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1.
Cancer Sci ; 115(1): 70-82, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37964506

RESUMEN

To evaluate the potential of zinc finger protein 1 (ZPR1) as a diagnostic biomarker and explore the underlying role for esophageal squamous cell carcinoma (ESCC). A human proteome microarray was customized to identify anti-ZPR1 autoantibody, and enzyme-linked immunosorbent assay (ELISA) was adopted to assess the diagnostic performance of anti-ZPR1 autoantibody in 294 patients with ESCC and 294 normal controls. The expression of ZPR1 protein was measured by immunohistochemistry. The effect of ZPR1 on the proliferation, migration, and invasion of ESCC cells was investigated through CCK-8, wound healing, and Transwell assays. The expression level of anti-ZPR1 autoantibody (fold change = 2.77) in ESCC patients was higher than that in normal controls. The receiver operating characteristic (ROC) analysis manifested anti-ZPR1 autoantibody achieved area under the ROC curve (AUC) of 0.726 and 0.734 to distinguish ESCC from normal controls with sensitivity of 50.0% and 42.3%, and specificity of 91.0% and 92.0% in the test group and validation group, respectively. The positive rate of ZPR1 protein was significantly higher in ESCC tissues (75.5%, 80/106) than paracancerous tissues (9.4%, 5/53). Compared with the human normal esophageal cell line, the expression level of ZPR1 mRNA and protein in ESCC lines (KYSE150, Eca109, and TE1) had an increased trend. The knockdown or overexpression of ZPR1 reduced and enhanced the proliferation, migration, and invasion of ESCC cell, respectively. ZPR1 was a potential immunodiagnostic biomarker for noninvasive detection and could be a promotional factor in tumor progression of ESCC.


Asunto(s)
Carcinoma de Células Escamosas , Neoplasias Esofágicas , Carcinoma de Células Escamosas de Esófago , Humanos , Carcinoma de Células Escamosas de Esófago/genética , Neoplasias Esofágicas/genética , Carcinoma de Células Escamosas/patología , Biomarcadores , Autoanticuerpos/metabolismo , Línea Celular Tumoral , Proliferación Celular , Movimiento Celular , Regulación Neoplásica de la Expresión Génica
2.
J Med Virol ; 96(3): e29530, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38529528

RESUMEN

Integration of hepatitis B virus (HBV) DNA into the human genome is recognized as an oncogenic factor and a barrier to hepatitis B cure. In the study, biopsy liver tissues were collected from adolescents and young adults with acute HBV infection younger than or equal to 35 years of age and from HBV-infected infant patients younger than or equal to 6 months of age. A high-throughput sequencing method was used to detect HBV DNA integration. Totally, 12 adolescents, young adults, and 6 infants were included. Among the 12 patients with acute HBV infection, immunohistochemical staining of intrahepatic hepatitis B surface antigen for all displayed negative results, and no HBV DNA integrants in the hepatocyte DNA were confirmed. All infant patients had elevated levels of alanine aminotransferase and high levels of serum HBV DNA. Numerous gene sites of hepatocyte DNA were integrated by HBV DNA for each infant patient, ranging from 120 to 430 integration sites. The fragile histidine triad gene was the high-frequency integrated site in the intragenic region for infant patients. In conclusion, hepatocyte DNA is integrated by HBV DNA in babies with active hepatitis B but seems seldom affected among adolescents and young adults with acute HBV infection. Infantile hepatitis B should be taken seriously considering abundant HBV DNA integration events.


Asunto(s)
Hepatitis B Crónica , Hepatitis B , Lactante , Adolescente , Humanos , Adulto Joven , Virus de la Hepatitis B/genética , ADN Viral/genética , Hígado/patología , Antígenos de Superficie de la Hepatitis B/genética , Antígenos e de la Hepatitis B , Genómica
3.
Br J Dermatol ; 2024 Apr 24.
Artículo en Inglés | MEDLINE | ID: mdl-38655652

