Publications by authors named "Jinxia Liu"

116 Publications

Removal of Zwitterionic PFAS by MXenes: Comparisons with Anionic, Nonionic, and PFAS-Specific Resins.

Environ Sci Technol 2022 May 9;56(10):6212-6222. Epub 2022 May 9.

Department of Chemical and Biological Engineering, University of British Columbia, Vancouver, British Columbia V6T 1Z3, Canada.

Zwitterionic per- and polyfluoroalkyl substances are increasingly detected in aquatic environments. The magnitude of their concentration and increased frequency of detection worldwide raise questions on their presence in drinking water and associated health risk. Scientific knowledge on the identification of treatment technologies to effectively capture such zwitterionic PFAS from contaminated water sources remains largely unknown. In this study, we investigated the application of anionic organic scavenger ion exchange (IX) resins (A860), nonionic IX resins (XAD 4 and XAD 7), PFAS-specific resins (A694 and A592), and TiC MXenes (novel two-dimensional metal carbides) for the removal of select fluorotelomer zwitterionic PFAS from natural waters. The cumulative removal of zwitterionic PFAS at pH ∼ 7 follows the order: TiC MXenes > A694 > A592 > A860 > XAD 4 ∼ XAD 7. TiC MXenes were able to capture >75% of the total influent zwitterionic PFAS and the performance remained consistent in natural and synthetic water. TiC MXenes also exhibited efficient regeneration (>90% recovery) with 0.4 M NaSO solution, while the regeneration efficacy of other IX resins generally remained below 20%. Treatment with ∼180 J/cm UV dosage in the 0.4 M NaSO regenerant brine solution yielded >99.9% reduction in the zwitterionic PFAS concentration indicating that UV-sulfite systems exhibit promising potential for the treatment of zwitterionic PFAS concentrates.
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http://dx.doi.org/10.1021/acs.est.1c03780DOI Listing
May 2022

Bifunctional Pdots-Based Novel ECL Nanoprobe with Qualitative and Quantitative Dual Signal Amplification Characteristics for Trace Cytokine Analysis.

Anal Chem 2022 May 2;94(19):7115-7122. Epub 2022 May 2.

School of Public Health, Nantong University, Nantong, 226019, P. R. China.

In this work, a novel methodology to design bifunctional ECL-luminophores with self-enhanced and TSA-amplified characteristics was proposed for improving the sensing performance of ECL-immunosensor toward trace cytokine analysis. Thanks to the qualitative- and quantitative- dual signal amplification technique, the as-prepared ECL biosensor demonstrated excellent detection performance. By analyzing the prospective cytokine biomarkers (IL-6), the ECL immunosensor exhibited a broad examination range with quite low detection limit and quite high selectivity, which was far superior to commercial ELISA kits and ever reported works. In particular, the novel ECL nanoprobe developed here could also be applied to monitor other immune toxicities or disease-related cytokines by using the respective antibodies corresponding to these targets. Moreover, the concept and construction strategy of self-amplified ECL-luminophores presented here could be further extended to design a series of Pdots-derived multicolored ECL probes to meet the needs of multipathway detection applications.
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http://dx.doi.org/10.1021/acs.analchem.2c01041DOI Listing
May 2022

Combination therapy based on targeted nano drug co-delivery systems for liver fibrosis treatment: a review.

J Drug Target 2022 Feb 24:1-12. Epub 2022 Feb 24.

Department of Pharmaceutics, School of Pharmacy, Ningxia Medical University, Yinchuan, China.

Liver fibrosis is the hallmark of liver disease and occurs prior to the stages of cirrhosis and hepatocellular carcinoma. Any type of liver damage or inflammation can result in fibrosis. Fibrosis does not develop overnight, but rather as a result of the long-term action of injury factors. At present, however, there are no good treatment methods or specific drugs other than removing the pathogenic factors. Drug application is still limited, which means that drugs with good performance cannot achieve good therapeutic effects , owing to various factors such as poor drug targeting, large side effects and strong hydrophobicity. Hepatic stellate cells (HSCs) are the primary effector cells in liver fibrosis. The nano-drug delivery system is a new and safe drug delivery system that has many advantages which are widely used in the field of liver fibrosis. Drug resistance and side effects can be reduced when two or more drugs are used in combination drug delivery. Combination therapy of drugs with different targets has emerged as a novel approach to treating liver fibrosis, and the nano co-delivery system enhances the benefits of combination therapy. While nano co-delivery systems can maximise benefits while avoiding drug side effects, this is precisely the advantage of the nano co-delivery system. This review briefly described the pathogenesis and current treatment strategies, the different co-delivery systems of combination drugs in the nano delivery system, and targeting strategies for nano delivery systems on liver fibrosis therapy. Due to their superior performance, nano delivery systems and targeting drug delivery systems have received a lot of attention in the new drug delivery system. The new delivery systems offer a new pathway in the treatment of liver fibrosis, and it is believed that it can be a new treatment for fibrosis in the future. Nano co-delivery system of combination drugs and targeting strategies has proven the effectiveness of anti-fibrosis at the experimental level.
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http://dx.doi.org/10.1080/1061186X.2022.2044485DOI Listing
February 2022

Microbial biotransformation of aqueous film-forming foam derived polyfluoroalkyl substances.

Sci Total Environ 2022 Jun 8;824:153711. Epub 2022 Feb 8.

Department of Civil and Environmental Engineering, Colorado School of Mines, Golden, CO, USA. Electronic address:

Per- and polyfluoroalkyl substances (PFASs) used in aqueous film-forming foam (AFFF) comprise some perfluoroalkyl substances but a larger variety of polyfluoroalkyl substances. Despite their abundance in AFFF, information is lacking on the potential transformation of these polyfluoroalkyl substances. Due to the biological and chemical stability of the repeating perfluoroalkyl -(CF)- moiety common to all known AFFF-derived PFASs, it is not immediately evident whether the microbial biotransformation mechanisms observed for other organic contaminants also govern the microbial biotransformation of polyfluoroalkyl substances. Herein, we aim to: 1) review the literature on the aerobic or anaerobic microbial biotransformation of AFFF-derived polyfluoroalkyl substances in environmental media; 2) compile and summarize proposed microbial biotransformation pathways for major classes of polyfluoroalkyl substances; 3) identify the dominant biotransformation intermediates and terminal biotransformation products; and 4) discuss these findings in the context of environmental monitoring and source allocation. This analysis revealed that much more is currently known about aerobic microbial biotransformation of polyfluoroalkyl substances, as compared to anaerobic biotransformation. Further, there are some similarities in microbial biotransformations of fluorotelomer and electrochemical fluorination-derived polyfluoroalkyl substances, but differences may be largely due to head group composition. Dealkylation, oxidation, and hydrolytic reactions appear to be particularly important for microbial biotransformation of AFFF-derived polyfluoroalkyl substances, and these biotransformations may lead to formation of some semi-stable intermediates. Finally, this review discusses key knowledge gaps and opportunities for further research.
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http://dx.doi.org/10.1016/j.scitotenv.2022.153711DOI Listing
June 2022

A highly sensitive electrochemical cytosensor based on a triple signal amplification strategy using both nanozyme and DNAzyme.

