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1.
Clin Anat ; 2024 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-38725353

RESUMO

Cadaveric study; To describe the characteristics of the nerve and its relationship with the lumbar intervertebral disc and psoas major muscle. Nerve injury is an understudied complication of extreme lateral interbody fusion. A detailed description of the nerve anatomy would be helpful for surgeons to minimize the risk of this complication. The lumbar plexus and lumbar sympathetic nerve of 10 embalmed male cadavers were dissected, and the distribution, number, and spatial orientation of the nerves on the L1/2 to L4/5 intervertebral discs were examined. Metal wires were applied along nerve paths through the psoas major muscle. The position of the nerves was examined on CT. In zone III at L1/2 and L4/5, no nerves were found. In zone II and zone III at L2/3, no lumbar plexus was found, and only the ramus communicans passed through. At the L1-L5 level, the density of nerves in the posterior half of the psoas major muscle was greater than that in the anterior half. The lumbar plexus was found in all of zone IV. The genitofemoral nerve emerges superficially and anteriorly from the medial border of the psoas major at the L3-4 level, but at the L1/2 level, the sympathetic trunk is located in zone II. The remaining disc-level sympathetic trunks appear in zone I. No nerves were found in zone III of the L1/2 or L4/5 disc. In zones II and III of L2/3, the lumbar plexus appears safe. The genitofemoral nerve travels through zones II and III of L3/4. The distribution density of nerves in the posterior half of the psoas major muscle was greater than that in the anterior half of that muscle at the L1-L5 level.

2.
Small ; 19(23): e2207666, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-36703516

RESUMO

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.

3.
Langmuir ; 38(2): 828-837, 2022 Jan 18.
Artigo em Inglês | MEDLINE | ID: mdl-34984900

RESUMO

Graphitic carbon nitride (g-C3N4) has attracted extensive research attention because of its virtues of a metal-free nature, feasible synthesis, and excellent properties. However, the low specific surface area and mediocre charge separation dramatically limit the practical applications of g-C3N4. Herein, porous nitrogen defective g-C3N4 (PDCN) was successfully fabricated by the integration of urea-assisted supramolecular assembly with the polymerization process. Advanced characterization results suggested that PDCN exhibited a much larger specific surface area and dramatically improved charge separation compared to bulk g-C3N4, leading to the formation of more active sites and the improvement in mass transfer. The synthesized PDCN rendered a 16-fold increase in photocatalytic tetracycline degradation efficiency compared to g-C3N4. Additionally, the hydrogen evolution rate of PDCN was 10.2 times higher than that of g-C3N4. Meanwhile, the quenching experiments and electron spin resonance (ESR) spectra suggested that the superoxide radicals and holes are the predominant reactive species for the photocatalytic degradation process. This study may inspire the new construction design of efficient g-C3N4-based visible-light photocatalysts.

4.
Small ; 17(50): e2100927, 2021 12.
Artigo em Inglês | MEDLINE | ID: mdl-34318613

RESUMO

As emerging micro/nano-scale devices, micro/nanomotors have been innovatively applied in the environmental and biomedical applications. In this paper, the recent advances of Mn-based micro/nanomotors (Mn-micro/nanomotors) in catalytic oxidation of organic contaminants and the mechanisms in decomposition of H2 O2 (e.g., the generation of O2 bubbles and reactive oxygen species) are reviewed. The intrinsic characteristics and synthetic strategies of Mn-based materials are discussed, aiming to gain comprehensive understandings on the asymmetric design of micro/nanomotors. Mn-micro/nanomotors have many advantages such as flexible structures, biocompatibility, powerful motion, long lifetime, and low-cost as compared to noble-metal micro/nanomotors. These merits fulfil Mn-micro/nanomotors great promises from proof-of-concept studies to realistic applications, including pollutant decomposition, trace detection of heavy metal ions, oil removal, drug delivery, isolation of biological targets, and killing bacteria and cancer cells. The great flexibility in fabrication enables diverse and innovative strategies to address challenges for Mn-micro/nanomotors, including high consumption of H2 O2 and non-directional motion. Meanwhile, a perspective of Mn-micro/nanomotors in water remediation by coupling the motors with other Fenton/Fenton-like systems to enhance the catalytic activity and to yield more reactive oxygen species is presented. Directions to the design of on-demand H2 O2 -fueled Mn-micro/nanomotors for advanced purification of organic contaminants in aquatic systems are also proposed.


