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1.
Small ; 20(13): e2308084, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-38243883

RESUMEN

Ammonia is an essential commodity in the food and chemical industry. Despite the energy-intensive nature, the Haber-Bosch process is the only player in ammonia production at large scales. Developing other strategies is highly desirable, as sustainable and decentralized ammonia production is crucial. Electrochemical ammonia production by directly reducing nitrogen and nitrogen-based moieties powered by renewable energy sources holds great potential. However, low ammonia production and selectivity rates hamper its utilization as a large-scale ammonia production process. Creating effective and selective catalysts for the electrochemical generation of ammonia is critical for long-term nitrogen fixation. Single-atom alloys (SAAs) have become a new class of materials with distinctive features that may be able to solve some of the problems with conventional heterogeneous catalysts. The design and optimization of SAAs for electrochemical ammonia generation have recently been significantly advanced. This comprehensive review discusses these advancements from theoretical and experimental research perspectives, offering a fundamental understanding of the development of SAAs for ammonia production.

2.
Environ Sci Technol ; 58(11): 4844-4851, 2024 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-38385614

RESUMEN

This perspective presents the latest advancements in selective polymerization pathways in advanced oxidation processes (AOPs) for removal of featured organic pollutants in wastewater. In radical-based homogeneous reactions, SO4• --based systems exhibit superior oxidative activity toward aromatics with electron-donating substituents via single electron transfer and radical adduct formation (RAF). The produced organic radical cations subsequently undergo coupling and polymerization reactions to produce polymers. For •OH-based oxidation, metal ions facilitate the production of monomer radicals via RAF. Additionally, heterogeneous catalysts can mediate both coupling and polymerization reactions via persulfate activation without generating inorganic radicals. Metal-based catalysts will mediate a direct oxidation pathway toward polymerization. In contrast, carbon-based catalysts will induce coupling reactions to produce low-molecular-weight oligomers (≤4 units) via an electron transfer process. In comparison to mineralization, polymerization pathways remarkably reduce peroxide usage, quickly separate pollutants from the aqueous phase, and generate polymeric byproducts. Thus, AOP-driven polymerization systems hold significant promise in reducing carbon emission and realizing carbon recycling in water treatment processes.


Asunto(s)
Contaminantes Químicos del Agua , Oxidación-Reducción , Carbono , Aguas Residuales , Metales , Polímeros
3.
Environ Sci Technol ; 58(19): 8554-8564, 2024 May 14.
Artículo en Inglés | MEDLINE | ID: mdl-38634679

RESUMEN

Peracetic acid (PAA) oxidation catalyzed by metal-free carbons is promising for advanced water decontamination. Nevertheless, developing reaction-oriented and high-performance carbocatalysts has been limited by the ambiguous understanding of the intrinsic relationship between carbon chemical/molecular structure and PAA transformation behavior. Herein, we comprehensively investigated the PAA activation using a family of well-defined sp2/sp3 carbon hybrids from annealed nanodiamonds (ANDs). The activity of ANDs displays a volcano-type trend, with respect to the sp2/sp3 ratio. Intriguingly, sp3-C-enriched AND exhibits the best catalytic activity for PAA activation and phenolic oxidation, which is different from persulfate chemistry in which the sp2 network normally outperforms sp3 hybridization. At the electron-rich sp2-C site, PAA undergoes a reduction reaction to generate a reactive complex (AND-PAA*) and induces an electron-transfer oxidation pathway. At the sp3-C site adjacent to C═O, PAA is oxidized to surface-confined OH* and O* successively, which ultimately evolves into singlet oxygen (1O2) as the primary reactive species. Benefiting from the dual nonradical regimes on sp2/sp3 hybrids, AND mediates a sustainable redox recycle with PAA to continuously generate reactive species to attack water contaminants, meanwhile maintaining structural/chemical integrity and exceptional reusability in cyclic runs.