RESUMEN

OBJECTIVE: Psoriasis is a common, chronic inflammatory disease with unclear etiology. Keratinocytes in psoriasis are susceptible to exogenous triggers that induce inflammatory cell death. This study investigated whether GSDME-mediated pyroptosis in keratinocytes contributes to the pathogenesis of psoriasis. METHODS: Skin samples from patients with psoriasis and healthy controls were collected to evaluate the expression of GSDME, cleaved-caspase-3, and inflammatory factors. We then analyzed the data series, GSE41662, to further compare the expression of GSDME between lesional and non-lesional skin samples in those with psoriasis. In vivo, caspase-3 inhibitor and GSDME deficiency mice (Gsdme-/-) were applied to block caspase-3/GSDME activation in the imiquimod-induced psoriasis model. Skin inflammation, disease severity, and pyroptosis-related proteins were analyzed. In vitro, tumor necrosis factor-α (TNF-α)-induced caspase-3/GSDME-mediated pyroptosis in the HACAT cell line was explored. RESULTS: Our analysis of the GSE41662 data series found that GSDME were upregulated in psoriasis lesions, compared to normal skin. High levels of inflammatory cytokines such as IL-1ß, IL-6, and TNF-α were also found in psoriasis lesions. In mice of Gsdme-/- and caspase-3 inhibitor groups, the severity of skin inflammation was attenuated, and GSDME and C-caspase-3 levels decreased after imiquimod treatment. Similarly, IL-1ß, IL-6, and TNF-α were decreased in Gsdme-/- and caspase-3 inhibitor groups. In vitro, TNF-α induced HACAT cell pyroptosis through caspase-3/GSDME pathway activation, which was suppressed by blocking caspase-3 or silencing GSDME. CONCLUSION: Our study provides a novel explanation that TNF-α/caspase-3/GSDME-mediated keratinocyte pyroptosis is highly responsible for the initiation and acceleration of skin inflammation and progression of psoriasis.

4.
Environ Sci Technol ; 58(6): 2891-2901, 2024 Feb 13.
Artículo en Inglés | MEDLINE | ID: mdl-38308618

RESUMEN

Direct interspecies electron transfer (DIET) provides an innovative way to achieve efficient methanogenesis, and this study proposes a new approach to upregulate the DIET pathway by enhancing quorum sensing (QS). Based on long-term reactor performance, QS enhancement achieved more vigorous methanogenesis with 98.7% COD removal efficiency. In the control system, methanogenesis failure occurred at the accumulated acetate of 7420 mg of COD/L and lowered pH of 6.04, and a much lower COD removal of 41.9% was observed. The more significant DIET in QS-enhancing system was supported by higher expression of conductive pili and the c-Cyts cytochrome secretion-related genes, resulting in 12.7- and 10.3-fold improvements. Moreover, QS enhancement also improved the energy production capability, with the increase of F-type and V/A-type ATPase expression by 6.3- and 4.2-fold, and this effect probably provided more energy for nanowires and c-Cyts cytochrome secretion. From the perspective of community structure, QS enhancement increased the abundance of Methanosaeta and Geobacter from 54.3 and 17.6% in the control to 63.0 and 33.8%, respectively. Furthermore, the expression of genes involved in carbon dioxide reduction and alcohol dehydrogenation increased by 0.6- and 7.1-fold, respectively. Taken together, this study indicates the positive effects of QS chemicals to stimulate DIET and advances the understanding of the DIET methanogenesis involved in environments such as anaerobic digesters and sediments.


Asunto(s)
Electrones , Percepción de Quorum , Anaerobiosis , Transporte de Electrón , Citocromos/metabolismo , Metano , Reactores Biológicos
5.
J Nanobiotechnology ; 22(1): 237, 2024 May 12.
Artículo en Inglés | MEDLINE | ID: mdl-38735920

RESUMEN

BACKGROUND: Myeloid-derived suppressor cells (MDSCs) promote tumor growth, metastasis, and lead to immunotherapy resistance. Studies revealed that miRNAs are also expressed in MDSCs and promote the immunosuppressive function of MDSCs. Currently, few studies have been reported on inducible cellular microvesicle delivery of nucleic acid drugs targeting miRNA in MDSCs for the treatment of malignant tumors. RESULTS AND CONCLUSION: In this study, we designed an artificial DNA named G-quadruplex-enhanced circular single-stranded DNA-9 (G4-CSSD9), that specifically adsorbs the miR-9 sequence. Its advanced DNA folding structure, rich in tandem repeat guanine (G-quadruplex), also provides good stability. Mesenchymal stem cells (MSCs) were prepared into nanostructured vesicles by membrane extrusion. The MSC microvesicles-encapsulated G4-CSSD9 (MVs@G4-CSSD9) was delivered into MDSCs, which affected the downstream transcription and translation process, and reduced the immunosuppressive function of MDSCs, so as to achieve the purpose of treating melanoma. In particular, it provides an idea for the malignant tumor treatment.


