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1.
Water Res ; 259: 121835, 2024 Aug 01.
Artículo en Inglés | MEDLINE | ID: mdl-38810345

RESUMEN

Simultaneous removal of heavy metals and organic contaminants remains a substantial challenge in the electro-Fenton (EF) system. Herein, we propose a facile and sustainable "iron-free" EF system capable of simultaneously removing hexavalent chromium (Cr (VI)) and para-chlorophenol (4-CP). The system comprises a nitrogen-doped and carbon-deficient porous carbon (dual-site NPC-D) cathode coupled with a MoS2 nanoarray promoter (MoS2 NA). The NPC-D/MoS2 NA system exhibits exceptional synergistic electrocatalytic activity, with removal rates for Cr (VI) and 4-CP that are 20.3 and 4.4 times faster, respectively, compared to the NPC-D system. Mechanistic studies show that the dual-site structure of NPC-D cathode favors the two-electron oxygen reduction pathway with a selectivity of 81 %. Furthermore, an electric field-driven uncoordinated Mo valence state conversion of MoS2 NA enchances the generation of dynamic singlet oxygen and hydroxyl radicals. Notably, this system shows outstanding recyclability, resilience in real wastewater, and sustainability during a 3 L scale-up operation, while effectively mitigating toxicity. Overall, this study presents an effective approach for treating multiple-component wastewater and highlights the importance of structure-activity correlation in synergistic electrocatalysis.


Asunto(s)
Carbono , Cromo , Electrodos , Molibdeno , Contaminantes Químicos del Agua , Molibdeno/química , Cromo/química , Carbono/química , Contaminantes Químicos del Agua/química , Porosidad , Hierro/química , Peróxido de Hidrógeno/química , Oxidación-Reducción , Aguas Residuales/química
2.
Sci Total Environ ; 927: 172300, 2024 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-38593873

RESUMEN

The decomposition of ammonia-N to environmental-friendly N2 remains a fundamental problem for water treatment. We proposed a way to selectively and efficiently oxidize ammonia to N2 through an integrated photoeletrocatalysis­chlorine reactions (PECCl) system based on a bifunctional TiO2 nanotube photoanode. The ·OH and HClO can be simultaneously generated on the TiO2 nanotube photoanode in this system, which can in situ form ClO· for efficient ammonia removal. Compared with electrochemical­chlorine (EC-Cl), photocatalysis­chlorine (PC-Cl) and photoelectrocatalysis (PEC) systems, the PEC-Cl system exhibited much higher electrocatalytic activity due to the synergetic effect of photoelectrocatalyst and electrocatalyst in bifunctional TiO2 nanotube electrode. The removal efficiency of ammonia-N and total-N reached 100.0 % and 93.3 % at 0.3 V (vs Ag/AgCl) in the PEC-Cl system. Moreover, the system was efficient under various pH conditions. The reactions between ClO-/ClO· and the N-containing intermediates contributed to the high performance of the system, which expanded the reactions from the electrode surface to the electrolyte. Furthermore, radical scavenging and free chlorine determination experiments confirmed that ClO· and free chlorine were the main active species that enabled the ammonia oxidation. This study presents new understanding on the role of active species for ammonia removal in wastewater.