J Mater Chem B 2022 02 2;10(5):700-706. Epub 2022 Feb 2.

School of Public Health, Nantong University, Nantong 226019, P. R. China.

The development of a sensitive cytosensor is beneficial for the early diagnosis and treatment of cancer. Herein, highly sensitive cytosensing was achieved by applying triple signal amplification strategies with [email protected] nanozymes and DNAzyme hybrids as electrochemical nanoprobes and toluidine blue (Tb) as the electron transfer medium. The [email protected] nanocomposites not only acted as nanozymes with excellent catalytic performance towards HO reduction but also served as promising scaffolds to carry massive electroactive substances and DNA probes. The dual-functional DNA probes were designed with the sequence of hemin/G-quadruplex to serve as the DNAzyme and the sequence of aptamer to recognize cancer cells. Furthermore, Tb was also conjugated to the surface of the [email protected] nanohybrids, working as the electron transport medium to magnify the electrochemical response. With the above design, the [email protected] nanozymes and hemin/G-quadruplex DNAzyme efficiently co-catalyzed the reduction of HO to accelerate the electron transfer of Tb, which realized triple signal amplification and finally improved the performance of the electrochemical cytosensor. The proposed cytosensor achieved a sensitive detection of HepG2 cells with a low detection limit of 20 cells mL, and could be potentially used as an effective analysis tool in early cancer diagnosis in the future.
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http://dx.doi.org/10.1039/d1tb02545gDOI Listing
February 2022

pH-Dominated Selective Imaging of Lipid Droplets and Mitochondria via a Polarity-Reversible Ratiometric Fluorescent Probe.

Anal Chem 2022 02 6;94(6):2901-2911. Epub 2022 Jan 6.

School of Public Health, Nantong University, Nantong 226019, P. R. China.

Elucidating the intrinsic relationship between mitochondrial pH (pH) fluctuation and lipid droplets (LDs) formation is vital in cell physiology. The development of small-molecular fluorescent probes for discrimination and simultaneous visualization of pH fluctuation toward LDs has not yet been reported. In this work, utilizing pH-driven polarity-reversible hemicyanine and rhodamine derivatives, a multifunctional fluorescent probe is developed for selectively identifying mitochondria and LDs under specific pH values via dual-emission channels. This rapid-response probe, Hcy-Rh, has two distinct chemical structures under acidic and alkaline circumstances. In acidic conditions, Hcy-Rh exhibits good hydrophilicity that can target mitochondria and display an intense red fluorescence. Conversely, the probe becomes lipophilic under weakly alkaline conditions and targets LDs, showing a strong blue emission. In this manner, Hcy-Rh can selectively label mitochondria and LDs, exhibiting red and blue fluorescence, respectively. Moreover, this ratiometric probe is applied to map pH changes in living cells under the stimulus with FCCP, NAC, and HO. The interplay of LD-mitochondria under oleic acid treatment and starvation-induced autophagy has been studied using this probe at different pH values. In a word, Hcy-Rh is a potential candidate for further exploring mitochondria-LD interaction mechanisms under pH fluctuation. Moreover, the polarity-dependent strategy is valuable for designing other functional biological probes in imaging multiple organelles.
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http://dx.doi.org/10.1021/acs.analchem.1c04806DOI Listing
February 2022

Per- and Polyfluoroalkyl Substances in Contaminated Soil and Groundwater at Airports: A Canadian Case Study.

Environ Sci Technol 2022 01 30;56(2):885-895. Epub 2021 Dec 30.

Department of Civil Engineering, McGill University, Montreal, Québec H3A 0C3, Canada.

The occurrence of 93 classes of per- and polyfluoroalkyl substances (PFASs) was investigated at aqueous film-forming foam (AFFF)-impacted sites of four Canadian airports. Surface/subsurface soil and groundwater samples were characterized using high-resolution mass spectrometry (HRMS) and an improved total oxidizable precursor (TOP) assay. PFAS profiles, loads, and spatial trends were highly site-specific, influenced by the AFFF use history, variations in sorption, transport, and transformation potential of PFASs. All sites have been impacted by more than one AFFF chemistry, with the active firefighter training area exhibiting a greater PFAS variety and total PFAS burden than decommissioned sites. Zwitterionic and cationic compounds composed a large percentage (34.5-85.5%) of the total PFAS mass in most surface soil samples in the source zone but a relatively low percentage (<20%) in groundwater samples. Background soils surrounding the source zone contained predominantly unidentified precursors attributed to atmospheric deposition, while in AFFF-impacted soils, precursors originating from AFFFs can be largely captured by HRMS using available suspect lists. Horizontal transfer of PFASs in surface soils was limited, but vertical migration down the soil column occurred even in locations of low permeability. This study provides a critical data set to support developing new priority analyte lists and integrating TOP assay for comprehensive PFAS monitoring at AFFF-impacted sites.
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http://dx.doi.org/10.1021/acs.est.1c04798DOI Listing
January 2022

Density Functional Theory Calculations Decipher Complex Reaction Pathways of 6:2 Fluorotelomer Sulfonate to Perfluoroalkyl Carboxylates Initiated by Hydroxyl Radical.

Environ Sci Technol 2021 12 9;55(24):16655-16664. Epub 2021 Dec 9.

Center for Green Chemistry and Catalysis, Department of Chemistry, McGill University, Montreal, Quebec H3A 0B8, Canada.

6:2 Fluorotelomer sulfonate (6:2 FTSA) is a ubiquitous environmental contaminant belonging to the family of per- and polyfluoroalkyl substances. Previous studies showed that hydroxyl radical (OH) efficiently transforms 6:2 FTSA into perfluoroalkyl carboxylates (PFCAs) of different chain lengths (C2-C7), yet the reaction mechanisms were not elucidated. This study used density functional theory (DFT) calculations to map the entire reaction path of 6:2 FTSA initiated by OH and experimentally verified the theoretical results. Optimal reaction pathways were obtained by comparing the rate constants calculated from the transition-state theory. We found that 6:2 FTSA was first transformed to C7 PFCA and CF; CF was then further reacted to C2-C6 PFCAs. The parallel addition of OH and O to CF was essential to producing C2-C6 PFCAs. The critical step is the generation of alkoxyl radicals, which withdraw electrons from the adjacent C-C groups to result in chain cleavage. The validity of the calculated optimal reaction pathways was further confirmed by the consistency with our experimental data in the aspects of O involvement, identified intermediates, and the final PFCA profile. This study provides valuable insight into the transformation of polyfluoroalkyl substances containing aliphatic carbons in OH-based oxidation processes.
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http://dx.doi.org/10.1021/acs.est.1c05549DOI Listing
December 2021

Novel and legacy per- and polyfluoroalkyl substances (PFAS) in freshwater sporting fish from background and firefighting foam impacted ecosystems in Eastern Canada.