Asunto(s)
Ácido Peracético , Ácido Peracético/química , Catálisis , Nanodiamantes/química , Purificación del Agua/métodos , Oxidación-Reducción , Contaminantes Químicos del Agua/química , Agua/química
4.
Proc Natl Acad Sci U S A ; 118(41)2021 10 12.
Artículo en Inglés | MEDLINE | ID: mdl-34620711

RESUMEN

The atrophic form of age-related macular degeneration (dry AMD) affects nearly 200 million people worldwide. There is no Food and Drug Administration (FDA)-approved therapy for this disease, which is the leading cause of irreversible blindness among people over 50 y of age. Vision loss in dry AMD results from degeneration of the retinal pigmented epithelium (RPE). RPE cell death is driven in part by accumulation of Alu RNAs, which are noncoding transcripts of a human retrotransposon. Alu RNA induces RPE degeneration by activating the NLRP3-ASC inflammasome. We report that fluoxetine, an FDA-approved drug for treating clinical depression, binds NLRP3 in silico, in vitro, and in vivo and inhibits activation of the NLRP3-ASC inflammasome and inflammatory cytokine release in RPE cells and macrophages, two critical cell types in dry AMD. We also demonstrate that fluoxetine, unlike several other antidepressant drugs, reduces Alu RNA-induced RPE degeneration in mice. Finally, by analyzing two health insurance databases comprising more than 100 million Americans, we report a reduced hazard of developing dry AMD among patients with depression who were treated with fluoxetine. Collectively, these studies identify fluoxetine as a potential drug-repurposing candidate for dry AMD.


Asunto(s)
Antidepresivos de Segunda Generación/farmacología , Reposicionamiento de Medicamentos/métodos , Fluoxetina/farmacología , Degeneración Macular/tratamiento farmacológico , Proteína con Dominio Pirina 3 de la Familia NLR/antagonistas & inhibidores , Epitelio Pigmentado de la Retina/efectos de los fármacos , Elementos Alu/genética , Animales , Ceguera/patología , Ceguera/prevención & control , Línea Celular , Citocinas/metabolismo , Depresión/tratamiento farmacológico , Modelos Animales de Enfermedad , Inflamasomas/metabolismo , Macrófagos/inmunología , Ratones , Ratones Endogámicos C57BL , ARN/genética , Retina/patología , Epitelio Pigmentado de la Retina/citología , Epitelio Pigmentado de la Retina/patología
5.
Proc Natl Acad Sci U S A ; 118(6)2021 02 09.
Artículo en Inglés | MEDLINE | ID: mdl-33526699

RESUMEN

Alu retroelements propagate via retrotransposition by hijacking long interspersed nuclear element-1 (L1) reverse transcriptase (RT) and endonuclease activities. Reverse transcription of Alu RNA into complementary DNA (cDNA) is presumed to occur exclusively in the nucleus at the genomic integration site. Whether Alu cDNA is synthesized independently of genomic integration is unknown. Alu RNA promotes retinal pigmented epithelium (RPE) death in geographic atrophy, an untreatable type of age-related macular degeneration. We report that Alu RNA-induced RPE degeneration is mediated via cytoplasmic L1-reverse-transcribed Alu cDNA independently of retrotransposition. Alu RNA did not induce cDNA production or RPE degeneration in L1-inhibited animals or human cells. Alu reverse transcription can be initiated in the cytoplasm via self-priming of Alu RNA. In four health insurance databases, use of nucleoside RT inhibitors was associated with reduced risk of developing atrophic macular degeneration (pooled adjusted hazard ratio, 0.616; 95% confidence interval, 0.493-0.770), thus identifying inhibitors of this Alu replication cycle shunt as potential therapies for a major cause of blindness.


Asunto(s)
Elementos Alu/genética , Elementos de Nucleótido Esparcido Largo/genética , Degeneración Macular/genética , Pigmentos Retinianos/metabolismo , Animales , Citoplasma/genética , ADN Complementario/genética , Epitelio/metabolismo , Epitelio/patología , Humanos , Degeneración Macular/patología , Pigmentos Retinianos/biosíntesis , Retroelementos/genética , Transcripción Reversa/genética
6.
Small ; 19(41): e2302875, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37309270

RESUMEN

Due to the depletion of fossil fuels and their-related environmental issues, sustainable, clean, and renewable energy is urgently needed to replace fossil fuel as the primary energy resource. Hydrogen is considered as one of the cleanest energies. Among the approaches to hydrogen production, photocatalysis is the most sustainable and renewable solar energy technique. Considering the low cost of fabrication, earth abundance, appropriate bandgap, and high performance, carbon nitride has attracted extensive attention as the catalyst for photocatalytic hydrogen production in the last two decades. In this review, the carbon nitride-based photocatalytic hydrogen production system, including the catalytic mechanism and the strategies for improving the photocatalytic performance is discussed. According to the photocatalytic processes, the strengthened mechanism of carbon nitride-based catalysts is particularly described in terms of boosting the excitation of electrons and holes, suppressing carriers recombination, and enhancing the utilization efficiency of photon-excited electron-hole. Finally, the current trends related to the screening design of superior photocatalytic hydrogen production systems are outlined, and the development direction of carbon nitride for hydrogen production is clarified.