3.
J Hazard Mater ; 471: 134354, 2024 Jun 05.
Artículo en Inglés | MEDLINE | ID: mdl-38653134

RESUMEN

Excessive discharge of nitrogen-containing chemical products into the natural water environment leads to the serious environmental problem of nitrate-nitrogen pollution, threatening the ecological balance and human health. In this study, we propose an efficient denitrification electrochemical method utilizing iron-doped zeolite imidazolium framework derived defective nitrogen-doped carbon (d-FeNC) catalysts. The d-FeNC catalyst exhibited 97 % nitrate removal efficiency and 94 % total nitrogen (TN) removal, and the reaction rate constant was increased from 0.73 h-1 of the Fe-undoped electrocatalyst (d-NC) to 1.11 h-1. The successful synthesis of d-FeNC with carbon defect sites and encapsulated Fe was confirmed by in-depth characterization. In situ electron paramagnetic resonance (EPR) analysis in conjunction with cyclic voltammetry (CV) tests confirmed the carbon substrates with defect enhanced the trapping of atomic hydrogen (H*) on the catalyst surface. Density functional theory (DFT) calculations clarified the doping of Fe facilitated the adsorption of nitrate, resulting in contact of H* with nitrate on the catalyst surface. In the synergy of the defective state organic framework and metal Fe, H* and nitrate realized a collision process. The electrochemical denitrification system achieved an excellent nitrate removal capacity of 7587 mgN·g-1cat in high-concentration nitrate solution and showed excellent stability under various conditions. Overall, this study underscores the potential of defective iron-doped carbon catalysts for efficient electrocatalytic denitrification, providing a promising approach for sustainable wastewater treatment.

4.
Phytomedicine ; 128: 155380, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38507854

RESUMEN

BACKGROUND: Spinal cord injury (SCI) is a traumatic injury to the central nervous system and can cause lipid peroxidation in the spinal cord. Ferroptosis, an iron-dependent programmed cell death, plays a key role in the pathophysiology progression of SCI. Celastrol, a widely used antioxidant drug, has potential therapeutic value for nervous system. PURPOSE: To investigate whether celastrol can be a reliable candidate for ferroptosis inhibitor and the molecular mechanism of celastrol in repairing SCI by inhibiting ferroptosis. METHODS: First, a rat SCI model was constructed, and the recovery of motor function was observed after treatment with celastrol. The regulatory effect of celastrol on ferroptosis pathway Nrf2-xCT-GPX4 was detected by Western blot and immunofluorescence. Finally, the ferroptosis model of neurons and oligodendrocytes was constructed in vitro to further verify the mechanism of inhibiting ferroptosis by celastrol. RESULTS: Our results demonstrated that celastrol promoted the recovery of spinal cord tissue and motor function in SCI rats. Further in vitro and in vivo studies showed that celastrol significantly inhibited ferroptosis in neurons and oligodendrocytes and reduced the accumulation of ROS. Finally, we found that celastrol could inhibit ferroptosis by up-regulating the Nrf2-xCT-GPX4 axis to repair SCI. CONCLUSION: Celastrol effectively inhibits ferroptosis after SCI by upregulating the Nrf2-xCT-GPX4 axis, reducing the production of lipid ROS, protecting the survival of neurons and oligodendrocytes, and improving the functional recovery.


Asunto(s)
Ferroptosis , Neuronas , Oligodendroglía , Triterpenos Pentacíclicos , Ratas Sprague-Dawley , Traumatismos de la Médula Espinal , Triterpenos , Ferroptosis/efectos de los fármacos , Animales , Traumatismos de la Médula Espinal/tratamiento farmacológico , Triterpenos Pentacíclicos/farmacología , Oligodendroglía/efectos de los fármacos , Neuronas/efectos de los fármacos , Ratas , Triterpenos/farmacología , Masculino , Factor 2 Relacionado con NF-E2/metabolismo , Modelos Animales de Enfermedad , Especies Reactivas de Oxígeno/metabolismo , Médula Espinal/efectos de los fármacos , Recuperación de la Función/efectos de los fármacos
5.
Small ; 20(9): e2308070, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-37849040