Sci Total Environ 2022 Apr 8;816:151563. Epub 2021 Nov 8.

Department of Chemistry, Université de Montréal (UdeM), Montréal, QC H3C 3J7, Canada. Electronic address:

Emerging PFAS were recently reported at sites impacted by aqueous film-forming foams (AFFFs) and near major manufacturing centers; however, few studies have evaluated whether these can occur far from release sites. Here, newly identified PFAS were investigated in wild sporting fish from boreal freshwater ecosystems (background sites, 2013-2014 summer seasons), compared to fish impacted by a major AFFF release (summer 2013 and autumn 2014). Different freshwater wild sporting fish species (Esox lucius, Esox masquinongy, Micropterus dolomieu, Sander vitreus, Perca flavescens, and Semotilus corporalis, n = 74) were collected from 13 ecosystems (lakes, reservoirs, and rivers) across Eastern Canada. Of 29 quantitative PFAS, 15 compounds were detected in fish from background sites, including perfluorocarboxylates (C), perfluoroalkane sulfonates (C), perfluorooctane sulfonamide (FOSA), 6:2 fluorotelomer sulfonate (6:2 FTSA), 7:3 fluorotelomer carboxylic acid (7:3 FTCA), and a zwitterionic PFAS-perfluorooctane sulfonamidoalkyl betaine (PFOSB). To our knowledge, this is the first report of PFOSB in biota. It is also one of the first reports of anionic fluorotelomers (6:2 FTSA, 7:3 FTCA, 9:3 FTCA) in wildlife from background sites. Long-chain fluorotelomer sulfonamidoalkyl betaines (e.g., 8:2 and 10:2 FTAB), fluorotelomer betaines (e.g., 9:3 and 9:1:2 FTB), and fluorotelomer sulfone propanoic acids (e.g., 8:2 FT(SO)-PA, 10:2 FT(SO)-PA)) were solely prevalent (up to 97% of summed suspect PFAS) in Smallmouth Bass (M. dolomieu) from the AFFF-impacted site. Perfluorobutane sulfonamide (FBSA), perfluorohexane sulfonamide (FHxSA), 6:2 FTSA and 7:3 FTCA were detected in at least one Smallmouth Bass sample both at the AFFF-impacted and background sites. According to the estimated chronic daily intake and current tolerable daily intake suggested by national agencies, the observed PFOS levels would not pose a health risk to anglers who might consume these wild-caught fish.
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http://dx.doi.org/10.1016/j.scitotenv.2021.151563DOI Listing
April 2022

Enhancing Interface Reactions by Introducing Microbubbles into a Plasma Treatment Process for Efficient Decomposition of PFOA.

Environ Sci Technol 2021 12 9;55(23):16067-16077. Epub 2021 Nov 9.

College of Environmental Science and Engineering, Donghua University, 2999 North Renmin Road, Shanghai 201620, China.

Efficient destruction of perfluoroalkyl compounds in contaminated waters remains a challenge because of highly stable C-F bonds. In this study, mineralization of perfluorooctanoic acid (PFOA) with high concentration (∼30 mg/L) was realized in a needle-plate pulsed discharge reactor integrated with a water jet (NPDW) to which microbubbles (MBs) with different carrier gases (air, N, and Ar) were introduced to enhance interfacial reactions. MBs effectively enrich dispersed PFOA from a bulk solution to a liquid surface to allow enhancing contact with reactive species and also expanding the plasma discharge area and channels. The PFOA removal efficiency in air and Ar discharge reached 81.5 and 95.3% in 2 h, respectively, with a defluorination ratio of no less than 50%. Energy requirements (EE/O) ranged from 216.49 to 331.95 kWh/m. Aside from fluoride, PFOA was degraded to a range of short-chain perfluoroalkyl acids and, to a minor extent, at least 20 other fluorinated transformation products. PFOA degradation mechanisms were proposed, including decarboxylation, hydroxylation, hydrogenation reduction, and defluorination reactions. Real water matrices (groundwater, tap water, wastewater effluent, and surface water) showed moderate impact on treatment outcomes, demonstrating the robustness of the treatment process. The study demonstrated an environmentally friendly nonthermal plasma technology for effective PFOA degradation.
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http://dx.doi.org/10.1021/acs.est.1c01724DOI Listing
December 2021

Target and Nontarget Screening of PFAS in Biosolids, Composts, and Other Organic Waste Products for Land Application in France.

Environ Sci Technol 2022 May 20;56(10):6056-6068. Epub 2021 Oct 20.

Département de Chimie, Université de Montréal, Montréal, Quebec H2 V 0B3, Canada.

Zwitterionic, cationic, and anionic per- and polyfluoroalkyl substances (PFAS) are increasingly reported in terrestrial and aquatic environments, but their inputs to agricultural lands are not fully understood. Here, we characterized PFAS in 47 organic waste products (OWP) applied in agricultural fields of France, including historical and recent materials. Overall, 160 PFAS from 42 classes were detected from target screening and homologue-based nontarget screening. Target PFAS were low in agriculture-derived wastes such as pig slurry, poultry manure, or dairy cattle manure (median ∑PFAS: 0.66 μg/kg dry matter). Higher PFAS levels were reported in urban and industrial wastes, paper mill sludge, sewage sludge, or residual household waste composts (median ∑PFAS: 220 μg/kg). Historical municipal biosolids and composts (1976-1998) were dominated by perfluorooctanesulfonate (PFOS), -ethyl perfluorooctanesulfonamido acetic acid (EtFOSAA), and cationic and zwitterionic electrochemical fluorination precursors to PFOS. Contemporaneous urban OWP (2009-2017) were rather dominated by zwitterionic fluorotelomers, which represented on average 55% of ∑PFAS (max: 97%). The fluorotelomer sulfonamidopropyl betaines (X:2 FTSA-PrB, median: 110 μg/kg, max: 1300 μg/kg) were the emerging class with the highest occurrence and prevalence in contemporary urban OWP. They were also detected as early as 1985. The study informs for the first time that urban sludges and composts can be a significant repository of zwitterionic and cationic PFAS.
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http://dx.doi.org/10.1021/acs.est.1c03697DOI Listing
May 2022

Assessing the risk from trace organic contaminants released via greywater irrigation to the aquatic environment.