7.
Small ; 19(23): e2207666, 2023 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-36703516

RESUMEN

H2 O2 -fueled micromotors are state-of-the-art mobile microreactors in environmental remediation. In this work, a magnetic FeOx @MnO2 @SiO2 micromotor with multi-functions is designed and demonstrated its catalytic performance in H2 O2 /peroxymonosulfate (PMS) activation for simultaneously sustained motion and organic degradation. Moreover, this work reveals the correlations between catalytic efficiency and motion behavior/mechanism. The inner magnetic FeOx nanoellipsoids primarily trigger radical species (• OH and O2 •- ) to attack organics via Fenton-like reactions. The coated MnO2 layers on FeOx surface are responsible for decomposing H2 O2 into O2 bubbles to provide a propelling torque in the solution and generating SO4 •- and • OH for organic degradation. The outer SiO2 microcapsules with a hollow head and tail result in an asymmetrical Janus structure for the motion, driven by O2 bubbles ejecting from the inner cavity via the opening tail. Intriguingly, PMS adjusts the local environment to control over-violent O2 formation from H2 O2 decomposition by occupying the Mn sites via inter-sphere interactions and enhances organic removal due to the strengthened contacts and Fenton-like reactions between inner FeOx and peroxides within the microreactor. The findings will advance the design of functional micromotors and the knowledge of micromotor-based remediation with controlled motion and high-efficiency oxidation using multiple peroxides.

8.
Blood ; 138(3): 259-272, 2021 07 22.
Artículo en Inglés | MEDLINE | ID: mdl-33827130

RESUMEN

Acetaminophen (APAP)-induced liver injury is associated with activation of coagulation and fibrinolysis. In mice, both tissue factor-dependent thrombin generation and plasmin activity have been shown to promote liver injury after APAP overdose. However, the contribution of the contact and intrinsic coagulation pathways has not been investigated in this model. Mice deficient in individual factors of the contact (factor XII [FXII] and prekallikrein) or intrinsic coagulation (FXI) pathway were administered a hepatotoxic dose of 400 mg/kg of APAP. Neither FXII, FXI, nor prekallikrein deficiency mitigated coagulation activation or hepatocellular injury. Interestingly, despite the lack of significant changes to APAP-induced coagulation activation, markers of liver injury and inflammation were significantly reduced in APAP-challenged high-molecular-weight kininogen-deficient (HK-/-) mice. Protective effects of HK deficiency were not reproduced by inhibition of bradykinin-mediated signaling, whereas reconstitution of circulating levels of HK in HK-/- mice restored hepatotoxicity. Fibrinolysis activation was observed in mice after APAP administration. Western blotting, enzyme-linked immunosorbent assay, and mass spectrometry analysis showed that plasmin efficiently cleaves HK into multiple fragments in buffer or plasma. Importantly, plasminogen deficiency attenuated APAP-induced liver injury and prevented HK cleavage in the injured liver. Finally, enhanced plasmin generation and HK cleavage, in the absence of contact pathway activation, were observed in plasma of patients with acute liver failure due to APAP overdose. In summary, extrinsic but not intrinsic pathway activation drives the thromboinflammatory pathology associated with APAP-induced liver injury in mice. Furthermore, plasmin-mediated cleavage of HK contributes to hepatotoxicity in APAP-challenged mice independently of thrombin generation or bradykinin signaling.