RESUMEN

Short-wavelength infrared photodetectors play a significant role in various fields such as autonomous driving, military security, and biological medicine. However, state-of-the-art short-wavelength infrared photodetectors, such as InGaAs, require high-temperature fabrication and heterogenous integration with complementary metal-oxide-semiconductor (CMOS) readout circuits (ROIC), resulting in a high cost and low imaging resolution. Herein, for the first time, a low-cost, high-performance, high-stable, and thin-film transistor (TFT) ROIC monolithic-integrated (Bi,Sb)2 Se3 alloy thin-film short-wavelength infrared photodetector is reported. The (Bi,Sb)2 Se3 alloy thin-film short-wavelength infrared photodetectors demonstrate a high external quantum efficiency (EQE) of 21.1% (light intensity of 0.76 µW cm-2 ) and a fast response time (3.24 µs). The highest EQE is about two magnitudes than that of the extrinsic photoconduction of Sb2 Se3 (0.051%). In addition, the unpackaged devices demonstrate high electric and thermal stability (almost no attenuation at 120 °C for 312 h), showing potential for in-vehicle applications that may experient such a high temperature. Finally, both the (Bi,Sb)2 Se3 alloy thin film and n-type CdSe buffer layer are directly deposited on the TFT ROIC (with a 64 × 64-pixel array) with a low-temperature process and the material identification and imaging applications are presented. This work is a significant breakthrough in ROIC monolithic-integrated short-wavelength infrared imaging chips.

6.
Heliyon ; 9(9): e20024, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37809922

RESUMEN

Spinal cord injury (SCI) is a highly complex neurological disease, but there is no effective repair method. Quercetin is a flavonol drug and has a variety of biological activities, such as scavenging oxygen free radicals in the body to resist oxidation, inhibiting inflammation, and so on. In this study, quercetin was firstly demonstrated to reduce tissue damage, promote neuron survival and repair motor function after SCI in rats through in vivo experiments. Then, 293 potential targets of quercetin repair for SCI were predicted by network pharmacology. GO analysis revealed that the biological processes of potential targets focused mainly on signal transduction, negative regulation of the apoptotic process, protein phosphorylation, drug response, and so on. Similarly, KEGG analysis suggested that these potential targets were involved in cell growth regulation, differentiation, apoptosis, and a few metabolic pathways. PPI network analysis predicted that the key genes were EP300, CREBBP, SRC, HSP90AA1, TP53, PIK3R1, EGFR, ESR1, and CBL. Further, the molecular docking showed that quercetin binds well with these proteins. Finally, RT-qPCR and Western blotting experiments verified that quercetin downregulated the expression levels of PIK3R1 and EGFR. It is suggested that quercetin can repair SCI in rats through PI3K-AKT signaling pathway and EGFR/MAPK pathway, which may provide a new theoretical basis for the repair of spinal cord injury.

7.
Biomed Pharmacother ; 165: 115250, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37531781

RESUMEN

Spinal cord injury (SCI) is a debilitating condition that results in significant impairment of motor function and sensation. Despite the ongoing efforts to develop effective treatments, there are currently very limited options available for patients with SCI. Celastrol, a natural anti-inflammatory compound extracted from Tripterygium wilfordii, has been shown to exhibit anti-inflammatory and anti-apoptotic properties. In this study, we aimed to explore the therapeutic potential of celastrol for SCI and elucidate the underlying molecular mechanisms involved. We found that local tissue often experiences a significant decrease in cAMP content and occurrs apoptosis after SCI. However, the treatment of celastrol could promote the production of cAMP by up-regulating the VIP-ADCYAP1R1-GNAS pathway. This could effectively inhibit the phosphorylation of JNK and prevent apoptosis, ultimately improving the exercise ability after SCI. Together, our results reveal celastrol may be a promising therapeutic agent for the treatment of SCI.


Asunto(s)
Traumatismos de la Médula Espinal , Triterpenos , Antiinflamatorios/farmacología , Apoptosis , Cromograninas/farmacología , Cromograninas/uso terapéutico , Subunidades alfa de la Proteína de Unión al GTP Gs/farmacología , Subunidades alfa de la Proteína de Unión al GTP Gs/uso terapéutico , Triterpenos Pentacíclicos/farmacología , Receptores del Polipéptido Activador de la Adenilato-Ciclasa Hipofisaria , Médula Espinal , Traumatismos de la Médula Espinal/tratamiento farmacológico , Triterpenos/farmacología , Triterpenos/uso terapéutico , Animales
8.
Chem Asian J ; 18(11): e202300202, 2023 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-37129348