Water Res 2021 Oct 15;205:117664. Epub 2021 Sep 15.

Department of Civil Engineering, McGill University, Montreal, Quebec, H3A 0C3, Canada. Electronic address:

Onsite non-potable reuse of greywater reduces the energy costs associated with the transport of wastewater and the stress on traditional source waters. However, greywater contains trace organic contaminants (TOrCs) that can be harmful to the aquatic environment when released via irrigation. In this work, the risk associated with TOrCs was evaluated for two potential irrigation scenarios, the use of untreated greywater and the use of greywater treated via conventional activated sludge. Risk quotient (RQ) ratios were calculated using the maximum concentration of each compound in the untreated or treated greywater divided by the relevant aquatic predicted no effect concentration. The TOrCs with RQs > 0.1 or 1 were classified as moderate and high priority, respectively. A review of greywater literature showed that a total of 350 compounds have been detected, with 132 classified as moderate or high priority in untreated greywater. Post-treatment 44 TOrCs remained as high priority due to high concentrations in greywater and/or poor removal during treatment, but only 14 of them were detected in multiple geographic locations. The final list of 14 TOrCs includes plasticizers/flame retardants (di-(2-ethylhexyl) phthalate, bisphenol A, and triphenyl phosphate), surfactants/preservatives/fragrances (4-nonylphenol, benzyldimethyl dodecylammonium chloride, tonalide, methylparaben, and 2-6-di-tert-butyl-4-methylphenol), UV-filters (benzophenone-3 and octocrylene), and pharmaceuticals/antibiotics (acetaminophen, trimethoprim, caffeine, and triclosan). This subset of TOrCs would be useful surrogates to monitor during greywater treatment for irrigation as potential hazards for nearby aquatic environments.
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http://dx.doi.org/10.1016/j.watres.2021.117664DOI Listing
October 2021

MiR-940 Serves as a Diagnostic Biomarker in Patients with Sepsis and Regulates Sepsis-Induced Inflammation and Myocardial Dysfunction.

J Inflamm Res 2021 9;14:4567-4574. Epub 2021 Sep 9.

Department of Critical Care Medicine, Yidu Central Hospital of Weifang, Weifang, Shandong, 262500, People's Republic of China.

Introduction: Sepsis is a heterogeneous syndrome with a life-long threat caused by infection. This study aimed to investigate the clinical function of miR-940 and its influence on cardiomyocyte models.

Methods: The relative expression of miR-940 was assessed by qRT-PCR and the roles in the clinical diagnosis of miR-940 were revealed by the ROC curve. The relationship between miR-940 and clinical parameters was validated by Pearson analysis. The sepsis rat models were established by treatment with cecal ligation and perforation (CLP) and clinical items including left ventricular systolic pressure (LVSP), left ventricular and end-diastolic pressure (LVEDP), maximum rate of increase/decrease in left ventricular blood pressure (± dp/dt) as well as troponin (cTnl), creatine kinase isoenzyme (CK-MB), TNF-α, IL-1β, and IL-6 were detected.

Results: The finding of qRT-PCR accentuated that the relative expression of miR-940 was significantly decreased in sepsis patients and CLP-stimulated models. The ROC curve proposed that miR-940 could be a satisfactory diagnostic biomarker for sepsis patients. Pearson analysis reinforced the expression of miR-940 was negatively associated with the PCT, WBC, CRP, Scr, SOFA score, and APACHE II score. The outcome of CLP-steered rat verified that overexpression of miR-940 inhibited the detrimental effects of CLP on myocardial dysfunction and inflammation reactions.

Conclusion: The downregulation of miR-940 was reported and it might be an underlying diagnostic marker in sepsis patients. Overexpression of miR-940 protected myocardial function from damage and inflammation induced by CLP.
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http://dx.doi.org/10.2147/JIR.S316169DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8437419PMC
September 2021

Immunogenicity, safety, and compliance of high- and standard-strength four-dose hepatitis B vaccination regimens in patients receiving methadone maintenance therapy in China: a randomized, parallel-arm controlled trial.

Expert Rev Vaccines 2021 Dec 16;20(12):1629-1635. Epub 2021 Sep 16.

School of Public Health, Shanxi Medical University, Taiyuan, Shanxi, China.

Background: We evaluated the safety and immunogenicity of four doses of 20 or 60 µg, and the immunogenicity and compliance of the short-term vaccination regimen (0, 1, and 2 months) among patients receiving MMT.

Research Design And Methods: We conducted a randomized controlled trial among 303 patients receiving MMT who were randomized to receive 3 or 4 doses of 20 or 60 µg of recombinant hepatitis B vaccine.

Results: At month 7, the seroconversion rates in both IM20 × 4 and IM60 × 4 groups were numerically higher than the IM20 × 3 group (0.05). The high-level responses and geometric mean concentration (GMC) of anti-HBs in both IM20 × 4 and IM60 × 4 groups were significantly higher than the IM20 × 3 group (0.05). The completion rate of the short-term high-strength vaccination group was significantly higher than the standard vaccination group (0.05), with similar immunogenicity (0.05).

Conclusions: Both the high-strength and standard-strength four-dose hepatitis B vaccine regimens could improve the immune response for patients receiving MMT. The high-strength short-term vaccination regimen could improve compliance and attain comparable immunogenicity with the standard vaccination regimen. The high-strength short-term vaccination regimen is recommended and the fourth dose is encouraged for this population considering the compliance and immunogenicity.

Clinical Trial Registration: ClinicalTrials.gov (NCT03962816).
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http://dx.doi.org/10.1080/14760584.2021.1977629DOI Listing
December 2021

Reduced bioaccumulation of fluorotelomer sulfonates and perfluoroalkyl acids in earthworms (Eisenia fetida) from soils amended with modified clays.

J Hazard Mater 2022 Feb 21;423(Pt A):126999. Epub 2021 Aug 21.