Asunto(s)
Acetaminofén/efectos adversos , Enfermedad Hepática Inducida por Sustancias y Drogas/metabolismo , Fibrinolisina/metabolismo , Fibrinólisis/efectos de los fármacos , Quininógenos/metabolismo , Proteolisis/efectos de los fármacos , Acetaminofén/farmacología , Animales , Enfermedad Hepática Inducida por Sustancias y Drogas/genética , Enfermedad Hepática Inducida por Sustancias y Drogas/patología , Factor XII/genética , Factor XII/metabolismo , Femenino , Fibrinolisina/genética , Humanos , Quininógenos/genética , Masculino , Ratones , Ratones Noqueados , Precalicreína/genética , Precalicreína/metabolismo
9.
Environ Sci Technol ; 57(32): 12094-12104, 2023 08 15.
Artículo en Inglés | MEDLINE | ID: mdl-37490389

RESUMEN

In this study, Ru(III) ions were utilized to activate periodate (PI) for oxidation of trace organic pollutants (TOPs, e.g., carbamazepine (CBZ)). The Ru(III)/PI system can significantly promote the oxidation of CBZ in a wide initial pH range (3.0-11.0) at 1 µM Ru(III), showing much higher performance than transition metal ions (i.e., Fe(II), Co(II), Zn(II), Fe(III), Cu(II), Ni(II), Mn(II), and Ce(III)) and noble metal ion (i.e., Ag(I), Pd(II), Pt(II), and Ir(III)) activated PI systems. Probe experiments, UV-vis spectra, and X-ray absorption near-edge structure (XANES) spectra confirmed high-valent Ru-oxo species (Ru(V)=O) as the dominant oxidant in the process. Because of the dominant role of Ru(V)=O, the Ru(III)/PI process exhibited a remarkable selectivity and strong anti-interference in the oxidation of TOPs in complex water matrices. The Ru(V)=O species can undertake 1-e- and 2-e- transfer reactions via the catalytic cycles of Ru(V)=O → Ru(IV) → Ru(III) and Ru(V)=O → Ru(III), respectively. The utilization efficiency of PI in the Ru(III)/PI process for the oxidation of TOPs can approach 100% under optimal conditions. PI stoichiometrically transformed into IO3- without production of undesired iodine species (e.g., HOI and I2). This study developed an efficient and environmentally benign advanced oxidation process for rapid removal of TOPs and enriched understandings on reactivity of Ru(V)=O and Ru catalytic cycles.


Asunto(s)
Contaminantes Ambientales , Compuestos Férricos , Metales , Oxidación-Reducción , Agua/química
10.
Environ Sci Technol ; 57(8): 3334-3344, 2023 02 28.
Artículo en Inglés | MEDLINE | ID: mdl-36734031

RESUMEN

Accelerating the rate-limiting Fe3+/Fe2+ circulation in Fenton reactions through the addition of reducing agents (or co-catalysts) stands out as one of the most promising technologies for rapid water decontamination. However, conventional reducing agents such as hydroxylamine and metal sulfides are greatly restricted by three intractable challenges: (1) self-quenching effects, (2) heavy metal dissolution, and (3) irreversible capacity decline. To this end, we, for the first time, introduced redox-active polymers as electron shuttles to expedite the Fe3+/Fe2+ cycle and promote H2O2 activation. The reduction of Fe3+ mainly took place at active N-H or O-H bonds through a proton-coupled electron transfer process. As electron carriers, H atoms at the solid phase could effectively inhibit radical quenching, avoid metal dissolution, and maintain long-term reducing capacity via facile regeneration. Experimental and density functional theory (DFT) calculation results indicated that the activity of different polymers shows a volcano curve trend as a function of the energy barrier, highest occupied molecular orbital-lowest unoccupied molecular orbital (HOMO-LUMO) gap, and vertical ionization potential. Thanks to the appropriate redox ability, polyaniline outperforms other redox-active polymers (e.g., poypyrrole, hydroquinone resin, poly(2,6-diaminopyridine), and hexaazatrinaphthalene framework) with a highest iron reduction capacity up to 5.5 mmol/g, which corresponds to the state transformation from leucoemeraldine to emeraldine. Moreover, the proposed system exhibited high pollutant removal efficiency in a flow-through reactor for 8000 bed volumes without an obvious decline in performance. Overall, this work established a green and sustainable oxidation system, which offers great potential for practical organic wastewater remediation.