Assuntos
Manganês , Nanotecnologia , Catálise , Íons , Movimento (Física)
5.
Small ; 17(16): e2004579, 2021 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-33464724

RESUMO

The development of novel single atom catalyst (SAC) is highly desirable in organic synthesis to achieve the maximized atomic efficiency. Here, a Co-based SAC on nitrogen-doped graphene (SACo@NG) with high Co content of 4.1 wt% is reported. Various characterization results suggest that the monodispersed Co atoms are coordinated with N atoms to form robust and highly effective catalytic centers to activate peroxymonosulfate (PMS) for organic selective oxidation. The catalytic performance of the SACo@NG/PMS system is conducted on the selective oxidation of benzyl alcohol (BzOH) showing high efficiency with over 90% conversion and benzaldehyde selectivity within 180 min under mild conditions. Both radical and non-radical processes occurred in the selective oxidation of BzOH, but the non-radical oxidation plays the dominant role which is accomplished by the adsorption of BzOH/PMS on the surface of SACo@NG and the subsequent electron transfer through the carbon matrix. This work provides new insights to the preparation of efficient transition metal-based single atom catalysts and their potential applications in PMS mediated selective oxidation of alcohols.

6.
Acc Chem Res ; 51(3): 678-687, 2018 03 20.
Artigo em Inglês | MEDLINE | ID: mdl-29494126

RESUMO

Catalytic processes have remarkably boosted the rapid industrializations in chemical production, energy conversion, and environmental remediation. As one of the emerging applications of carbocatalysis, metal-free nanocarbons have demonstrated promise as catalysts for green remediation technologies to overcome the poor stability and undesirable metal leaching in metal-based advanced oxidation processes (AOPs). Since our reports of heterogeneous activation of persulfates with low-dimensional nanocarbons, the novel oxidative system has raised tremendous interest for degradation of organic contaminants in wastewater without secondary contamination. In this Account, we showcase our recent contributions to metal-free catalysis in advanced oxidation, including design of nanocarbon catalysts, exploration of intrinsic active sites, and identification of reactive species and reaction pathways, and we offer perspectives on carbocatalysis for future environmental applications. The journey starts with the discovery of peroxymonosulfate (PMS) and peroxydisulfate (PDS) activation by graphene-based materials. With the systematic investigations on most carbon allotropes, for the first time the carbocatalysis for PMS or PDS activation was correlated with the pristine carbon configuration, oxygen functionality (ketonic groups), defect degree (exposed edge sites and vacancies), and dimensional structure. Moreover, an intrinsic difference in catalytic oxidation does exist between PMS and PDS activation. For example, the PMS/carbon reaction is dominated by free radicals, while PDS/carbon catalysis was unveiled as a singlet oxygen- or nonradical-based process in which the surface-activated PDS complex directly degrades the organic pollutants without relying on the generation of free radicals. Nitrogen doping significantly enhances the carbocatalysis because of the positively charged carbon domains, which strongly bind with persulfates to form reactive intermediates toward organic reactions. More importantly, N doping substantially alters the catalytic oxidation from a radical process to a nonradical pathway in PMS activation. Codoping of sulfur or boron with nitrogen at a rational level will synergistically promote the catalysis as a result of the formation of more catalytic centers by improved charge/spin redistribution of the carbon framework. Furthermore, a structure-performance relationship was established for annealed nanodiamonds with a characteristic sp3/sp2 (core/shell) hybridization, where the catalytic pathways were intimately dependent on the thickness of the graphitic shells. Interestingly, the introduction of structural defects and N dopants into the well-defined graphitic carbon framework and alteration of graphene/diamond hybrids can transform the persulfate/carbon system from a radical oxidation pathway to a nonradical pathway. Encapsulation of metal nanoparticles within carbon layers further modulates the electronic states of the interacting carbon via charge transport to increase the electron density. Overall, this Account contributes to unveiling the mist of carbocatalysis in AOPs and to summarizing the achievements of metal-free remediation. We also present future research directions on underpinning the knowledge base to facilitate the applications of nanocarbons in sustainable catalysis and environmental chemistry.