RESUMEN

Eutrophication has posed a threat to aquatic ecosystems, so it's urgent to remove excessive phosphate from water. In this study, we developed an adsorbent material, cerium/terephthalic-acid metal-organic-frameworks (Ce-MOF), to remove phosphate from different water systems. The optimal Ce-MOF presented a maximum phosphate adsorption capacity of 377.2 mg/g, approximately 3.7 times higher than that of the commercial phosphate adsorbent (Phoslock: 101.6 mg/g). Experimental and computational analysis suggested that pH dominated the adsorption process. The main forces driving the adsorption process changed from the synergistic effect of electrostatic attraction and ligand exchange at lower pH to only ligand exchange at the increased pH values. Hence, the Ce-MOF is applicable for phosphate adsorption in a wide pH range. Impressively, the adsorbent remained an excellent phosphate adsorption performance in the real water containing various interfering ions and organic matters, indicating the potential of Ce-MOF for the practical use to solve the water eutrophication issue.

9.
Adv Sci (Weinh) ; 10(18): e2300034, 2023 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-37088791

RESUMEN

Regulating the charge migration and separation in photoactive materials is a great challenge for developing photoelectrochemical (PEC) applications. Herein, inspired by capacitors, well-defined CuInSe2 /N-doped carbon (CISe/N-C) nanorod arrays are synthesized by Cu/In-metal organic frame-derived method. Like the charge process of capacitor, the N-doped carbon can capture the photogenerated electron of CISe, and the strong interfacial coupling between CISe and N-doped carbon can modulate the charge migration and separation. The optimized the CISe/N-C photoanode achieves a maximum photocurrent of 4.28 mA cm-2 at 1.23 V versus reversible hydrogen electrode (RHE) in neutral electrolyte solution under AM 1.5 G simulated sunlight (100 mW cm-2 ), which is 8.4 times higher than that of the CuInSe2 photoanode (0.51 mA cm-2 ). And a benefit of the strong electronic coupling between CISe and N-doped carbon, the charge transfer rate is increased to 1.3-13 times higher than that of CISe in the range of 0.6-1.1 V versus RHE. The interfacial coupling effects on modulating the carrier transfer dynamics are investigated by Kelvin probe force microscopy analysis and density functional theory calculation. This work provides new insights into bulk phase carrier modulation to improve the performance of photoanode for PEC water splitting.


Asunto(s)
Carbono , Nanotubos , Electrodos , Electrónica , Excipientes , Agua
10.
Water Res ; 229: 119464, 2023 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-36509034

RESUMEN

Conventional electrocatalytic degradation of pollutants involves either cathodic reduction or anodic oxidation process, which caused the low energy utilization efficiency. In this study, we successfully couple the anodic activation of sulfates with the cathodic H2O2 production/activation to boost the generation of sulfate radical (SO4·-) and hydroxyl radical (·OH) for the efficient degradation of emerging contaminants. The electrocatalysis reactor is composed of a modified-graphite-felt (GF) cathode, in-situ prepared by the carbonization of polyaniline (PANI) electrodeposited on a GF substrate, and a boron-doped diamond (BDD) anode. In the presence of sulfates, the electrocatalysis system shows superior activities towards the degradation of pharmaceutical and personal care products (PPCPs), with the optimal performance of completely degrading the representative pollutant carbamazepine (CBZ, 0.2 mg L-1) within 150 s. Radicals quenching experiments indicated that ·OH and SO4·- act as the main reactive oxygen species for CBZ decomposition. Results from the electron paramagnetic resonance (EPR) and chronoamperometry studies verified that the sulfate ions were oxidized to SO4·-radicals at the anode, while the dissolve oxygen molecules were reduced to H2O2 molecules which were further activated to produce ·OH radicals at the cathode. It was also found that during the catalytic reactions SO4·-radicals could spontaneously convert into peroxydisulfate (PDS) which were subsequently reduced back to SO4·-at the cathodes. The quasi-steady-state concentrations of ·OH and SO4·-were estimated to be 0.51×10-12 M and 0.56×10-12 M, respectively. This study provides insight into the synergistic generation of ·OH/SO4·- from the integrated electrochemical anode oxidation of sulfate and cathode reduction of dissolved oxygen, which indicates a potential practical approach to efficiently degrade the emerging organic water contaminants.