Asunto(s)
Peróxido de Hidrógeno , Hierro , Hierro/química , Peróxido de Hidrógeno/química , Sustancias Reductoras , Electrones , Oxidación-Reducción
11.
J Digit Imaging ; 36(4): 1782-1793, 2023 08.
Artículo en Inglés | MEDLINE | ID: mdl-37259008

RESUMEN

The objective of this study is to analyse the diffusion rule of the contrast media in multi-phase delayed enhanced magnetic resonance (MR) T1 images using radiomics and to construct an automatic classification and segmentation model of brain metastases (BM) based on support vector machine (SVM) and Dpn-UNet. A total of 189 BM patients with 1047 metastases were enrolled. Contrast-enhanced MR images were obtained at 1, 3, 5, 10, 18, and 20 min following contrast medium injection. The tumour target volume was delineated, and the radiomics features were extracted and analysed. BM segmentation and classification models in the MR images with different enhancement phases were constructed using Dpn-UNet and SVM, and differences in the BM segmentation and classification models with different enhancement times were compared. (1) The signal intensity for BM decreased with time delay and peaked at 3 min. (2) Among the 144 optimal radiomics features, 22 showed strong correlation with time (highest R-value = 0.82), while 41 showed strong correlation with volume (highest R-value = 0.99). (3) The average dice similarity coefficients of both the training and test sets were the highest at 10 min for the automatic segmentation of BM, reaching 0.92 and 0.82, respectively. (4) The areas under the curve (AUCs) for the classification of BM pathology type applying single-phase MRI was the highest at 10 min, reaching 0.674. The AUC for the classification of BM by applying the six-phase image combination was the highest, reaching 0.9596, and improved by 42.3% compared with that by applying single-phase images at 10 min. The dynamic changes of contrast media diffusion in BM can be reflected by multi-phase delayed enhancement based on radiomics, which can more objectively reflect the pathological types and significantly improve the accuracy of BM segmentation and classification.


Asunto(s)
Neoplasias Encefálicas , Medios de Contraste , Humanos , Imagen por Resonancia Magnética/métodos , Neoplasias Encefálicas/diagnóstico por imagen , Neoplasias Encefálicas/patología , Máquina de Vectores de Soporte , Estudios Retrospectivos
12.
Angew Chem Int Ed Engl ; 62(30): e202305639, 2023 Jul 24.
Artículo en Inglés | MEDLINE | ID: mdl-37254229

RESUMEN

In photosynthesis, solar energy is harvested by photosensitizers, and then, the excited electrons transfer via a Z-Scheme mode to enzymatic catalytic centers to trigger redox reactions. Herein, we constructed a core-shell Z-scheme heterojunction of semiconductor@single-atom catalysts (SACs). The oxygen-vacancy-rich ZnO core and single-atom Co-N4 sites supported on nitrogen-rich carbon shell (SA-Co-CN) act as the photosensitizer and the enzyme-mimicking active centers, respectively. Driven by built-in electric field across the heterojunction, photoexcited electrons could rapidly (2 ps) transfer from the n-type ZnO core to the p-type SA-Co-CN shell, finally boosting the catalytic performance of the surface-exposed single-atom Co-N4 sites for peroxymonosulfate (PMS) activation under light irradiation. The synergies between photocatalysis and heterogeneous Fenton-like reaction lead to phenomenally enhanced production of various reactive oxygen species for rapid degradation of various microcontaminants in water. Experimental and theoretical results validate that the interfacial coupling of SA-Co-CN with ZnO greatly facilitates PMS adsorption and activation by reducing the adsorption energy and enhancing the cascade electron transfer processes for the photo-Fenton-like reaction.

13.
J Cell Mol Med ; 26(3): 840-854, 2022 02.
Artículo en Inglés | MEDLINE | ID: mdl-34970843

RESUMEN

At present, liver fibrosis is a major challenge of global health. When hepatocyte regeneration cannot compensate for hepatocyte death, it will develop into liver fibrosis in chronic liver disease. Initially, collagen produced by myofibroblasts plays a role in maintaining liver integrity, but excessive collagen accumulation can inhibit the residual liver function, leading to liver failure. At present, many scientists are actively looking for drugs to alleviate liver fibrosis. In the current study, we investigated the potential role of uridine in the treatment of liver fibrosis (uridine is a plant/animal-derived pyrimidine nucleoside, therefore uridine can also be ingested and absorbed by the body, accompanied by the process of food intake). For this, we systematically studied the effect of uridine on CCl4-induced liver fibrosis in vitro and in vivo through a series of technologies, such as Western blot, laser confocal scanning microscope, ELISA and immunohistochemistry. The experimental results showed that uridine can effectively reduce the accumulation of collagen in liver. Furthermore, uridine can improve the activity of liver cells and alleviate CCl4-induced liver injury. Furthermore, uridine can significantly alleviate the risk factors caused by hepatic stellate cell activation, uridine treatment significantly down-regulated the expression of α-SMA, collagen type-I and fibronectin. In conclusion, the current research shows that uridine can alleviate CCl4-induced liver fibrosis, suggesting that uridine can be used as a potential drug to alleviate liver fibrosis.