Department of Civil Engineering, McGill University, Montréal, QC, Canada. Electronic address:

Soils contaminated by per- and polyfluoroalkyl substances (PFAS) pose long-term sources to adjacent water bodies and soil invertebrates. The study investigated the stabilization using a modified clay adsorbent (FLUORO-SORB100®) in reducing the bioaccumulation of 13 anionic PFAS by earthworms (Eisenia fetida), as compared to coal-based granular activated carbon. The target PFAS included four perfluoroalkyl sulfonates such as perfluorooctane sulfonate (PFOS), six perfluoroalkyl carboxylates (e.g., perfluorooctanoate PFOA), and three (X:2) fluorotelomer sulfonates. Laboratory-spiked surface soil and the soil collected from a site contaminated by aqueous film-forming foams were examined. Both adsorbents resulted in reduced earthworm PFAS body burdens at the end of the 28-day uptake phase. The highest adsorbent amendment concentration (4 w/w%) was most effective, achieving >95% reduction of PFAS body burden. Soil leaching tests indicated better immobilization performance by the clay adsorbent for most analytes; in comparison, the activated carbon performed better at reducing total PFAS body burdens, possibly owing to the avoidance of larger-sized particles by earthworms. Strong positive logarithm relationships were observed between leachate concentrations and earthworm body burdens for most PFAS in the spiked soil. The study demonstrated that stabilization of PFAS using modified clay adsorbents can achieve concurrent benefits of lowering leachability and reducing bioaccumulation.
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http://dx.doi.org/10.1016/j.jhazmat.2021.126999DOI Listing
February 2022

The characterization, expression and activity analysis of three superoxide dismutases in Eriocheir hepuensis under azadirachtin stress.

Fish Shellfish Immunol 2021 Oct 18;117:228-239. Epub 2021 Aug 18.

Beibu Gulf University, Qinzhou, Guangxi, 530005, PR China; School of Marine Sciences, State Key Laboratory for Conservation and Utilization of Subtropical Agro-Bioresources, Guangxi University, Nanning, Guangxi, 530005, PR China. Electronic address:

Superoxide dismutase (SOD) can effectively eliminate of excess ROS, which causes oxidative damage to lipids, proteins, and DNA. In this study, we cloned the CuZn-SOD, cMn-SOD1, and cMn-SOD2 genes in Eriocheir hepuensis, and found that the coding sequence (CDS) lengths were 627 bp, 861 bp and 1062 bp, which encoded 208, 286, and 353 amino acids, respectively. Phylogenetic analysis indicated that all SOD genes were evolutionarily conserved, while cMn-SOD2 had an extra gap (67 amino acids) in the conserved domain compared with cMn-SOD1 without huge changes in the tertiary structure of the conserved domain, suggesting that cMn-SOD2 may be a duplicate of cMn-SOD1. qRT-PCR showed that the three SOD genes were widely expressed in all the tested tissues, CuZn-SOD and cMn-SOD1 were mostly expressed in the hepatopancreas, while cMn-SOD2 was mostly expressed in thoracic ganglia. Under azadirachtin stress, the oxidation index of surviving individuals, including the T-AOC, SOD activity, and MDA contents increased in the early stage and then remained steady except for a decrease in MDA contents in the later stage. qRT-PCR showed that the three SOD genes displayed the same trends as SOD activity in surviving individuals, and the highest expressions of CuZn-SOD in the hepatopancreas, heart, and gill were 14.16, 1.41, and 30.87 times that of the corresponding control group, respectively. The changes were 1.35, 5.77 and 3.33 fold for cMn-SOD1 and 1.62, 1.71 and 1.79 fold for cMn-SOD2, respectively. However, the activity and expression of SOD genes in dead individuals were lower than that observed in surviving individuals. These results reveal that SOD plays a significant role in the defence against azadirachtin-induced oxidative stress.
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http://dx.doi.org/10.1016/j.fsi.2021.08.010DOI Listing
October 2021

Spatiotemporal Immune Landscape of Colorectal Cancer Liver Metastasis at Single-Cell Level.

Cancer Discov 2022 01 20;12(1):134-153. Epub 2021 Aug 20.

Department of Liver Surgery and Transplantation, and Key Laboratory of Carcinogenesis and Cancer Invasion (Ministry of Education), Liver Cancer Institute, Zhongshan Hospital, Fudan University, Shanghai, China.

Liver metastasis, the leading cause of colorectal cancer mortality, exhibits a highly heterogeneous and suppressive immune microenvironment. Here, we sequenced 97 matched samples by using single-cell RNA sequencing and spatial transcriptomics. Strikingly, the metastatic microenvironment underwent remarkable spatial reprogramming of immunosuppressive cells such as M2-like macrophages. We further developed scMetabolism, a computational pipeline for quantifying single-cell metabolism, and observed that those macrophages harbored enhanced metabolic activity. Interestingly, neoadjuvant chemotherapy could block this status and restore the antitumor immune balance in responsive patients, whereas the nonresponsive patients deteriorated into a more suppressive one. Our work described the immune evolution of metastasis and uncovered the black box of how tumors respond to neoadjuvant chemotherapy. SIGNIFICANCE: We present a single-cell and spatial atlas of colorectal liver metastasis and found the highly metabolically activated M2-like macrophages in metastatic sites. Efficient neoadjuvant chemotherapy can slow down such metabolic activation, raising the possibility to target metabolism pathways in metastasis..
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http://dx.doi.org/10.1158/2159-8290.CD-21-0316DOI Listing
January 2022

The relationship between post-traumatic stress and negative emotions in patients with breast cancer: the mediating role of emotion regulation.

J Psychosoc Oncol 2021 Aug 14:1-13. Epub 2021 Aug 14.

School of Psychology, Weifang Medical University, Weifang, China.

Purpose: Negative emotions can adversely affect the treatment and recovery of breast cancer patients. Post-traumatic stress caused by cancer can increase the negative emotions of patients. This study assessed the relationship between post-traumatic stress and emotional regulation strategies, and the role of emotional regulation in the relationship between post-traumatic stress and negative emotions in breast cancer patients.

Design: Cross-sectional questionnaire with sample of 214 Chinese women with breast cancer.

Methods: Participants completed the Impact of Event Scale-Revised, Hospital Anxiety and Depression Scale, and Emotion Regulation Questionnaire. Correlation and mediation analyses were conducted to assess associations among the scores of these scales.

Findings: Patients with low post-traumatic stress chose cognitive reappraisal strategies, while those with high post-traumatic stress chose expressive suppression strategies. Cognitive reappraisal had a significant negative predictive effect on negative emotions, while expressive suppression had a significant positive predictive effect on patient's negative emotions.

Conclusions: Cognitive reappraisal may reduce the impact of post-traumatic stress on negative emotions experienced by breast cancer patients. Implications for psychosocial providers or policy: Psychosocial workers in China should conduct cognitive reappraisal training for breast cancer patients with high negative emotions and severe post-traumatic stress. For Chinese breast cancer patients living in other regions, the local oncology social workers should take into account their cultural background and lack of expression, and encourage them to choose cognitive reappraisal strategies.
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http://dx.doi.org/10.1080/07347332.2021.1950885DOI Listing
August 2021

Innovative strategies for enhanced tumor photodynamic therapy.