Asunto(s)
ADN de Cadena Simple , G-Cuádruplex , Células Madre Mesenquimatosas , MicroARNs , Células Supresoras de Origen Mieloide , Animales , Células Supresoras de Origen Mieloide/metabolismo , Ratones , ADN de Cadena Simple/química , Línea Celular Tumoral , Ratones Endogámicos C57BL , Micropartículas Derivadas de Células/química , Micropartículas Derivadas de Células/metabolismo , ADN Circular/química , Humanos , Melanoma/tratamiento farmacológico
6.
BMC Biol ; 21(1): 169, 2023 08 08.
Artículo en Inglés | MEDLINE | ID: mdl-37553612

RESUMEN

BACKGROUND: The nutrient-absorbing villi of small intestines are renewed and repaired by intestinal stem cells (ISCs), which reside in a well-organized crypt structure. Genetic studies have shown that Wnt molecules secreted by telocytes, Gli1+ stromal cells, and epithelial cells are required for ISC proliferation and villus homeostasis. Intestinal stromal cells are heterogeneous and single-cell profiling has divided them into telocytes/subepithelial myofibroblasts, myocytes, pericytes, trophocytes, and Pdgfralow stromal cells. Yet, the niche function of these stromal populations remains incompletely understood. RESULTS: We show here that a Twist2 stromal lineage, which constitutes the Pdgfralow stromal cell and trophocyte subpopulations, maintains the crypt structure to provide an inflammation-restricting niche for regenerating ISCs. Ablating Twist2 lineage cells or deletion of one Wntless allele in these cells disturbs the crypt structure and impairs villus homeostasis. Upon radiation, Wntless haplo-deficiency caused decreased production of anti-microbial peptides and increased inflammation, leading to defective ISC proliferation and crypt regeneration, which were partially rescued by eradication of commensal bacteria. In addition, we show that Wnts secreted by Acta2+ subpopulations also play a role in crypt regeneration but not homeostasis. CONCLUSIONS: These findings suggest that ISCs may require different niches for villus homeostasis and regeneration and that the Twist2 lineage cells may help to maintain a microbe-restricted environment to allow ISC-mediated crypt regeneration.


Asunto(s)
Linaje de la Célula , Homeostasis , Intestinos , Nicho de Células Madre , Células Madre , Células Madre/citología , Células Madre/metabolismo , Intestinos/citología , Intestinos/metabolismo , Mucosa Intestinal/citología , Mucosa Intestinal/metabolismo , Animales , Ratones
7.
J Sci Food Agric ; 104(10): 6262-6275, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-38466088

RESUMEN

BACKGROUND: Early weaning is prone to damage intestinal barrier function, resulting in diarrhea, whereas rutin, as a natural flavonoid with multiple biological functions, shows potential in piglets. Therefore, the effects of dietary rutin on growth, antidiarrheal, barrier function, antioxidant status and cecal microbiota of weaned piglets were investigated with the control group (CON) (basal diet) and Rutin (basal diet+500 mg kg-1 rutin) groups fed for 14 days. RESULTS: The results showed that dietary 500 mg kg-1 rutin significantly decreased diarrhea index, serum diamine oxidase activity and total aerobic bacterial population in mesenteric lymph nodes, whereas it significantly increased the gain-to-feed ratio (G:F) and serum growth hormone content, jejunal villus height and villus height to crypt depth ratio, and also enhanced jejunal claudin-1 and zonula occludens-1 mRNA and protein expression. Meanwhile, dietary rutin significantly decreased inflammation-associated mRNA expression, malondialdehyde (MDA) content, swollen mitochondrial number and mitochondrial area in the jejunum, whereas it increased the total superoxide dismutase (T-SOD) and glutathione peroxidase activities and activated the Nrf2 signaling pathway. Moreover, dietary rutin significantly increased Firmicutes abundance and decreased Campylobacterota abundance, which were closely associated with the decreased diarrhea index and MDA content or increased Claudin-1 expression and T-SOD activity. CONCLUSION: Dietary 500 mg kg-1 rutin increased G:F by improving intestinal morphology, and alleviated diarrhea by enhancing intestinal barrier, which might be associated with the enhanced antioxidant capacity via activating the Nrf2/Keap1 signaling pathway and the improved cecal microbial composition in weaned piglets. © 2024 Society of Chemical Industry.