7.
Environ Sci Technol ; 53(19): 11391-11400, 2019 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-31436973

RESUMO

The maximization of the numbers of exposed active sites in supported metal catalysts is important to achieve high reaction activity. In this work, a simple strategy for anchoring single atom Fe on SBA-15 to expose utmost Fe active sites was proposed. Iron salts were introduced into the as-made SBA-15 containing the template and calcined for simultaneous decomposition of the iron precursor and the template, resulting in single atom Fe sites in the nanopores of SBA-15 catalysts (SAFe-SBA). X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy (UV-vis DRS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and extended X-ray absorption fine structure (EXAFS) imply the presence of single atom Fe sites. Furthermore, EXAFS analysis suggests the structure of one Fe center with four O atoms, and density functional theory calculations (DFT) simulate this structure. The catalytic performances of SAFe-SBA were evaluated in Fenton-like catalytic oxidation of p-hydroxybenzoic acid (HBA) and phenol. It was found that the single atom SAFe-SBA catalysts displayed superior catalytic activity to aggregated iron sites (AGFe-SBA) in both HBA and phenol degradation, demonstrating the advantage of SAFe-SBA in catalysis.


Assuntos
Ferro , Fenol , Catálise , Oxirredução , Difração de Raios X
8.
Small ; 11(25): 3036-44, 2015 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-25786381

RESUMO

Sulfur and nitrogen co-doped reduced graphene oxide (rGO) is synthesized by a facile method and demonstrated remarkably enhanced activities in metal-free activation of peroxymonosulfate (PMS) for catalytic oxidation of phenol. Based on first-order kinetic model, S-N co-doped rGO (SNG) presents an apparent reaction rate constant of 0.043 ± 0.002 min(-1) , which is 86.6, 22.8, 19.7, and 4.5-fold as high as that over graphene oxide (GO), rGO, S-doped rGO (S-rGO), and N-doped rGO (N-rGO), respectively. A variety of characterization techniques and density functional theory calculations are employed to investigate the synergistic effect of sulfur and nitrogen co-doping. Co-doping of rGO at an optimal sulfur loading can effectively break the inertness of carbon systems, activate the sp(2) -hybridized carbon lattice and facilitate the electron transfer from covalent graphene sheets for PMS activation. Moreover, both electron paramagnetic resonance (EPR) spectroscopy and classical quenching tests are employed to investigate the generation and evolution of reactive radicals on the SNG sample for phenol catalytic oxidation. This study presents a novel metal-free catalyst for green remediation of organic pollutants in water.

9.
Environ Sci Technol ; 47(11): 5882-7, 2013 Jun 04.
Artigo em Inglês | MEDLINE | ID: mdl-23651050

RESUMO

Three one-dimensional MnO2 nanoparticles with different crystallographic phases, α-, ß-, and γ-MnO2, were synthesized, characterized, and tested in heterogeneous activation of Oxone for phenol degradation in aqueous solution. The α-, ß-, and γ-MnO2 nanostructured materials presented in morphologies of nanowires, nanorods, and nanofibers, respectively. They showed varying activities in activation of Oxone to generate sulfate radicals for phenol degradation depending on surface area and crystalline structure. α-MnO2 nanowires exhibited the highest activity and could degrade phenol in 60 min at phenol concentrations ranging in 25-100 mg/L. It was found that phenol degradation on α-MnO2 followed first order kinetics with an activation energy of 21.9 kJ/mol. The operational parameters, such as MnO2 and Oxone loading, phenol concentration and temperature, were found to influence phenol degradation efficiency. It was also found that α-MnO2 exhibited high stability in recycled tests without losing activity, demonstrating itself to be a superior heterogeneous catalyst to the toxic Co3O4 and Co(2+).


