydrogel Films Ionically Bonded with Acetylsalicylic Acid for Biomedical Materials
No full textThe aim of the current study is to develop chitosan-based biomaterials which can sustainably release acetylsalicylic acid while presenting significant biological activity. Herein, an innovative ionic bonding strategy between hydroxypropyl trimethyl ammonium chloride chitosan (HACC) and acetylsalicylic acid (AA) was proposed, skillfully utilizing the electrostatic attraction of the ionic bond to achieve the controlled release of drugs. Based on this point, six crosslinked N-[(2-hydroxy-3-trimethylammonium)propyl]chitosan acetylsalicylic acid salt (CHACAA) hydrogel films with varying acetylsalicylic acid contents were prepared by a crosslinking reaction. The results of 1H nuclear magnetic resonance spectroscopy (1H NMR) and scanning electron morphology (SEM) confirmed the crosslinked structure, while the obtained hydrogel films possessed favorable thermal stability, mechanical properties, and swelling ability. In addition, the drug release behavior of the hydrogel films was also investigated. As expected, the prepared hydrogel films demonstrated the capability for the sustainable release of acetylsalicylic acid due to ion pair attraction dynamics. Furthermore, the bioactivities of CHACAA-3 and CHACAA-4 hydrogel films with acetylsalicylic acid molar equivalents of 1.25 and 1.5 times those of HACC were particularly pronounced, which not only exhibited an excellent drug sustained-release ability and antibacterial effect, but also had a higher potential for binding and scavenging inflammatory factors, including NO and TNF-alpha. These findings suggest that CHACAA-3 and CHACAA-4 hydrogel films hold great potential for applications in wound dressing, tissue engineering scaffolds, and drug carriers
Dissolved N pollution and its biogeochemical constraints along a river-sea continuum of a typical dense oyster mariculture coastal water, northwest South China Sea
No full textDissolved nutrients, including nitrate (NO-3-N) and its dual isotopes (615N-NO- 3 and 618O-NO-3) were systematically studied along a river-sea continuum, wherein dense oyster mariculture is implemented, to constrain the pollution sources and biogeochemical cycling mechanisms of nitrogen (N). Total dissolved N, mainly composed of inorganic N, showed strong anthropogenic influence. Based on MixSIAR model results, N pollution was predominantly sourced from sewage/wastewater (55.9-64.3 %). Nutrient stoichiometry revealed DIP and DSi stress, and surface water in the riverine region was severely eutrophic. The occurrences of eutrophication and changes in nutrient stoichiometry were significantly related to N pollution sources in both summer and winter. N dynamics were controlled by anthropogenic activities and physical mixing. However, due to the insignificance of biological processes such as denitrification, phytoplankton assimilation, N2 fixation, and nitrification, including the lack of significant isotopic fractionation associated with these processes, and the poor fit of both the Rayleigh Model and Open system Model to the measured data, it is speculated that the several-fold reduction in N load and eutrophication along the river-sea continuum could be attributed to a combination of significant N removal by dense oyster mariculture and nutrient dilution due to physical mixing of river and seawater during winter and summer