Asunto(s)
Antidiarreicos , Antioxidantes , Ciego , Diarrea , Microbioma Gastrointestinal , Mucosa Intestinal , Rutina , Destete , Animales , Porcinos/metabolismo , Porcinos/crecimiento & desarrollo , Microbioma Gastrointestinal/efectos de los fármacos , Antioxidantes/metabolismo , Ciego/microbiología , Ciego/metabolismo , Mucosa Intestinal/metabolismo , Diarrea/microbiología , Diarrea/dietoterapia , Diarrea/veterinaria , Antidiarreicos/administración & dosificación , Bacterias/clasificación , Bacterias/aislamiento & purificación , Bacterias/genética , Bacterias/metabolismo , Enfermedades de los Porcinos/microbiología , Enfermedades de los Porcinos/metabolismo , Claudina-1/metabolismo , Claudina-1/genética , Alimentación Animal/análisis , Yeyuno/metabolismo , Yeyuno/microbiología , Suplementos Dietéticos/análisis , Masculino , Superóxido Dismutasa/metabolismo , Malondialdehído/metabolismo , Funcion de la Barrera Intestinal
8.
BMC Oral Health ; 24(1): 23, 2024 01 04.
Artículo en Inglés | MEDLINE | ID: mdl-38178129

RESUMEN

BACKGROUND: The purpose of this study is to explore the effects of CB2 on bone regulation during orthodontic tooth movement. METHODS: Thirty male mice were allocated into 2 groups (n = 15 in each group): wild type (WT) group and CB2 knockout (CB2-/-) group. Orthodontic tooth movement (OTM) was induced by applying a nickel-titanium coil spring between the maxillary first molar and the central incisors. There are three subgroups within the WT groups (0, 7 and 14 days) and the CB2-/- groups (0, 7 and 14 days). 0-day groups without force application. Tooth displacement, alveolar bone mass and alveolar bone volume were assessed by micro-CT on 0, 7 and 14 days, and the number of osteoclasts was quantified by tartrate-resistant acid phosphatase (TRAP) staining. Moreover, the expression levels of RANKL and OPG in the compression area were measured histomorphometrically. RESULTS: The WT group exhibited the typical pattern of OTM, characterized by narrowed periodontal space and bone resorption on the compression area. In contrast, the accelerated tooth displacement, increased osteoclast number (P < 0.0001) and bone resorption on the compression area in CB2-/- group. Additionally, the expression of RANKL was significantly upregulated, while OPG showed low levels in the compression area of the CB2 - / - group (P < 0.0001). CONCLUSIONS: CB2 modulated OTM and bone remodeling through regulating osteoclast activity and RANKL/OPG balance.


Asunto(s)
Remodelación Ósea , Resorción Ósea , Receptor Cannabinoide CB2 , Técnicas de Movimiento Dental , Animales , Masculino , Ratones , Remodelación Ósea/fisiología , Osteoclastos , Receptor Cannabinoide CB2/genética
9.
J Environ Sci (China) ; 146: 118-126, 2024 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-38969440

RESUMEN

With the increasing demand of recycling disposal of industrial wastewater, oil-in-water (O/W) emulsion has been paid much attention in recent years owing to its high oil content. However, due to the presence of surfactant and salt, the emulsion was usually stable with complex physicochemical interfacial properties leading to increased processing difficulty. Herein, a novel flow-through electrode-based demulsification reactor (FEDR) was well designed for the treatment of saline O/W emulsion. In contrast to 53.7% for electrical demulsification only and 80.3% for filtration only, the COD removal efficiency increased to 92.8% under FEDR system. Moreover, the pore size of electrode and the applied voltage were two key factors that governed the FEDR demulsification performance. By observing the morphology of oil droplets deposited layer after different operation conditions and the behavior of oil droplets at the electrode surface under different voltage conditions, the mechanism was proposed that the oil droplets first accumulated on the surface of flow-through electrode by sieving effect, subsequently the gathered oil droplets could further coalesce with the promoting effect of the anode, leading to a high-performing demulsification. This study offers an attractive option of using flow-through electrode to accomplish the oil recovery with simultaneous water purification.