Assuntos
Compostos de Manganês/química , Nanoestruturas/química , Óxidos/química , Fenol/química , Poluentes Químicos da Água/química , Adsorção , Catálise , Cristalografia , Nanopartículas/química , Nanotubos/química , Nanofios , Sulfatos , Ácidos Sulfúricos , Temperatura
10.
J Hazard Mater ; 460: 132400, 2023 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-37639789

RESUMO

Over the past few years, advanced oxidation processes (AOPs) have shown promising efficiencies for wastewater remediation. Carbocatalysis, in particular, has been exploited widely thanks to its sustainable and economical properties but has an issue of recovery and reusability of the catalysts. To address this, three-dimensional (3D) binary and ternary graphene-based composites in the form of macro discs were created to activate peroxymonosulfate (PMS) for catalytic oxidation of sulfamethoxazole (SMX). Graphene oxide served as the base, while graphitic carbon nitride (g-C3N4) and/or single-walled carbon nanotubes (SWCNTs) were added. Among the various discs synthesized, rGNTCN discs (ternary composite) were proven to be the most efficient by completely degrading SMX in 60 min owing to their large surface area and nitrogen loading. The catalytic system was further optimized by varying the reaction parameters, and selective radical quenching and electron paramagnetic resonance tests were performed to identify the active radical, revealing the synergistic role of both radical and non-radical pathways. This led to the development of possible SMX degradation pathways. This research not only provides insights into ternary carbocatalysis but also gives a novel breakthrough in catalyst recovery and reusability by transforming nanocatalysts into macro catalysts.

11.
Small Methods ; 7(10): e2300588, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37415309

RESUMO

Industrial and disinfection wastewater typically contains high levels of organic pollutants and residue hydrogen peroxide, which have caused environmental concerns. In this work, dual-asymmetric MnO2 @polymer microreactors are synthesized via pollutant polymerization for self-driven and controlled H2 O2 decomposition. A hollow and asymmetric MnO2 nanotube is derived from MnO2 nanorods by selective acid etching and then coated by a polymeric layer from an aqueous phenolic pollutant via catalytic peroxymonosulfate (PMS)-induced polymerization. The evolution of particle-like polymers is controlled by solution pH, molar ratios of PMS/phenol, and reaction duration. The polymer-covered MnO2 tubing-structured micromotors presented a controlled motion velocity, due to the reverse torque driven by the O2 bubbles from H2 O2 decomposition in the inner tunnels. In addition, the partially coated polymeric layer can regulate the exposure and population of Mn active sites to control the H2 O2 decomposition rate, thus avoiding violent motions and massive heat caused by vigorous H2 O2 decomposition. The microreactors can maintain the function of mobility in an ultra-low H2 O2 environment (<0.31 wt.%). This work provides a new strategy for the transformation of micropollutants to functional polymer-based microreactors for safe and controlled hydrogen peroxide decomposition for environmental remediation.

12.
J Colloid Interface Sci ; 634: 972-982, 2023 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-36571859

RESUMO

Photo-Fenton-like catalysis allows development of novel advanced oxidation technology with promising application in wastewater treatment. In this work, carbon dots (CDs) were intercalated between CuO nanoparticles and coralloid flower-like graphitic carbon nitride (g-C3N4) to fabricate a ternary CuO/CDs/g-C3N4 hybrid for synergetic visible-light-driven photo-Fenton-like oxidation. The CuO/CDs/g-C3N4 hybrid showed remarkable degradation efficiency towards recalcitrant organic contamination, excellent tolerance to realistic environmental conditions, exceptional stability and wide universality, declaring great potential for practical applications. •OH and •O2- radicals were demonstrated to be the primary contributors in the photo-Fenton-like system. Mechanism studies reveal dual charge transfer pathways in the Z-scheme CuO/g-C3N4 heterojunction assisted by interfacial electron transmission bridges of CDs, which can simultaneously boost the reduction of Cu2+ to Cu+ in the Fenton-like cycle and accelerate the Z-scheme electron flow from CuO to g-C3N4, leading to synergistic enhancement of the catalytic performance. This work would afford a feasible strategy to develop reinforced solar energy-assisted photo-Fenton-like catalysis systems for water remediation.