Asunto(s)
Peróxido de Hidrógeno , Contaminantes Químicos del Agua , Radical Hidroxilo/química , Electrodos , Sulfatos/química , Oxidación-Reducción , Oxígeno , Contaminantes Químicos del Agua/química
11.
Water Res ; 223: 118967, 2022 Sep 01.
Artículo en Inglés | MEDLINE | ID: mdl-35973248

RESUMEN

Dissolved organic matter (DOM), ubiquitous in natural waters, is known to inhibit the degradation of micropollutants in the advanced oxidation processes such as the UV/peroxydisulfate process. However, the quantitative understanding of the inhibitory pathways is missing. In this study, guanosine, aniline and catechol belonging to amines, purines and phenols were first investigated due to their resistance to UV irradiation at 254 nm and similar reactivity with SO4•- and HO•, respectively. The presence of 0.5 mgC L-1 Suwannee River NOM (SRNOM) inhibited their degradation rates by 72.9%, 54.5%, and 32.4%, respectively, despite their similar degradation rates in the absence of SRNOM. The results highlight the importance of reverse reduction of oxidation intermediates to the parent compound by antioxidant moieties in SRNOM besides the inner filtering and radical scavenging effects. The three inhibitory pathways were quantified for 34 common micropollutants. In the presence of 0.5 mgC L-1 SRNOM, inner filtering effect was found to contribute less than 2.8% of the inhibitory percentages (IP). Radical scavenging effects contribute between 10.7% and 38.9% and compounds having lower reactivity with SO4•- (< 4.0 × 109 M-1 s-1) tended to be inhibited more strongly. The IP of reverse reduction effects of SRNOM varied significantly from none up to 70.8%. It was linearly related with a micropollutant's reduction potential. Purines and amines generally exhibited more pronounced reverse reduction inhibition than phenols. The results of this study provide guidance on improving the elimination efficiency of micropollutants.


Asunto(s)
Contaminantes Químicos del Agua , Purificación del Agua , Compuestos de Anilina , Antioxidantes , Catecoles , Materia Orgánica Disuelta , Guanosina , Cinética , Oxidación-Reducción , Fenoles , Purinas , Rayos Ultravioleta , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos
12.
Meat Sci ; 185: 108724, 2022 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-34952489

RESUMEN

The objective of this study was to investigate the protective effects and the underlying mechanisms of resveratrol (RES) against hydrogen peroxide (H2O2)-induced oxidative stress in bovine skeletal muscle cells (BMCs). Pretreatment of BMCs with RES prior to H2O2 exposure increased cell viability, attenuated reactive oxygen species, and stabilized the redox state. H2O2 exposure activated sirtuin type 1 (SIRT1) and nuclear factor E2-related factor 2 (NRF2)-mediated signaling pathways. Pretreatment with RES did not alter SIRT1-regulated genes but inhibited the upregulation of NRF2, whereas enhanced heme oxygenase 1 (HO-1) expression. Pretreatment with RES prior to H2O2 exposure failed to suppress NRF2 expression when NRF2 was knocked down by RNA interference. However, HO-1 expression still could be induced by RES. These results suggest that RES has benifical effects against oxidative stress. NRF2-mediated pathway play an important role, and HO-1 upregulation is the key process in RES regulation. RES may be used as a therapeutic agent for meat quality improvement in beef cattle.