Asunto(s)
Electrodos , Filtración , Eliminación de Residuos Líquidos , Purificación del Agua , Purificación del Agua/métodos , Filtración/métodos , Eliminación de Residuos Líquidos/métodos , Aceites/química , Aguas Residuales/química , Contaminantes Químicos del Agua/química , Emulsiones/química , Técnicas Electroquímicas/métodos , Técnicas Electroquímicas/instrumentación
10.
Zhongguo Dang Dai Er Ke Za Zhi ; 26(6): 659-664, 2024 Jun 15.
Artículo en Zh | MEDLINE | ID: mdl-38926385

RESUMEN

In infants with severe bronchopulmonary dysplasia (sBPD), severe pulmonary lobar emphysema may occur as a complication, contributing to significant impairment in ventilation. Clinical management of these infants is extremely challenging and some may require lobectomy to improve ventilation. However, prior to the lobectomy, it is very difficult to assess whether the remaining lung parenchyma would be able to sustain adequate ventilation postoperatively. In addition, preoperative planning and perioperative management are also quite challenging in these patients. This paper reports the utility of selective bronchial occlusion in assessing the safety and efficacy of lobectomy in a case of sBPD complicated by severe right upper lobar emphysema. Since infants with sBPD already have poor lung development and significant lung injury, lobectomy should be viewed as a non-traditional therapy and be carried out with extreme caution. Selective bronchial occlusion test can be an effective tool in assessing the risks and benefits of lobectomy in cases with sBPD and lobar emphysema. However, given the technical difficulty, successful application of this technique requires close collaboration of an experienced interdisciplinary team.


Asunto(s)
Displasia Broncopulmonar , Recien Nacido Prematuro , Enfisema Pulmonar , Humanos , Enfisema Pulmonar/cirugía , Displasia Broncopulmonar/etiología , Recién Nacido , Bronquios , Masculino , Neumonectomía , Femenino
11.
J Am Chem Soc ; 145(3): 1759-1768, 2023 Jan 25.
Artículo en Inglés | MEDLINE | ID: mdl-36607337

RESUMEN

Integrating different reaction sites offers new prospects to address the difficulties in single-atom catalysis, but the precise regulation of active sites at the atomic level remains challenging. Here, we demonstrate a sodium-directed photon-induced assembly (SPA) strategy for boosting the atomic utilization efficiency of single-atom catalysts (SACs) by constructing multifarious Au sites on TiO2 substrate. Na+ was employed as the crucial cement to direct Au single atoms onto TiO2, while the light-induced electron transfer from excited TiO2 to Au(Na+) ensembles contributed to the self-assembly formation of Au nanoclusters. The synergism between plasmonic near-field and Schottky junction enabled the cascade electron transfer for charge separation, which was further enhanced by oxygen vacancies in TiO2. Our dual-site photocatalysts exhibited a nearly 2 orders of magnitude improvement in the hydrogen evolution activity under simulated solar light, with a striking turnover frequency (TOF) value of 1533 h-1 that exceeded other Au/TiO2-based photocatalysts reported. Our SPA strategy can be easily extended to prepare a wide range of metal-coupled nanostructures with enhanced performance for diverse catalytic reactions. Thus, this study provides a well-defined platform to extend the boundaries of SACs for multisite catalysis through harnessing metal-support interactions.

12.
Pharmacol Res ; 188: 106661, 2023 02.
Artículo en Inglés | MEDLINE | ID: mdl-36669583

RESUMEN

Hepatocellular carcinoma (HCC) is one of the leading causes of death, which deserves further study to reveal the underlying molecular mechanisms. Studies have shown that miR-9 in associated with poor prognosis in HCC patients. However, the mechanisms of transcriptional activation regulation of miR-9 and its role in the malignant progression of HCC have been rarely investigated. Some transcriptional coactivators can form phase-separated condensates at super-enhancers that compartmentalize and concentrate the transcription apparatus to drive robust gene expression. Here, we demonstrate that Twist1 and YY1 could form a transcriptional complex with p300, creating local high-concentration phase-separated interaction hubs at the super-enhancers of miR-9 and activate its expression to promote the malignant progression of HCC by stimulating the migration and invasion of hepatocellular carcinoma cells. Twist1-YY1-p300 phase-separated condensates were disrupted by metformin (Met) and thus reduce miR-9 expression, thereby inhibiting the malignant progression of HCC. Our study demonstrates that the Twist1 transcriptional factor complex involved in the malignant progression of HCC can form phase separation condensates at super-enhancers of miR-9 to promote the expression of oncogenes in HCC cells. It provides a potential target for the therapy of HCC and offers insights into the mechanism of Met in HCC inhibition.