13.
J Colloid Interface Sci ; 632(Pt A): 117-128, 2023 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-36410293

RESUMO

Increasing water pollution has imposed great threats to public health, and made efficient monitoring and remediation technologies critical to a clean environment. In this study, a versatile heterojunction of Au nanoparticles modified phosphorus doped carbon nitride (Au/P-CN) is designed and fabricated. The Au/P-CN heterostructure demonstrates improved light absorption, rapid separation of charge carriers, and improved electrical conductivity. Taking the toxic 4-chlorophenol (4-CP) as an example, an ultrasensitive photoelectrochemical (PEC) sensor is successfully demonstrated, exhibiting a wide linear range (0.1-52.1 µM), low detection limit (∼0.02 µM), significant stability and selectivity, as well as reliable analysis in real samples. Moreover, efficient photocatalytic degradation with a high removing efficiency (∼87%) toward 4-CP is also achieved, outperforming its counterpart of Au nanoparticles (NPs) modified graphitic carbon nitride (Au/g-CN, ∼59%). This work paves a new way for efficient and simultaneous detection and remediation of organic pollutants over versatile photoactive catalysts.


Assuntos
Ouro , Nanopartículas Metálicas , Fósforo
14.
J Hazard Mater ; 448: 130874, 2023 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-36716559

RESUMO

Membrane separation and sulfate radicals-based advanced oxidation processes (SR-AOPs) can be combined as an efficient technique for the elimination of organic pollutants. The immobilization of metal oxide catalysts on ceramic membranes can enrich the membrane separation technology with catalytic oxidation avoiding recovering suspended catalysts. Herein, nanostructured Co3O4 ceramic catalytic membranes with different Co loadings were fabricated via a simple ball-milling and calcination process. Uniform distribution of Co3O4 nanoparticles in the membrane provided sufficient active sites for catalytic oxidation of 4-hydroxybenzoic acid (HBA). Mechanistic studies were conducted to determine the reactive radicals and showed that both SO4•- and •OH were present in the catalytic process while SO4•- plays the dominant role. The anti-fouling performance of the composite Co@Al2O3 membranes was also evaluated, showing that a great flux recovery was achieved with the addition of PMS for the fouling caused by humic acid (HA).

16.
Cir Cir ; 90(5): 632-637, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36327468

RESUMO

OBJECTIVE: The objective of this study was to investigate the role of sirtuin 6 (SIRT6) in severe community acquired pneumonia (CAP) in child patients. METHODS: This prospective observational research enrolled a total of 75 severe child CAP patients who went to our hospital during April 2016 to December 2020, and 75 mild/moderate CAP child patients were included as control. SIRT6 and inflammatory factors C-reactive protein (CRP), interleukin (IL)-6, and procalcitonin (PCT) were tested by the enzyme linked immunosorbent assay (ELISA). Demographic data including age, sex, as well as clinical symptoms, duration of ICU stay, duration of mechanical ventilation were collected. The routine blood test was conducted for all patients and WBC amount and neutrophil ratio were recorded. The pediatric critical illness score (PCIS) and 1-month mortality were collected. RESULTS: Levels of SIRT6 were remarkably lower in severe CAP patients or deceased patients compared with mild/moderate or survival patients, respectively. Levels of CRP, PCT, and interleukin-6 (IL-6) were markedly higher in severe patients than mild/moderate patients. However, only levels of CRP were significantly higher in deceased CAP patients and serum levels of SIRT6 were negatively correlated with serum levels of CRP, PCT, and IL-6. The higher levels of CRP, PCT and IL-6, as well as higher mortality rate and lower levels of PCIS were found in patients with lower SIRT6 compared with parents with higher SIRT6. SIRT6 had the potential for diagnosis of severe CAP and patients with lower SIRT1 showed shorter 1-month survival. Further, logistic regression showed that only age and CRP were independent risk factors for 1-month mortality of CAP child parents. CONCLUSION: Down-regulated SIRT6 in severe CAP child patients predicted higher expression of inflammatory factors, severer clinical outcomes and poor prognosis.