Asunto(s)
Tetracloruro de Carbono , Células Estrelladas Hepáticas , Animales , Tetracloruro de Carbono/efectos adversos , Células Estrelladas Hepáticas/metabolismo , Hepatocitos/metabolismo , Hígado/metabolismo , Cirrosis Hepática/inducido químicamente , Cirrosis Hepática/tratamiento farmacológico , Cirrosis Hepática/metabolismo , Uridina/metabolismo , Uridina/farmacología , Uridina/uso terapéutico
14.
Funct Integr Genomics ; 22(4): 643-653, 2022 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-35451652

RESUMEN

The detailed regulatory mechanism of LINC00174 in lung cancer (LC) development remains largely unknown. This research was designed to probe into the impacts of LINC00174 in LC cells through modulating the microRNA (miR)-584-3p/ribosomal protein S24 (RPS24) axis. LINC00174, miR-584-3p, and RPS24 expression levels in LC cells and tissues were examined. The constructs altering LINC00174, miR-584-3p, or RPS24 expression were transfected into LC cells to examine the malignant phenotypes of LC cells. The relations among LINC00174, miR-584-3p, and RPS24 were validated. LINC00174 and RPS24 were high-expressed while miR-584-3p was low-expressed in LC. Downregulated LINC00174 or RPS24 or upregulated miR-584-3p inhibited the malignant biological behaviors of LC cells. The silenced miR-584-3p could reverse the repressive effects of reduced LINC00174 on the development of LC cells; while RPS24 overexpression inverted the repressive effects of miR-584-3p elevation on LC cells. Mechanically, LINC00174 bound to miR-584-3p that targeted RPS24. Repressed LINC00174 can relieve the malignant phenotypes of LC cells via modulating the miR-584-3p/RPS24 axis.


Asunto(s)
Neoplasias Pulmonares , MicroARNs , ARN Largo no Codificante , Proteínas Ribosómicas , Línea Celular Tumoral , Movimiento Celular , Proliferación Celular , Regulación Neoplásica de la Expresión Génica , Humanos , Neoplasias Pulmonares/genética , Neoplasias Pulmonares/patología , MicroARNs/genética , ARN Largo no Codificante/genética , Proteínas Ribosómicas/genética
15.
Blood ; 135(20): 1783-1787, 2020 05 14.
Artículo en Inglés | MEDLINE | ID: mdl-31977004

RESUMEN

Vaso-occlusive crisis (VOC) is the primary cause of morbidity and hospitalization in sickle cell disease (SCD); however, only 4 therapies (hydroxyurea, l-glutamine, crizanlizumab, and voxeletor) are currently approved in SCD. These agents limit the duration, severity, and frequency of crises. Activation of coagulation is a hallmark of SCD. Studies in animal models of SCD have shown that coagulation contributes to the chronic inflammation and end-organ damage associated with the disease; however, it is unknown whether coagulation directly contributes to the microvascular stasis that causes VOC. Herein, we demonstrate that inhibition of tissue factor (TF) and the downstream coagulation proteases factor Xa and thrombin significantly attenuates heme-induced microvascular stasis in mouse models of VOC. Pharmacologic inhibition of the principal thrombin receptor, protease activated receptor-1 (PAR-1), as well as deficiency of PAR-1 in all nonhematopoietic cells, also reduces stasis in sickle mice. PAR-1 deficiency was associated with reduced endothelial von Willebrand factor expression, which has been shown to mediate microvascular stasis. In addition, TF inhibition reduces lung vaso-occlusion in sickle mice mediated by arteriolar neutrophil-platelet microemboli. In sum, these results suggest that prophylactic anticoagulation might attenuate the incidence of VOC.