Asunto(s)
Carcinoma Hepatocelular , Neoplasias Hepáticas , Metformina , MicroARNs , Humanos , Carcinoma Hepatocelular/tratamiento farmacológico , Carcinoma Hepatocelular/genética , Carcinoma Hepatocelular/metabolismo , Neoplasias Hepáticas/tratamiento farmacológico , Neoplasias Hepáticas/genética , Neoplasias Hepáticas/metabolismo , Metformina/farmacología , Metformina/uso terapéutico , Regulación Neoplásica de la Expresión Génica , MicroARNs/genética , MicroARNs/metabolismo , Línea Celular Tumoral , Proliferación Celular , Proteínas Nucleares/genética , Proteínas Nucleares/metabolismo , Proteína 1 Relacionada con Twist/genética , Proteína 1 Relacionada con Twist/metabolismo , Factor de Transcripción YY1/genética , Factor de Transcripción YY1/metabolismo
13.
Cell Biol Int ; 47(11): 1825-1834, 2023 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-37545170

RESUMEN

Gemcitabine (GEM)-based chemotherapy represents the first choice for locally unresectable advanced pancreatic cancer, while the benefit is limited due to acquired chemoresistance or drug delivery insufficiency. Hyperthermia treatment potentially improves the clinical efficacy of GEM. However, the underlying mechanism is incompletely revealed. Our study aims to investigate the effect and involved mechanism of thermochemotherapy on cell survival. Pancreatic cancer cells PANC-1 and ASPC-1 were either treated with GEM or thermochemotherapy, then cell viability, apoptosis, migration, invasion, reactive oxygen species (ROS) production, and Sp1 expression were evaluated. The results showed that GEM dose and time-dependently affected cell viability, and 30 µM GEM achieved favorable effect in suppressing cancer cell growth. Meanwhile, hyperthermia preconditioning (43°C for 60 min) 24 h before GEM treatment yielded superior effect than other treatment sequence. GEM caused significant cell apoptosis and proapoptotic genes of both cancer cells, and thermochemotherapy further promoted apoptosis and genes transcription, accompanied by excessive ROS production. Thermochemotherapy was superior to GEM in suppressing cell migration and invasion of pancreatic cancer cells. Meanwhile, GEM significantly reduced Sp1 mRNA and protein and its downstream gene Cox-2, and thermochemotherapy further suppressed their expressions. ROS elimination with N-acetyl-l-cysteine notably neutralizes the suppressive effect of GEM and thermochemotherapy on cell growth and expressions of Sp1 and Cox-2. In conclusion, thermochemotherapy inhibited pancreatic cell viability, migration and invasion, and promoted cell apoptosis by inducing excessive ROS production, which subsequently suppressed Sp1 expression and the downstream Cox-2.

14.
Environ Sci Technol ; 57(32): 12083-12093, 2023 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-37530558

RESUMEN

Demulsification using membranes is a promising method to coalesce highly stable emulsified oil droplets for oil recovery. Nevertheless, a structure of the current filtration medium that is not efficient for oil droplet coalescence impedes rapid permeability, thereby inevitably restricting their practical applications. Herein, we report a hydrophobic-hydrophilic-hydrophobic (3H) demulsification medium that exhibits a benchmark permeability of ∼2.1 × 104 L m-2 h-1 with a demulsification efficiency of >98.0%. Remarkably, this 3H demulsification medium maintains over 90% demulsification efficiency in the oil-in-water (O/W) emulsions with a wide range of surfactant concentrations, which shows excellent applicability. Based on the combined results of quasi situ microscope images and molecular dynamics simulations, we show that the polydimethylsiloxane-modified hydrophobic layer facilitates the capture and coalescence of oil droplets, the hydrophilic inner layer assists in squeezing the coalescence of enlarged droplets, and the third hydrophobic layer accelerates the discharge of demulsified oil to sustain permeability. The sequential demulsification mechanism between this 3H filtration layer provides a general guide for designing a demulsifying membrane with high demulsification efficiency and high flux toward oil recovery.