OBJETIVO: Investigar el papel de sirtuin 6 (SIRT6) en la neumonía adquirida en la comunidad (NAC) grave en pacientes infantiles. MÉTODOS: Esta investigación observacional prospectiva inscribió a un total de 459 pacientes con NAC infantil grave que acudieron a nuestro hospital entre abril de 2016 y diciembre de 2020, y se incluyeron como control 459 pacientes con NAC infantil leve/moderada. RESULTADOS: Los niveles de SIRT6 fueron notablemente más bajos en pacientes con NAC grave o pacientes fallecidos en comparación con los pacientes leves/moderados o con supervivencia, respectivamente. Todos los niveles de PCR, PCT e Interleukin-6 (IL-6) fueron significativamente más altos en pacientes con CAP fallecidos y los niveles séricos de SIRT6 se correlacionaron negativamente con los niveles séricos de CRP, PCT e IL-6. Los niveles más altos de PRISM, CRP, PCT e IL-6, así como una mayor tasa de mortalidad y niveles más bajos de PCIS se encontraron en pacientes con menor SIRT6 en comparación con los padres con mayor SIRT6. SIRT6 tenía potencial para el diagnóstico de NAC grave. CONCLUSIÓN: La SIRT6 regulada a la baja en pacientes infantiles con NAC grave predijo una mayor expresión de factores inflamatorios, resultados clínicos más graves y mal pronóstico.


Assuntos
Infecções Comunitárias Adquiridas , Pneumonia , Sirtuínas , Humanos , Criança , Interleucina-6 , Pró-Calcitonina , Proteína C-Reativa/análise , Biomarcadores , Prognóstico
17.
Environ Sci Pollut Res Int ; 29(37): 56379-56392, 2022 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-35334050

RESUMO

Carbon quantum dots (CQDs) can be used to modify TiO2 to extend the light absorption threshold and enhance its photocatalytic efficiency. In this study, different amounts of CQDs modified TiO2 (CQDs-x/TiO2) were synthesized by a facile, mild, and environmental friendly hydrothermal method at a low temperature. The physicochemical properties were investigated by a variety of advanced characterization techniques. It was found that the anchoring of CQDs endowed the CQDs-x/TiO2 with a large specific surface area, which is beneficial to adsorb more organic pollutants and promote the rate of photocatalytic oxidation. The XRD results also showed that the in situ formation of CQDs on the surface of TiO2 made the crystallinity of TiO2 tend to be complete. Among these photocatalysts, CQDs-20/TiO2 showed the highest pollutant removal efficiency under visible light irradiations. The classical quenching tests revealed that the O2•-, •OH, and hole (h+) were the oxidizing species. Among them, h+ was the primary factor contributing to the degradation. The electrochemical tests showed that the anchoring of CQDs on TiO2 increased the photocurrent by about four times, as compared with the pure TiO2. In particular, the cyclic voltammetry results showed that the photo-generated electrons of CQDs were freer to transfer to TiO2 under visible light irradiations, promoting the separation of photo-generated electrons and holes. This study explains adequately why the CQDs/TiO2 system has a good photocatalytic degradation of organic compounds.