Asunto(s)
Anemia de Células Falciformes/metabolismo , Trastornos de la Coagulación Sanguínea/etiología , Receptor PAR-1/metabolismo , Trombina/metabolismo , Anemia de Células Falciformes/complicaciones , Anemia de Células Falciformes/genética , Anemia de Células Falciformes/patología , Animales , Trastornos de la Coagulación Sanguínea/genética , Trastornos de la Coagulación Sanguínea/metabolismo , Plaquetas/metabolismo , Constricción Patológica/genética , Constricción Patológica/metabolismo , Modelos Animales de Enfermedad , Femenino , Hemoglobina Falciforme/genética , Humanos , Masculino , Ratones , Ratones Transgénicos , Microvasos/metabolismo , Microvasos/patología , Receptor PAR-1/genética , Enfermedades Vasculares/etiología , Enfermedades Vasculares/metabolismo
16.
Environ Sci Technol ; 56(1): 78-97, 2022 01 04.
Artículo en Inglés | MEDLINE | ID: mdl-34932343

RESUMEN

Persulfate-based nonradical oxidation processes (PS-NOPs) are appealing in wastewater purification due to their high efficiency and selectivity for removing trace organic contaminants in complicated water matrices. In this review, we showcased the recent progresses of state-of-the-art strategies in the nonradical electron-transfer regimes in PS-NOPs, including design of metal and metal-free heterogeneous catalysts, in situ/operando characterization/analytical techniques, and insights into the origins of electron-transfer mechanisms. In a typical electron-transfer process (ETP), persulfate is activated by a catalyst to form surface activated complexes, which directly or indirectly interact with target pollutants to finalize the oxidation. We discussed different analytical techniques on the fundamentals and tactics for accurate analysis of ETP. Moreover, we demonstrated the challenges and proposed future research strategies for ETP-based systems, such as computation-enabled molecular-level investigations, rational design of catalysts, and real-scenario applications in the complicated water environment. Overall, this review dedicates to sharpening the understanding of ETP in PS-NOPs and presenting promising applications in remediation technology and green chemistry.


Asunto(s)
Contaminantes Químicos del Agua , Purificación del Agua , Catálisis , Transporte de Electrón , Electrones , Oxidación-Reducción , Contaminantes Químicos del Agua/análisis
17.
Environ Sci Technol ; 56(19): 14019-14029, 2022 10 04.
Artículo en Inglés | MEDLINE | ID: mdl-36062466

RESUMEN

In electrochemical advanced oxidation processes (EAOPs), the rate-limiting step is the mass transfer of pollutants to the electrodes due to the limited active surface areas. To this end, we established a three-dimensional (3D) EAOP system by coupling conventional graphite electrodes with dispersed carbon nanotubes (CNTs). The electrodes (particularly the anode) induced electric field spontaneously polarized CNTs into dispersed reactive particle electrodes (CNT-PEs) in the solution, which remarkably promoted electrochemical activation of peroxydisulfate (PDS) to generate surface CNT-PDS* complexes and surface-bound radicals (SBRs). Based on the excited potential (ECNT-PEs) at different positions in the 3D electric field, CNT-PEs were activated into three states. (i) ECNT-PEs < Eorganic, CNT-PEs are chemically inert toward DCP oxidation; (ii) Eorganic < ECNT-PEs < Ewater, CNT-PEs will oxidize DCP via an electron-transfer process (ETP); (iii) ECNT-PEs > Ewater, both CNT-PDS* complexes and the anode will oxidize water to produce SBRs. Thus, DCP could be oxidized by CNT-PDS* complexes via ETP to form polychlorophenols on the CNT surface, causing rapid deactivation of the micro-electrodes. In contrast, SBRs attack DCP directly into chloride ions and hydroxylated products, maintaining the surface cleanliness and activity of CNT-PEs for long-term operations.