15.
Environ Sci Technol ; 57(32): 12117-12126, 2023 08 15.
Artículo en Inglés | MEDLINE | ID: mdl-37525979

RESUMEN

Regulation of the free radical types is crucial but challenging in the ubiquitous heterogeneous catalytic oxidation for chemosynthesis, biotherapy, and environmental remediation. Here, using aromatic pollutant (AP) removal as a prototype, we identify the massive accumulation of the benzoquinone (BQ) intermediate in the hydroxyl radical (•OH)-mediated AP degradation process. Theoretical prediction and experiments demonstrate that BQ is both a Lewis acid and base because of its unique molecular and electronic structure caused by the existence of symmetrical carbonyl groups; therefore, it is hard to be electrophilically added by oxidizing •OH as a result of the high reaction energy barrier (ΔG = 1.74 eV). Fortunately, the introduction of the superoxide anion (•O2-) significantly lowers the conversion barrier (ΔG = 0.91 eV) of BQ because •O2- can act as the electron donor and acceptor simultaneously, electrophilically and nucleophilically add to BQ synchronously, and break it down. Subsequently, the breakdown products can then be further oxidized by •OH until completely mineralized. Such synergistic oxidation based on •OH and •O2- timely eliminates BQ, potentiates AP mineralization, and inhibits electrode fouling caused by high-resistance polymeric BQ; more importantly, it effectively reduces toxicity, saves energy and costs, and decreases the environmental footprint, evidenced by the life cycle assessment.


Asunto(s)
Radical Hidroxilo , Superóxidos , Oxidación-Reducción , Benzoquinonas/química , Benzoquinonas/metabolismo
16.
Environ Sci Technol ; 57(2): 1134-1143, 2023 01 17.
Artículo en Inglés | MEDLINE | ID: mdl-36602374

RESUMEN

In situ synthesis of reactive oxygen species (ROS) on demand via oxygen activation (OA) is significant in biological, chemical, and environmental fields. Thus, the design of OA catalysts with adequate reactivity, durability, and selectivity is critical but challenging. Here, we report a CuxO@C core@shell photoelectrode prepared by encapsulating Cu/Cu2O/CuO into a carbon layer through anodic electropolymerization (electrophoresis-coupled self-assembly of carbon quantum dots). Theoretical prediction and experiments indicate that the carbon layer can effectively facilitate optical trapping and charge transfer, thus promoting photoelectric conversion and anti-photocorrosion performance of CuxO@C. The inner CuxO core acts as an electron reservoir and continuously injects electrons into the outer carbon layer shell, and the carbon atoms adjacent to oxygen-enriched functional groups (C-O-C and -COOH) in the electron-rich carbon layer work as the reactive sites to adsorb O2 and donate electrons to the antibonding orbital [lowest unoccupied molecular orbital (π*)] of dioxygen. Optimized adsorption and hydrogenation of the critical intermediates (*O2, *OOH, and *H2O2) and thermodynamically tunable O-O bond cleavage enable O2 being selectively reduced to the superoxide anion and hydroxyl radical via the mixed multielectron processes consisting of one- and three-electron pathways. Sulfamethoxazole, an emerging refractory organic contaminant widely present in the environment, can be effectively degraded (∼100% removal) in such an electrochemical platform, benefiting from the abundant ROS generated in situ. Our findings demonstrate an innovative strategy to develop highly efficient and selective OA catalysts for practical water purification.


Asunto(s)
Oxígeno , Purificación del Agua , Especies Reactivas de Oxígeno/química , Peróxido de Hidrógeno/química , Carbono
17.
Environ Sci Technol ; 57(36): 13658-13668, 2023 09 12.
Artículo en Inglés | MEDLINE | ID: mdl-37647171

RESUMEN

Ionic contaminants such as Cr(VI) pose a challenge for water purification using membrane-based processes. However, existing membranes have low permeability and selectivity for Cr(VI). Therefore, in this study, we prepared an electrically controlled adsorptive membrane (ECAM-L) by coating a loose Cl--doped polypyrrole layer on a carbon nanotube substrate, and we evaluated the performance of ECAM-L for Cr(VI) separation from water. We also used electrochemical quartz crystal microbalance measurements and molecular dynamics and density functional theory calculations to investigate the separation mechanisms. The adsorption and desorption of Cr(VI) could be modulated by varying the electrostatic interactions between ECAM-L and Cr(VI) via potential control, enabling the cyclic use of the ECAM-L without additional additives. Consequently, the oxidized ECAM-L showed high Cr(VI) removal performance (<50 µg/L) and treatment capacity (>3500 L/m2) at a high water flux (283 L/m2/h), as well as reusability after the application of a potential. Our study demonstrates an efficient membrane design for water decontamination that can selectively separate Cr(VI) through a short electric stimulus.