Asunto(s)
Apoptosis , Peróxido de Hidrógeno , Animales , Antioxidantes/farmacología , Bovinos , Músculo Esquelético , Estrés Oxidativo , Especies Reactivas de Oxígeno , Resveratrol/farmacología
13.
Environ Sci Technol ; 55(12): 8341-8350, 2021 06 15.
Artículo en Inglés | MEDLINE | ID: mdl-34076409

RESUMEN

Defective MIL-88B(Fe) nanorods are exploited as exemplary iron-bearing metal-organic framework (MOF) catalyst for molecular oxygen (O2) activation at ambient temperature, triggering effective catalytic oxidation of formaldehyde (HCHO), one of the major indoor air pollutants. Defective MIL-88B(Fe) nanorods, growing along the [001] direction, expose abundant coordinatively unsaturated Fe-sites (Fe-CUSs) along extended hexagonal channels with a diameter of ca. 5 Å, larger enough for the diffusion of O2 (3.46 Å) and HCHO (2.7 Å). The Lewis acid-base interaction between Fe-CUSs and accessible HCHO accelerates the FeIII/FeII cycle, catalyzing Fenton-like O2 activation to produce reactive oxidative species (ROSs), including superoxide radicals (•O2-), hydroxyl radicals (•OH), and singlet oxygen (1O2). Consequently, adsorbed HCHO can be oxidized into CO2 with a considerable mineralization efficiency (over 80%) and exceptional recyclability (4 runs, 48 h). Dioxymethylene (CH2OO), formate (HCOO-) species, and formyl radicals (•CHO) are recorded as the main reaction intermediates during HCHO oxidation. HCHO, H2O, and O2 are captured and activated by abundant FeIII/FeII-CUSs as acid/base and redox sites, triggering synergetic ROS generation and HCHO oxidation, involving cooperative acid-base and redox catalysis processes. This study will bring new insights into exploiting novel MOF catalysts for efficient O2 activation and reliable indoor air purification at ambient temperature.


Asunto(s)
Compuestos Férricos , Nanotubos , Catálisis , Formaldehído , Oxidación-Reducción , Oxígeno , Temperatura
14.
Water Res ; 197: 117042, 2021 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-33784605

RESUMEN

Bromide (Br-) is a typical scavenger to sulfate radical (SO4•-) and hydroxyl radical (HO•), which simultaneously forms secondary reactive bromine species (RBS) such as Br• and Br2•-. This study investigated the effects of Br- at fresh water levels (~µM) on the radical chemistry in the UV/peroxydisulfate (UV/PDS) process by combining the degradation kinetics of probe compounds (nitrobenzene, metronidazole, and benzoate) with kinetic model. Br- at 1 - 50 µM promoted the conversion from SO4•- to HO• and RBS in the UV/PDS process. At pH 7, the concentration of SO4•- monotonically decreased by 31.5 - 94.8% at 1 - 50 µM Br-, while that of HO• showed an increasing and then decreasing pattern, with a maximum increase by 171.7% at 5 µM Br-. The concentrations of Br• and Br2•- (10-12 - 10-10 M) were 2 - 3 orders of magnitude higher than SO4•- and HO•. Alkaline condition promoted the conversion from SO4•- to HO•, and drove the transformation from RBS to HO•, resulting in much lower concentrations of RBS at pH 10. Br- at 1 µM and 5 µM decreased the pseudo-first-order reaction rates (k's) of 15 pharmaceuticals and personal care products (PPCPs) by 15.2 - 73.9%, but increased k's of naproxen and ibuprofen by 13.7 - 57.3% at pH 7. The co-existence of 10 - 1000 µM Cl- with 5 µM Br- further promoted the conversion from SO4•- to HO• compared to Br- alone. Bicarbonate consumed SO4•- and HO• but slightly affected RBS, while natural organic matter (NOM) exerted scavenging effects on HO• and RBS more significantly than SO4•-. This study demonstrated that Br- at fresh water levels significantly altered the radical chemistry of the UV/PDS process, especially for promoting the formation of HO•.