J Mater Chem B 2021 09 22;9(36):7347-7370. Epub 2021 Sep 22.

School of Public Health, Nantong University, No. 9, Seyuan Road, Nantong 226019, China.

Photodynamic therapy (PDT) is an approved and promising treatment approach that utilizes a photosensitizer (PS) to produce cytotoxic reactive oxygen species (ROS) through irradiation to achieve tumor noninvasive therapy. However, the limited singlet oxygen generation, the nonspecific uptake of PS in normal cells, and tumor hypoxia have become major challenges in conventional PDT, impeding its development and further clinical application. This review summarizes an overview of recent advances for the enhanced PDT. The development of PDT with innovative strategies, including molecular engineering and heavy atom-free photosensitizers is presented and future directions in this promising field are also provided. This review aims to highlight the recent advances in PDT and discuss the potential strategies that show promise in overcoming the challenges of PDT.
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http://dx.doi.org/10.1039/d1tb01466hDOI Listing
September 2021

A portable analytical system for rapid on-site determination of total nitrogen in water.

Water Res 2021 Sep 5;202:117410. Epub 2021 Jul 5.

Department of Mechanical and Industrial Engineering, University of Toronto, 5 King's College Park, Toronto, ON M5S 3G8, Canada; Institute of Biomedical Engineering, University of Toronto, 164 College Street, Toronto, ON M5S 3G9, Canada. Electronic address:

Excessive total nitrogen (TN) in the aqueous environment causes a notable negative impact on agriculture, human health, and the economy on a global scale. Conventional analytical techniques for determining TN in water usually involve long and tedious procedures with extensive sample preparation for digestion and titration. In recent years, lab-on-a-chip platforms have enabled in-situ measurements of water pollutants such as nitrate, nitrite, and ammonium. However, the digestion of organic nitrogen compounds in aqueous solutions still remains to be a challenge for portable analytical systems. In this paper, a portable TN analytical system is developed for on-site measurement of TN in a short assay time. It contains a TN reaction chamber for nitrogen digestion and reduction, and an optical measurement chamber for colorimetric determination of total nitrite. The ultraviolet-C (UVC)-thermal digestion method and the United States Environmental Protection Agency (EPA)-standard nitrate-nitrite determination method are implemented on the TN analytical system. Thorough investigations are performed to explore the optimum reaction conditions and reagent volumes in the process of TN oxidation, nitrate reduction, and nitrite detection, including oxidation time, temperature and substrate, oxidizer concentrations, nitrate reduction time, nitrite colorimetric reaction time, and reagents stability over time. Our system can complete fast oxidation and colorimetric determination of TN within 36 min, with a measurement range of 1 μg/L to 10 g/L and a limit of detection of 1.2 mg/L (lower than the World Health Organization standard of 10 mg/L). This portable TN analytical system enables the digestion and measurement of TN in a quick, portable, and low-cost manner.
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http://dx.doi.org/10.1016/j.watres.2021.117410DOI Listing
September 2021

Environmental Sources, Chemistry, Fate, and Transport of Per- and Polyfluoroalkyl Substances: State of the Science, Key Knowledge Gaps, and Recommendations Presented at the August 2019 SETAC Focus Topic Meeting.

Environ Toxicol Chem 2021 12 21;40(12):3234-3260. Epub 2021 Oct 21.

Naval Sea Systems Command, Laboratory Quality and Accreditation Office, Goose Creek, South Carolina, USA.

A Society of Environmental Toxicology and Chemistry (SETAC) Focused Topic Meeting (FTM) on the environmental management of per- and polyfluoroalkyl substances (PFAS) convened during August 2019 in Durham, North Carolina (USA). Experts from around the globe were brought together to critically evaluate new and emerging information on PFAS including chemistry, fate, transport, exposure, and toxicity. After plenary presentations, breakout groups were established and tasked to identify and adjudicate via panel discussions overarching conclusions and relevant data gaps. The present review is one in a series and summarizes outcomes of presentations and breakout discussions related to (1) primary sources and pathways in the environment, (2) sorption and transport in porous media, (3) precursor transformation, (4) practical approaches to the assessment of source zones, (5) standard and novel analytical methods with implications for environmental forensics and site management, and (6) classification and grouping from multiple perspectives. Outcomes illustrate that PFAS classification will continue to be a challenge, and additional pressing needs include increased availability of analytical standards and methods for assessment of PFAS and fate and transport, including precursor transformation. Although the state of the science is sufficient to support a degree of site-specific and flexible risk management, effective source prioritization tools, predictive fate and transport models, and improved and standardized analytical methods are needed to guide broader policies and best management practices. Environ Toxicol Chem 2021;40:3234-3260. © 2021 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC.
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http://dx.doi.org/10.1002/etc.5182DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8745034PMC
December 2021

The feasibility of family-centred early intervention for children with disabilities in mainland China: Practitioners' perceptions.

Child Care Health Dev 2021 11 22;47(6):869-876. Epub 2021 Jul 22.

Division of Vocational Education, Shenzhen Yuanping Special School, Shenzhen, China.

Background: Family-centred practice (FCP) has become a recommended practice for early intervention services for children with disabilities in many countries. However, its feasibility in Chinese context has been unclear. This study is the first to explore the perceptions of early intervention service practitioners about the implementation of FCP in mainland China.

Methods: Focus groups were employed to collect data from 37 early intervention practitioners who attended a workshop about FCP in Wuhan, China and two officers from the provincial disabled persons' federation. The data were analysed thematically.

Results: Four themes were identified: (a) family-centred early intervention is possible, (b) traditional concepts are not friendly towards FCP, (c) parents do not collaborate and (d) financing and personal resources are not sufficient to implement FCP. Chinese practitioners agreed with the philosophies of FCP; however, there was concern that widespread implementation may meet conceptual and practical challenges.

Conclusions: The results highlighted practitioners were optimistic and keen for FCP implementation in the Chinese context, but to do so across China may still be some way in the future.
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http://dx.doi.org/10.1111/cch.12898DOI Listing
November 2021

STXM-XANES and computational investigations of adsorption of per- and polyfluoroalkyl substances on modified clay.

Water Res 2021 Aug 17;201:117371. Epub 2021 Jun 17.

Department of Civil Engineering, McGill University, 817 Sherbrooke Street West, Montreal, QC, Abbreviation.

