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1.
J Environ Manage ; 358: 120902, 2024 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-38657411

RESUMO

Poorly managed faecal sludge (FS) poses significant challenges to public health and the environment. Anaerobic digestion (AD) of FS provides an effective method for energy recovery while reducing FS associated threats. Recognizing the critical role of the dewatering process before AD, this study investigates the synergistic application of chemical coagulation and mesophilic AD for synthetic FS treatment. FeCl3, AlCl3, Fe2(SO4)3, poly ferric sulfate (PFS) and poly aluminium ferric chloride (PAFC) were utilized at varying dosages to examine their impact on FS properties and subsequent biogas production from the dewatered FS. It was found that coagulation enhances sedimentation efficiencies and dewaterability through mechanisms such as charge neutralization, charge patching and bridging, thereby improving the FS feasibility for AD. Notably, polymer coagulant PFS showed good performance in balancing pollutant removal and methane recovery, contributing to facilitating the hydrolysis and acidogenesis microorganisms involved in the AD process. Optimal dosage was identified at 150 mg/g TS (1.7 g/L FS), achieving prominent removal efficiencies for total COD (67%), turbidity (85%), and total phosphorus (60%), while simultaneously enhancing AD performance with specific CH4 production reaching 517 ml CH4/g VS or 24.8 ml CH4/g AD wet feedstock compared to 309 ml CH4/g VS or 2.7 ml CH4/g AD wet feedstock in untreated FS.

2.
Adv Sci (Weinh) ; : e2309555, 2024 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-38502881

RESUMO

Photo-rechargeable zinc-ion batteries (PRZIBs) have attracted much attention in the field of energy storage due to their high safety and dexterity compared with currently integrated lithium-ion batteries and solar cells. However, challenges remain toward their practical applications, originating from the unsatisfactory structural design of photocathodes, which results in low photoelectric conversion efficiency (PCE). Herein, a flexible MoS2 /SnO2 -based photocathode is developed via constructing a sunflower-shaped light-trapping nanostructure with 3D hierarchical and self-supporting properties, enabled by the hierarchical embellishment of MoS2 nanosheets and SnO2 quantum dots on carbon cloth (MoS2 /SnO2 QDs@CC). This structural design provides a favorable pathway for the effective separation of photogenerated electron-hole pairs and the efficient storage of Zn2+ on photocathodes. Consequently, the PRZIB assembled with MoS2 /SnO2 QDs@CC delivers a desirable capacity of 366 mAh g-1 under a light intensity of 100 mW cm-2 , and achieves an ultra-high PCE of 2.7% at a current density of 0.125 mA cm-2 . In practice, an integrated battery system consisting of four series-connected quasi-solid-state PRZIBs is successfully applied as a wearable wristband of smartwatches, which opens a new door for the application of PRZIBs in next-generation flexible energy storage devices.

3.
Environ Sci Pollut Res Int ; 31(13): 19687-19698, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38366321

RESUMO

As a visible-light response semiconductor materials, bismuth vanadate (BiVO4) is extensively applied in photodegradation organic dye field. In this study, we synthesized C3N5 nanosheets and coupled with decahedral BiVO4 to construct a Z-scheme C3N5/BiVO4 heterostructure with close interface contact. By introducing C3N5 into BiVO4, the built Z-scheme transfer pathway provides silky channel for charge carrier migration between different moieties and enables photoexcited electrons and holes accumulated on the surface of BiVO4 and C3N5. The accelerated separation of charge carriers ensures C3N5/BiVO4 heterostructures with a powerful oxidation capacity compared with pure BiVO4. Due to the synergistic effect in Z-scheme heterostructure, the C3N5/BiVO4 demonstrated an improved photodegradation ability of rhodamine B (RhB) and methylene blue (MB) that of bare BiVO4.