Asunto(s)
Contaminantes Químicos del Agua , Purificación del Agua , Bromuros , Agua Dulce , Peróxido de Hidrógeno , Cinética , Oxidación-Reducción , Rayos Ultravioleta , Contaminantes Químicos del Agua/análisis
15.
Water Res ; 180: 115925, 2020 Aug 01.
Artículo en Inglés | MEDLINE | ID: mdl-32413592

RESUMEN

Pharmaceuticals and personal care products (PPCPs), an emerging class of highly recalcitrant water contaminants, have raised considerable concerns in environment community. Graphitic carbon nitride (CN) has shown a great potential towards the photodegradation of water contaminants under visible light irradiation. However, the conventional bulk CN (BCN) presents the amorphous structure, resulting in an inefficient yield of hydroxyl radicals (•OH) for the complete mineralization of PPCPs. This study provides fundamental insights into significantly enhancing the hydroxyl radical generation via improving the crystallinity of the pristine CN materials. Experimental measurements and accompanying density functional theory (DFT) computational analysis suggest that the crystalline carbon nitride (CCN) exhibited an enhanced adsorption ability towards the dissolved O2. Upon the light irradiation, the adsorbed O2 molecules readily undergo a direct two-electron reduction reaction on the CCN surface, instead of the conventional two successive single-electron reduction reactions on the BCN surface, to produce H2O2 subsequently converting into •OH radicals. Along with the improved charge separation efficiency and electron transfer ability, CCN-based materials show superior photocatalytic activity towards PPCPs-type pollutants, compared with the pristine BCN catalysts. Importantly, the catalyst show excellent photodegradation activities under natural sunlight irradiation, at low PPCPs concentration (20 µg/L), in the mixed PPCPs solution or in the real wastewater/water samples, indicating the potential of CCN to enable practical ex situ destructive treatment of PPCPs-contaminated groundwater.


Asunto(s)
Cosméticos , Contaminantes Químicos del Agua , Grafito , Peróxido de Hidrógeno , Compuestos de Nitrógeno , Fotólisis , Agua
16.
Nanoscale ; 12(17): 9385-9391, 2020 May 07.
Artículo en Inglés | MEDLINE | ID: mdl-32196033

RESUMEN

Water treatment techniques for destructive removal of nitrates by reducing them to harmless N2 have recently begun to emerge. In this study, we present a novel three-dimensional (3D) Cu nanobelt cathode for efficient electrochemical nitrate reduction. Upon an applied potential of -1.4 V vs. Ag/AgCl, the removal efficiency of nitrates by the 3D Cu nanobelt electrode reaches 100% at 60 min, compared to 2.6% for the Cu foam electrode under the same conditions. Based on the mass balance on nitrogen atoms, the major product is determined to be ammonia. In the simulated wastewater containing NaCl, the as-generated ammonia ions are simultaneously oxidized into harmless N2 by the in situ generated ClO- ions from the Pt anode, resulting in the complete removal of inorganic nitrogen (nitrate, nitride and ammonia) from wastewater. The mechanism for the improvement of electrocatalytic activity is systematically investigated. Firstly, the large surface area of the 3D Cu nanobelt electrode facilitates the mass transfer of nitrates, resulting in accelerated electrochemical kinetics. Secondly, linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS) measurements confirm that the 3D Cu nanobelt electrode exhibits improved charge transfer ability. Also, further investigations demonstrate that the 3D Cu nanobelt electrode preferentially reacts with nitrates, compared to the pristine Cu foam electrode readily reacting with the dissolved oxygen (DO) to generate H2O2. This study might expand the prospects of electrocatalytic techniques towards the destructive removal of inorganic nitrogen pollutants in wastewater.