Asunto(s)
Polímeros , Pirroles , Adsorción , Agua
18.
Environ Sci Technol ; 57(45): 17640-17648, 2023 11 14.
Artículo en Inglés | MEDLINE | ID: mdl-37906121

RESUMEN

Membrane technology provides an attractive approach for water purification but faces significant challenges in separating small molecules due to its lack of satisfactory permselectivity. In this study, a polypyrrole-based active membrane with a switchable multi-affinity that simultaneously separates small ionic and organic contaminants from water was created. Unlike conventional passive membranes, the designed membrane exhibits a good single-pass filtration efficiency (>99%, taking 1-naphthylamine and Pb2+ as examples) and high permeability (227 L/m2/h). Applying a reversible potential can release the captured substances from the membrane, thus enabling membrane regeneration and self-cleaning without the need for additives. Advanced characterizations reveal that potential switching alters the orientation of the doped amphipathic molecules with the self-alignment of the hydrophobic alkyl chains or the disordered sulfonate anions to capture the target organic molecules or ions via hydrophobic or electrostatic interactions, respectively. The designed smart membrane holds great promise for controllable molecular separation and water purification.


Asunto(s)
Polímeros , Purificación del Agua , Polímeros/química , Pirroles , Filtración , Electricidad , Iones
19.
Environ Sci Technol ; 57(12): 5003-5012, 2023 03 28.
Artículo en Inglés | MEDLINE | ID: mdl-36931868

RESUMEN

The adsorption of contaminants by porous carbon has been extensively studied by conventional isotherm and kinetic methods. However, the co-adsorption behavior and sorption sites of multiple contaminants in different-sized pores remain unclear. Herein, the nuclear magnetic resonance (NMR) approach is performed to investigate the adsorption mechanism of toluene and cetane in the confined space of carbon at the molecular level. The ring current effect induces the variation in the NMR chemical shifts of in-pore adsorbed toluene and cetane, realizing the identification of pore-dependent adsorption sites for contaminant removal. Cetane has a slower adsorption kinetic but a higher binding energy than toluene, which could squeeze toluene from micropores to larger pores with increasing adsorption quantity. This leads to a stronger competitive adsorption effect in small micropores than in mesopores. Accordingly, hierarchical porous carbons are determined to be the most effective adsorbents for the adsorption of coexisting contaminants. This study not only provides an effective NMR method to reveal the adsorption mechanism in the confined space of porous carbon at the molecular level but also offers new insights into the pore size-dependent adsorption of activated carbon for petroleum contaminant treatment.


Asunto(s)
Carbón Orgánico , Tolueno , Tolueno/química , Porosidad , Espectroscopía de Resonancia Magnética , Adsorción , Ácido Ascórbico
20.
Environ Sci Technol ; 57(21): 7913-7923, 2023 05 30.
Artículo en Inglés | MEDLINE | ID: mdl-37188658

RESUMEN

Antiviral transformation products (TPs) generated during wastewater treatment are an environmental concern, as their discharge, in considerable amounts, into natural waters during a pandemic can pose possible risks to the aquatic environment. Identification of the hazardous TPs generated from antivirals during wastewater treatment is important. Herein, chloroquine phosphate (CQP), which was widely used during the coronavirus disease-19 (COVID-19) pandemic, was selected for research. We investigated the TPs generated from CQP during water chlorination. Zebrafish (Danio rerio) embryos were used to assess the developmental toxicity of CQP after water chlorination, and hazardous TPs were estimated using effect-directed analysis (EDA). Principal component analysis revealed that the developmental toxicity induced by chlorinated samples could be relevant to the formation of some halogenated TPs. Fractionation of the hazardous chlorinated sample, along with the bioassay and chemical analysis, identified halogenated TP387 as the main hazardous TP contributing to the developmental toxicity induced by chlorinated samples. TP387 could also be formed in real wastewater during chlorination in environmentally relevant conditions. This study provides a scientific basis for the further assessment of environmental risks of CQP after water chlorination and describes a method for identifying unknown hazardous TPs generated from pharmaceuticals during wastewater treatment.


Asunto(s)
COVID-19 , Contaminantes Químicos del Agua , Animales , Desinfección/métodos , Cloro/análisis , Pez Cebra , Contaminantes Químicos del Agua/toxicidad , Contaminantes Químicos del Agua/análisis , Tratamiento Farmacológico de COVID-19 , Agua
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