Assuntos
Luz , Semicondutores , Catálise , Fotólise , Azul de Metileno/química
4.
Langmuir ; 39(48): 17458-17470, 2023 12 05.
Artigo em Inglês | MEDLINE | ID: mdl-37989129

RESUMO

The construction of Z-scheme heterostructures using matching band semiconductors is an effective strategy for producing highly efficient photocatalysts. In this study, MgIn2S4(MIS) was grown in situ on In2O3 microrods created with an In-based MOF material (In-MIL-68) as a template to successfully establish a unique MIS-In2O3 heterojunction with a well-matched Z-scheme interface charge transfer channel. Tetracycline (TC) as a typical antibiotic was chosen as the target pollutant to evaluate the photocatalytic activity. After 120 min of visible light irradiation, the MIS-In2O3-(10:1) material had the greatest photocatalytic degradation activity of tetracycline with 96.55%, which was 2.39 and 4.26 times that of MIS and In2O3, respectively. The improved photocatalytic activity is attributed to the in situ growth of MIS on In2O3, forming a Z-scheme heterojunction at the interface, which not only increases the specific surface area, exposes the abundant active site, and improves light utilization but also facilitates the migration and separation of photogenic carriers. The photocatalytic degradation products of TC were detected by liquid chromatography-mass spectrometry (LC-MS), and a preliminary degradation pathway was proposed. Radical capture experiments and ESR analysis confirmed that the main active species were holes (h+), superoxide radicals (•O2-), and superoxide and hydroxyl radicals (•OH). Finally, combined with band position analysis, this study proposes a direct Z-scheme heterojunction mechanism to improve the photocatalytic degradation of tetracycline in MIS under visible light.


Assuntos
Superóxidos , Tetraciclina , Antibacterianos , Radical Hidroxila , Luz
5.
J Colloid Interface Sci ; 651: 948-958, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37579669

RESUMO

To effectively separate electron-hole pairs produced by light, a heterojunction arrangement can be employed, thereby improving photocatalytic efficiency. In this study, a simple hydrothermal process is used to manufacture carbonized polymer dots/ZnIn2S4 (CPDs/ZIS) heterostructure, which enhances the light absorption and charge carrier lifetime in comparison to bare ZnIn2S4 (ZIS). Upon irradiation with visible light, the 3-CPDs/ZIS composite generates hydrogen at a rate of 133 µmol g-1 h-1, which is 8.9 times faster than that of pure ZIS. The addition of CPDs can increase the range of light that can be absorbed, extend the service life of the optical charge, increase the specific surface area, and promote charge separation and transmission, which could effectively accelerate the photocatalytic reduction reaction. The presence of CPDs results in the introduction of multiple transition energy states and a decrease in the H* adsorption free energy, which enhances the hydrogen evolution activity according to the theoretical calculation findings of density functional theory (DFT) and Gibbs free energy of the hydrogen evolution process. Combining theoretical calculations and experimental results, a direct Z-type heterojunction mechanism is proposed for the hydrogen evolution promotion effectiveness of CPDs/ZIS under visible light.

6.
Small ; 19(28): e2301323, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-36988022

RESUMO

The pinhole-free and defect-less perovskite film is crucial for achieving high efficiency and stable perovskite solar cells (PSCs), which can be prepared by widely used anti-solvent crystallization strategies. However, the involvement of anti-solvent requires precise control and inevitably brings toxicity in fabrication procedures, which limits its large-scale industrial application. In this work, a facile and effective co-solvent engineering strategy is introduced to obtain high- quality perovskite film while avoiding the usage of anti-solvent. The uniform and compact perovskite polycrystalline films have been fabricated through the addition of co-solvent that owns strong coordination capacity with perovskite components , meanwhile possessing the weaker interaction with main solvent . With those strategies, a champion power conversion efficiency (PCE) of 22% has been achieved with the optimal co-solvent, N-methylpyrrolidone (NMP) and without usage of anti-solvent. Subsequently, PSCs based on NMP show high repeatability and good shelf stability (80% PCE remains after storing in ambient condition for 30 days). Finally, the perovskite solar module (5 × 5 cm) with 7 subcells connects in series yielding champion PCE of 16.54%. This strategy provides a general guidance of co-solvent selection for PSCs based on anti-solvent free technology and promotes commercial application of PSCs.

7.
Chemistry ; 29(21): e202203917, 2023 Apr 13.
Artigo em Inglês | MEDLINE | ID: mdl-36647269

RESUMO

It has been rarely reported the morphological control of derivatives of metal-organic frameworks (MOFs) in hydrothermal conditions for photocatalytic applications. We report here a family of highly efficient composite photocatalysts composed of terephthalic acid/terephthalate (TPA) ligand and TiO2 with various morphologies (e. g., nanoparticles, nanosheets, and nanorods). The composites are synthesized by a simple one-step hydrothermal method in various solvents (i. e., H2 O, HF, H2 SO4 , HCl, and HNO3 ) using Ti-based MOF (MIL-125(Ti)) as precursor. The formation mechanism of composite materials with different morphological features is discussed. Impressively, the composite of TiO2 nanoparticles/TPA synthesized using H2 O as solvent under hydrothermal condition exhibits the highest photocatalytic H2 activity among the studied materials, with a photocatalytic H2 production rate of 6.38 mmol g-1 h-1 , which is approximately 7.5-fold higher than pure TiO2 (Degussa, P25) and prominent apparent quantum efficiency (AQE) of 65 % at 365 nm. Furthermore, the mechanism of boosted photocatalytic H2 production is discussed.