17.
Water Res ; 175: 115684, 2020 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-32171099

RESUMEN

Photocatalysis provides a "green" strategy to produce the clean energy of H2. However, the realization of efficient H2 production is usually accomplished by the consumption of electron donors, which are costly energy carriers themselves. Here, we attempted to utilize the naturally abundant humic acid (HA), a representative natural organic matter (NOM), as the source of electron donor in a cascading oxic-anoxic photocatalytic system. Results showed that degradation of HA and remarkable H2 yield (1660.9 µmol g-1 h-1 at optimal condition) were obtained successively, whereas the anoxic photocatalytic treatment of pristine HA did not improve H2 yield but substantially eliminated the H2 production and HA degradation efficiency. These phenomena suggested the preoxidation process played a vital role in counteracting the detrimental effect of HA on photocatalytic H2 production. Electrochemical measurement indicated that the preoxidized HA harbored more redox-active moieties than the untreated HA and thus leading to a higher photo-induced charge carrier separation efficiency. A variety of advanced spectroscopic analyses revealed that the photocatalytic oxic pre-treatment resulted in breakdown of chemically inert, electron mediating and chromophoric aromatic macrostructure of HA to form smaller sized oxygenated organic intermediates. These intermediates were more nucleophilic than the pristine HA and acted as sacrificial reagent in the subsequent anoxic process for boosting H2 production. This study showcases an energy recovering water remediation process and paves the way for the design of novel photocatalytic technologies for environmental application.


Asunto(s)
Sustancias Húmicas , Purificación del Agua , Electrones , Hidrógeno , Oxidación-Reducción
18.
Chem Commun (Camb) ; 56(21): 3179-3182, 2020 Mar 12.
Artículo en Inglés | MEDLINE | ID: mdl-32065209

RESUMEN

We report a facile alkali-assisted salt molten method to construct crystalline carbon nitride with rich nitrogen vacancies. Experimental and computational results show that the crystalline structure allows efficient charge transfer and the nitrogen vacancies provide more active sites, resulting in the enhanced photocatalytic hydrogen production.

19.
Materials (Basel) ; 12(23)2019 Nov 30.
Artículo en Inglés | MEDLINE | ID: mdl-31801299

RESUMEN

In this paper, an Al2O3 coated CaF2 (CaF2@Al2O3) nanocomposite powder is used as the additive phase of a Ti(C,N)-based self-lubricating cermet material. A novel self-lubricating ceramic material with a multilayer core-shell microstructure was prepared using a vacuum hot-pressing sintering process. The results show that the surface of the CaF2 powder is coated with Al2O3, and when introduced into a Ti(C,N)-Mo-Co-Ni material system, it can utilize the high-temperature liquid phase diffusion mechanism of the metal Mo-Co-Ni phase in the sintering process. The CaF2@Al2O3@Mo-Co-Ni multilayer core-shell microstructure is formed in the material. Compared with the direct addition of CaF2 and Al2O3, the hardness and fracture toughness of the material are increased by 24.31% and 22.56%, reaching 23.93 GPa and 9.94 MPa·m1/2, respectively. The formation of the multilayer core-shell microstructure is the main reason for the improvement of the mechanical properties of the material.

20.
Front Genet ; 10: 1351, 2019.
Artículo en Inglés | MEDLINE | ID: mdl-32038711

RESUMEN

Shandong indigenous pig breeds are an invaluable source of data on genetics in Chinese pigs. However, information on the genetic basis of these breeds remains limited. In this study, we used specific-locus amplified fragment sequencing to conduct whole-genome screening to investigate genetic diversity in Shandong indigenous breeds and Western pig breeds. The results showed that Duroc pigs (DD) had clear genetic relationships with Dapulian pigs (DPL; Fst = 0.4386) and Laiwu pigs (LW; Fst = 0.5134), and DPL and LW were relatively close genetically (Fst = 0.2334). In general, Shandong indigenous breeds showed greater genetic variety than the Western breeds. Both neighbor-joining trees and principal components analyses were able to differentiate the breeds, but population structure analyses indicated that the Western breeds genetically influenced the Shandong indigenous breeds to some extent. A total of 162 differentially selected regions (DSRs) with 841 genes and 157 DSRs with 707 genes were identified in DPL and LW, respectively. Gene annotation of the selected regions identified a series of genes regulating immunity and fat deposition. Our data confirm the rationality and accuracy of the current classification of pig breeds in Shandong province. Our results point to candidate genes in Shandong indigenous pig breeds and further promote the importance of follow-up research on functional verification.

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