Asunto(s)
Contaminantes Ambientales , Grafito , Nanotubos de Carbono , Cloruros , Electrodos , Nanotubos de Carbono/química , Oxidación-Reducción , Agua
18.
Environ Sci Technol ; 56(19): 13996-14007, 2022 10 04.
Artículo en Inglés | MEDLINE | ID: mdl-36083161

RESUMEN

In this study, a wet scrubber coupled with a persulfate-based advanced oxidation process [carbocatalysts/peroxymonosulfate (PMS)] was demonstrated to efficiently remove gaseous volatile organic compounds (VOCs). The removal efficiency of a representative VOC, styrene, was stable at above 98%, and an average mineralization rate was achieved at 76% during 2 h. The removal efficiency of the carbocatalysts/PMS wet scrubber for styrene was much higher than that of pure water, carbocatalysts/water, or PMS/water systems. Quenching experiments, electron spin resonance spectroscopy, in-situ Raman spectroscopy and density functional theory (DFT) calculations indicated that singlet oxygen (1O2) and oxidative complexes are the main reactive oxygen species and that both contributed to styrene removal. In particular, carbonyl groups (C═O) in the carbocatalyst were found to be the active sites for activating PMS during styrene oxidation. The role of 1O2 was discovered to be benzene ring breaking and a possible non-radical oxidation pathway of styrene was proposed based on time-of-flight mass spectroscopy which was further verified by DFT calculations. In particular, the electron transfer process of multi world carbon nanotubes-PMS* in styrene oxidation was further studied in-depth by experiments and DFT calculations. The unstable vinyl on styrene was simultaneously degraded by the oxidative complexes and 1O2 into benzene, and finally oxidized by 1O2 into H2O and CO2. This study provides an effective method for VOC removal and clearly illustrates the complete degradation mechanism of styrene in a nonradical PMS-based process by a wet scrubber.


Asunto(s)
Nanotubos de Carbono , Compuestos Orgánicos Volátiles , Benceno , Dióxido de Carbono , Gases , Peróxidos/química , Especies Reactivas de Oxígeno , Oxígeno Singlete , Estirenos , Agua
19.
Int J Equity Health ; 21(1): 107, 2022 08 13.
Artículo en Inglés | MEDLINE | ID: mdl-35964119

RESUMEN

BACKGROUND: China now faces an increasingly aging society which may exert economic pressure in the long run. This study illustrates the spatial pattern and evolution of population aging and economic development in China. The coupling coordination degree of population aging and economic development at the national and provincial levels are calculated and demonstrated, and the spatial patterns and characteristics are investigated. METHODS: This paper presents a coupling analysis of the elderly population rate (EPR) and per capita Gross Regional Product (GRPpc) in China by using the coupling and coordination model. Further, the spatial pattern and evolution of population aging and economic development are investigated based on the standard deviational ellipse. The collected data is at the level of provincial administrative units in mainland China covering the period 2002 to 2020. RESULTS: The results reveal the spatial difference in the coupling and coordination degree between EPR and GRPpc across provinces. The eastern coastal areas are higher than the central and western regions of China. The orientation and directions of EPR are more than GRPpc, indicating that the polarization in population aging is more severe than economic development. Significant positive correlations between coupling coordination degree and sustainable competitiveness are detected. CONCLUSIONS: Policymakers should fully consider regional differences and sustainable development in policy formulation of China. The western and northeastern provinces should be given priority in the regional sustainable development plan. At the same time, the coordination between population aging and economic development also requires to be examined especially.


Asunto(s)
Envejecimiento , Desarrollo Económico , Anciano , China , Humanos
20.
Environ Res ; 204(Pt D): 112368, 2022 03.
Artículo en Inglés | MEDLINE | ID: mdl-34774832

RESUMEN

Developing novel heterojunction photocatalysts with visible-light response and remarkable photocatalytic activity have been verified to applying for the photodegradation of antibiotics in water environment. Herein, NH2-MIL-125(Ti) was integrated with flowerlike ZnIn2S4 to construct NH2-MIL-125(Ti)@ZnIn2S4 heterostructure using a one-pot solvothermal method. The photocatalytic performance was evaluated by the degradation of tetracycline (TC) under visible light illumination. The optimized NM(2%)@ZIS possesses a photodegradation rate (92.8%) and TOC removal efficiency (58.5%) superior to pristine components, which can be principally attributed to the positive cooperative effects of well-matched energy level positions, strong visible-light-harvesting capacity, and abundant coupling interfaces between the two. Moreover, the probable TC degradation mechanism was also clarified using the active species trapping experiments. This study inspires further design and construction of NH2-MIL-125(Ti) and ZnIn2S4 based photocatalysts for effective removal of antibiotics in water environment.


Asunto(s)
Luz , Titanio , Catálisis , Tetraciclina , Titanio/química
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