The study investigated molecular mechanisms of per- and polyfluoroalkyl substances (PFAS) on a surfactant modified clay (SMC), which rivals or exceeds the performance of granular activated carbon in removing long-chain PFAS from contaminated water. The adsorption isotherms of four anionic and one neutral PFAS from 1 × 10 to 1 × 10 mol/L were measured to be piecewise, accompanied by the expansion of the SMC interlayer. Based on the spatial distribution of perfluorocarboxylic acid (PFOA) on SMC at the submicron scale, achieved by synchrotron-based scanning transmission X-ray microscopy (STXM) coupled with X-ray absorption near-edge structure spectroscopy (XANES), PFOA molecules were confirmed to enter the interlayer space of SMC and could form charge-charge interaction with the intercalants (quaternary ammonia cations). Revealed by the all-atom molecular dynamics (MD) simulation and density functional theory-based quantum calculations, the interactions between the positively charged surfactant and representative PFAS include charge-charge, charge-dipole, and dipole-dipole interactions. The adsorption mechanisms vary from one PFAS structure to another in terms of adsorption energy and spatial arrangement. Those interactions overcome the interaction between PFAS and water, allowing PFAS to be retained in the SMC's interlayer space. The study provides fundamental insights into how PFAS interact with clay-based materials, supporting the use of the materials for PFAS treatment and remediation.
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http://dx.doi.org/10.1016/j.watres.2021.117371DOI Listing
August 2021

Nano drug delivery system reconstruct tumour vasculature for the tumour vascular normalisation.

J Drug Target 2022 02 20;30(2):119-130. Epub 2021 May 20.

Department of Pharmaceutics, School of Pharmacy, Ningxia Medical University, Yinchuan, China.

The abnormal structure and function of blood vessels in the TME are obvious characteristics of the tumour. Abnormal blood vessels with high leakage support the occurrence of malignant tumours and increase the possibility of tumour cell invasion and metastasis. The formation of abnormal vascular also enhances immunosuppression and prevents the delivery of chemotherapy drugs to deeper tumours. Therefore, the normalisation of tumour blood vessels is a very promising approach to improve anti-tumour efficacy, aiming to restore the structural integrity of vessels and improve drug delivery efficiency and anti-tumour immunity. In this review, we have summarised strategies to improve cancer treatment that via nano drug delivery technology regulates the normalisation of tumour blood vessels. The treatment strategies related to the structure and function of tumour blood vessels such as angiogenesis factors, tumour-associated macrophages, tumour vascular endothelial cells, tumour-associated fibroblasts and immune checkpoints in the TME were mainly discussed. The normalisation of tumour blood vessels presents new opportunities and challenges for the more efficient delivery of nanoparticles to tumour tissues and cells and an innovative combination of treatments for cancer.
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http://dx.doi.org/10.1080/1061186X.2021.1927056DOI Listing
February 2022

Detoxification of Oral Exposure to Benzo(a)pyrene by Lactobacillus plantarum CICC 23121 in Mice.

Mol Nutr Food Res 2021 06 10;65(12):e2001149. Epub 2021 May 10.

College of Biological Science & Biotechnology, Beijing Key Laboratory of Forest Food Processing and Safety, Beijing Forestry University, Beijing, 100083, China.

This study's previous work showed that the carcinogen and mutagen benzo(a)pyrene (BaP) can be adsorbed by Lactobacillus cells in vitro. However, in vivo BaP detoxification by lactic acid bacteria has not yet been investigated. The present study evaluates the effects of orally administered Lactobacillus plantarum CICC 23121 in BaP-treated mice. Oral administration of 50 mg kg BaP perturbed the intestinal microflora, caused Proteobacteria to predominate, and severely damaged DNA. However, oral administration of 5 × 10 CFU mL CICC 23121 in BaP-treated mice enhances fecal BaP excretion from 181.70 ± 1.04 µg/(g∙h) to 271.47 ± 11.71 µg/(g∙h) after 6 h. Fecal BaP excretion reaches up to 280.66 ± 22.97 µg/(g∙h) after the first 4 days of orally administered CICC 23121 and decreased to 94.31 ± 2.64 µg/(g∙h) by day 11. Intestinal microbiota are restored and Firmicutes predominates. CICC 23121 alleviates BaP-induced DNA damage and reduces tail length from 56.37 ± 5.31  to 39.69 ± 4.27 µm. Therefore, oral CICC23121 consumption is a promising strategy for reducing BaP toxicity in mice. To the best of our knowledge, this report is the first report to demonstrate in vivo that Lactobacillus cells can detoxify BaP.
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http://dx.doi.org/10.1002/mnfr.202001149DOI Listing
June 2021

Stability of Nitrogen-Containing Polyfluoroalkyl Substances in Aerobic Soils.

Environ Sci Technol 2021 04 19;55(8):4698-4708. Epub 2021 Mar 19.

Department of Civil Engineering, McGill University, Montreal, QC H3A 0C3, Canada.

Zwitterionic per- and polyfluoroalkyl substances (PFASs) used in aqueous film-forming foams (AFFFs) could face diverse environmental fates once released at military bases, airports, fire-training areas, and accidental release sites. Here, we studied for the first time the transformation potential of four electrochemical fluorination (ECF)-based PFAS zwitterions (two carboxyl betaines and two tertiary amines) in aerobic soils. The two perfluoroalkyl sulfonamide derivatives were precursors to perfluorooctanesulfonate (PFOS), while the amide derivatives were precursors to perfluorooctane carboxylate (PFOA). These zwitterions and four other previously reported zwitterions or cations were compared for their transformation pathways and kinetics. Structural differences, especially the nitrogen head groups, largely influenced the persistence of these compounds in aerobic soils. The perfluoroalkyl sulfonamide-based compounds showed higher microbial stability than the corresponding perfluoroalkyl amide-based ones. Their stability in aerobic soils is ranked based on the magnitude of DT (time for 50% of substance to disappear): quaternary ammonium ≈ carboxyl betaine ≫ tertiary amine > amine oxide. The PFASs containing quaternary ammonium or betaine groups showed high stability in soils, with the longest DT likely to be years or decades, while those with tertiary amine or amine oxide groups showed DT of weeks or months. These eight ECF-based precursors provide insights into the degradation pathways and persistence in surface soils of other perfluoroalkyl cations and zwitterions present in AFFFs.
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http://dx.doi.org/10.1021/acs.est.0c05811DOI Listing
April 2021

Fate and transport of per- and polyfluoroalkyl substances (PFASs) in the vadose zone.

Sci Total Environ 2021 Jun 26;771:145427. Epub 2021 Jan 26.