18.
J Hazard Mater ; 423(Pt A): 127083, 2022 02 05.
Artigo em Inglês | MEDLINE | ID: mdl-34488092

RESUMO

Porous carbon serves as a green material for efficient wastewater purification by adsorption and advanced oxidation processes. However, a clear understanding of the simultaneous removal of multiple pollutants in water is still ambiguous. Herein, the synergistic effect of adsorption and peroxydisulfate (PS) activation on kinetics and mechanism of removing single and binary antibiotic pollutants, sulfamethoxazole (SMX) and ibuprofen (IBP), from water by biomass-derived N-doped porous carbon was investigated. Our findings suggest that adsorption contributed to efficient removals of SMX/IBP. Comparative quenching experiments and electrochemical analysis demonstrated that hydroxyl (•OH) and sulfate (SO4•-) radicals, as well as singlet oxygen (1O2) led to the catalytic degradation of SMX, while only 1O2 reacted for IBP oxidation. Superoxide ion (O2•-) radicals were not related to SMX/IBP degradation. Electron transfer pathway accounted for PS activation but was not involved in direct SMX/IBP oxidation. Only slight differences were found between the degradation kinetics of SMX and IBP in the binary and single SMX or IBP solutions. This arose from the non-selective effect of adsorption and 1O2 attack for SMX/IBP removal, and the weak selective oxidation process of SMX by •OH and SO4•-. This study provides a new viewpoint on the role of adsorption in catalysis and enriches the mechanistic study of multi-component antibiotic degradation.


Assuntos
Carbono , Poluentes Químicos da Água , Adsorção , Antibacterianos , Cinética , Porosidade , Poluentes Químicos da Água/análise
19.
J Colloid Interface Sci ; 615: 865-875, 2022 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-35182856

RESUMO

Rational design with fine-tuning of the electrocatalyst material is vital for achieving the desired sensitivity, selectivity, and stability for an electrochemical sensor. In this study, a three-dimensional (3D) hierarchical core-shell catalyst was employed as a self-standing, binder-free electrode for non-enzymatic glucose sensing. The catalyst was prepared by decorating the shell of NiFe layered double hydroxide (LDH) nanosheets (NSs) on the core of Cu nanowires (NWs) grown on a Cu foam support. The optimized 3D core-shell Cu@NiFe LDH sensor demonstrated higher sensitivity (7.88 mA mM-1cm-2), lower limit of detection (0.10 µM) and wider linear range (1 µM to 0.9 mM) in glucose sensing with a low working potential (0.4 V). The applied sensor also showed excellent stability, reproducibility, interference ability as well as practicability in real environment. The detection of real samples further suggests its great feasibility for practical applications. The superior electrocatalytic performance is collectively ascribed to the excellent electro-conductivity of the Cu substrate, the distinct self-standing 3D porous nanostructure, the ultrathin homogenous architecture, and the appropriate loading amount of NiFe LDH NSs. This study then provides a non-enzymatic glucose sensor with 3D Cu@NiFe LDH electrode for ultrahigh sensitivity and stability.


Assuntos
Glucose , Nanofios , Eletrodos , Glucose/química , Hidróxidos , Nanofios/química , Reprodutibilidade dos Testes
20.
J Hazard Mater ; 434: 128866, 2022 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-35413519

RESUMO

Solar-driven advanced oxidation processes (AOPs) via direct photodegradation or indirect photocatalytic activation of typical oxidants, such as hydrogen peroxide (H2O2), peroxymonosulfate (PMS), and peroxydisulfate (PDS), have been deemed to be an efficient technology for wastewater remediation. Artificial Z-scheme structured materials represent a promising class of photocatalysts due to their spatially separated charge carriers and strong redox abilities. Herein, we summarize the development of metal-free graphitic carbon nitride (g-C3N4, CN)-based direct and indirect Z-scheme photocatalysts for solar-driven AOPs in removing organic pollutants from water. In the work, the classification of AOPs, definition and validation of Z-schemes are summarized firstly. The innovative engineering strategies (e.g., morphology and dimensionality control, element doping, defect engineering, cocatalyst loading, and tandem Z-scheme construction) over CN-based direct Z-scheme structure are then examined. Rational design of indirect CN-based Z-scheme systems using different charge mediators, such as solid conductive materials and soluble ion pairs, is further discussed. Through examining the relationship between the Z-scheme structure and activity (charge transfer and separation, light absorption, and reaction kinetics), we aim to provide more insights into the construction strategies and structure modification on CN-based Z-schemes towards improving their catalytic performances in AOPs. Lastly, limitations, challenges, and perspectives on future development in this emerging field are proposed.

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