Department of Civil and Environmental Engineering, Colorado State University, Fort Collins, CO 80523, USA. Electronic address:

Per- and polyfluoroalkyl substances (PFASs) are a heterogeneous group of persistent organic pollutants that have been detected in various environmental compartments around the globe. Emerging research has revealed the preferential accumulation of PFASs in shallow soil horizons, particularly at sites impacted by firefighting activities, agricultural applications, and atmospheric deposition. Once in the vadose zone, PFASs can sorb to soil, accumulate at interfaces, become volatilized, be taken up in biota, or leach to the underlying aquifer. At the same time, polyfluorinated precursor species may transform into highly recalcitrant perfluoroalkyl acids, changing their chemical identity and thus transport behavior along the way. In this review, we critically discuss the current state of the knowledge and aim to interconnect the complex processes that control the fate and transport of PFASs in the vadose zone. Furthermore, we identify key challenges and future research needs. Consequently, this review may serve as an interdisciplinary guide for the risk assessment and management of PFAS-contaminated sites.
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http://dx.doi.org/10.1016/j.scitotenv.2021.145427DOI Listing
June 2021

Occurrence and Distribution of Per- and Polyfluoroalkyl Substances in Tianjin, China: The Contribution of Emerging and Unknown Analogues.

Environ Sci Technol 2020 11 6;54(22):14254-14264. Epub 2020 Nov 6.

Department of Chemistry, Université de Montréal, Montreal, Quebec H3C 3J7, Canada.

Tianjin, located in Bohai Bay, China, constitutes a relevant study area to investigate emerging per- and polyfluoroalkyl substances (PFASs) due to its high population density, clustering of chemical and aircraft industries, as well as international airports, harbors, and oil rigs. In this study, 53 anionic, zwitterionic, and cationic PFASs were monitored in river surface water, groundwater, seawater, and sediments in this area (overall = 226). 6:2 chlorinated polyfluorinated ether sulfonic acid (Cl-PFESA), perfluorooctanoic acid, and perfluorooctane sulfonic acid were generally the predominant PFASs. 6:2 fluorotelomer sulfonamidoalkyl betaine (6:2 FTAB) was also widespread (occurrence >86%), with the highest concentration (1300 ng/L) detected at contamination hot spots impacted by wastewater effluents. The aqueous film-forming foam (AFFF)-related PFASs with sulfonamide betaine, amine oxide, amine, or quaternary ammonium moieties are also reported for the first time in river water and seawater samples. Fifteen classes of infrequently reported PFASs, including :2 FTABs and :2 fluorotelomer sulfonamide amines, hydrogen-substituted PFESA homologues, and -perfluorous nonenoxybenzenesulfonate (OBS), were also identified in the water and sediment samples using suspect screening. Field-derived sediment-water distribution coefficients () of these emerging PFASs are provided for the first time, confirming that cationic and zwitterionic PFASs tend to be strongly associated with sediments.
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http://dx.doi.org/10.1021/acs.est.0c00934DOI Listing
November 2020

A novel β2-AR/YB-1/β-catenin axis mediates chronic stress-associated metastasis in hepatocellular carcinoma.

Oncogenesis 2020 Sep 24;9(9):84. Epub 2020 Sep 24.

Department of Gastroenterology, Affiliated Hospital of Nantong University, Nantong, China.

β-Adrenergic receptor (β-AR) signalling is strongly associated with tumour progression by the coupling of β-ARs with either a G protein or β-arrestin; however, the related mechanism underlying hepatocellular carcinoma (HCC) metastasis is not clear. Here, we reveal that the transcription factor Y-box binding protein 1 (YB-1) interacts with β2-adrenergic receptor (β2-AR) following stimulation with the agonist isoproterenol (ISO). Clinicopathological analysis demonstrated that β2-AR is significantly correlated with YB-1, which favours the progression of HCC. The binding of YB-1 with β2-AR resulted in YB-1 phosphorylation at serine 102 (S102) via the β-arrestin-1-dependent activation of the PI3K/AKT pathway, followed by the translocation of YB-1 to the nucleus to carry out its tumour-related function. β2-AR-mediated activation of YB-1 facilitated epithelial-to-mesenchymal transition (EMT) and HCC metastasis. The interference of YB-1 expression significantly attenuated liver tumour metastasis induced by chronic stress. Analysis of the transcriptional profile and chromatin immunoprecipitation (ChIP) identified β-catenin as a crucial target of YB-1. Our results unveiled a novel β2-AR-mediated regulatory axis in HCC metastasis that might be helpful for the development of HCC therapeutics.
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http://dx.doi.org/10.1038/s41389-020-00268-wDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7515897PMC
September 2020

Tumor Microenvironment-Triggered Charge Reversal Polymetformin-Based Nanosystem Co-Delivered Doxorubicin and IL-12 Cytokine Gene for Chemo-Gene Combination Therapy on Metastatic Breast Cancer.

ACS Appl Mater Interfaces 2020 Oct 29;12(41):45873-45890. Epub 2020 Sep 29.

Department of Pharmaceutics, School of Pharmacy, Ningxia Medical University, No. 1160, Shengli Street, Yinchuan 750004, China.

Cancer metastasis is the leading cause of high mortality and disease recurrence in breast cancer. In this study, a novel tumor microenvironment charge reversal polymetformin (PMet)-based nanosystem co-delivering doxorubicin (DOX) and plasmid encoding IL-12 gene (pIL-12) was developed for chemo-gene combination therapy on metastatic breast cancer. Cationic PMet was readily self-assembled into micelles for DOX physical encapsulation and pIL-12 complexation, and a hyaluronidase-sensitive thiolated hyaluronic acid (HA-SH) was then collaboratively assembled to the pIL-12/DOX-PMet micelleplexes, abbreviated as HA/pIL-12/DOX-PMet. DOX/pIL-12 loaded in HA/pIL-12/DOX-PMet micelleplexes presented prolonged circulation in blood, efficient accumulation in tumors, and internalization in tumor cells via CD44 receptor-mediated tumor specific-targeting, and DOX/pIL-12 was co-released in endo/lysosomes tumor microenvironment followed by HAase-triggered HA-SH deshielding from HA/pIL-12/DOX-PMet micelleplexes. Moreover, HA/PMet micelleplexes displayed excellent pIL-12 transfection and IL-12 expression in tumors of 4T1 tumor-bearing mice. Importantly, HA/pIL-12/DOX-PMet micelleplexes synergistically enhanced the NK cells and tumor infiltrated cytotoxic T lymphocytes and modulated the polarization from protumor M2 macrophages to activated antitumor M1 macrophages, with concomitant decreasing of the immunosuppressive regulatory T (Treg) cells, accompanied by an increase in the cytokines expression of IL-12, IFN-γ and TNF-α, consequently showing an improved antitumor and antimetastasis activity in 4T1 breast cancer lung metastasis mice model. In conclusion, the tumor microenvironment charge reversal HA/PMet nanosystem holds great promise for DOX/pIL-12 co-delivery and exploitation in chemo-gene combination therapy on metastatic breast cancer.
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http://dx.doi.org/10.1021/acsami.0c14405DOI Listing
October 2020
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