8.
Dalton Trans ; 51(42): 16389-16396, 2022 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-36250669

RESUMO

Introducing piezoelectric materials with the built-in electric field caused by mechanical force has been confirmed as an effective strategy to boost the separation efficiency of photoexcited charge carriers that determines the photocatalytic performance. In this study, we introduced Bi4Ti3O12 with superior piezoelectric properties into BiVO4-Bi4V2O10 materials to synthesize a 2D Bi4Ti3O12-BiVO4-Bi4V2O10 photocatalyst via a facile hydrothermal method. Compared with bare BiVO4, the Bi4Ti3O12-BiVO4-Bi4V2O10 piezo-photocatalytic activity towards Cr(VI) removal and oxygen evolution is boosted remarkably under both illumination and ultrasound treatments. The promoted photocatalytic activity can be ascribed to the accelerated photoexcited carrier separation efficiency driven by the polarization electric field and the synergy effect in the heterostructure. This work provides a simple and sustainable strategy for the design and development of piezo-photocatalysts with high photoredox activity capacity.

9.
Langmuir ; 38(24): 7558-7566, 2022 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-35666859

RESUMO

Bismuth vanadate (BiVO4) is a promising photocatalyst for water pollution degradation and photocatalytic oxygen evolution. In this work, we prepared 2D/2D BiVO4-Bi4V2O10 heterostructure with tight interfacial contact via a facile one-step hydrothermal process. The crystal structure and morphology of the samples could be easily regulated by changing the pH values of the solution. The BiVO4-Bi4V2O10 heterostructure exhibited an enhanced photodegradation rate of Cr(VI) and oxygen evolution that of bare BiVO4, indicating that the synergistic effect and the interfacial fusions between BiVO4 and Bi4V2O10 can effectively promote the migration and separation rate of photoexcited charge carriers.

10.
J Colloid Interface Sci ; 625: 128-135, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35716608

RESUMO

The development of hydrogen energy is limited by the high cost of platinum group metals (PGM). There is an urgent need to design efficient PGM-free electrocatalysts in the hydrogen electrode. Herein, Janus Ni/W bimetallic materials are proposed as an effective PGM-free bifunctional hydrogen electrocatalyst. By constructing the bimetallic materials, a synergistic effect is realized to enhance the reaction kinetics and improve the catalytic performance. In general, Ni can provide excellent Had sites, and W serves as OHad sites. Therefore, the synergistic effect of Ni and W can improve the kinetics of hydrogen evolution reaction and the hydroxide oxidation reaction. Ni/W@NF can obtain the hydrogen evolution reaction current density of 10 mA cm-2 with an overpotential of only 62.6 mV, and the exchange current density of hydroxide oxidation reaction can reach 1.83 mA cm-2. This work provides a new idea for the design of high-efficiency and low-cost PGM-free bifunctional hydrogen electrocatalysts.

12.
ACS Appl Mater Interfaces ; 13(33): 39470-39479, 2021 Aug 25.
Artigo em Inglês | MEDLINE | ID: mdl-34433246

RESUMO

Hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR) have aroused great interest, but the high price of platinum group metals (PGMs) limits their development. The electronic reconstruction at the interface of a heterostructure is a promising strategy to enhance their catalytic performance. Here, MoO2/Ni heterostructure was synthesized to provide effective HER in an alkaline electrolyte and exhibit excellent HOR performance. Theoretical and experimental analyses prove that the electron density around the Ni atom is reduced. The electron density modulation optimizes the hydrogen adsorption and hydroxide adsorption free energy, which can effectively improve the activity of both HER and HOR. Accordingly, the prepared MoO2/Ni@NF catalyst reveals robust HER activity (η10 = 50.48 mV) and HOR activity (j0 = ∼1.21 mA cm-2). This work demonstrates an effective method to design heterostructure interfaces and tailor the surface electronic structure to improve HER/HOR performance.

13.
Dalton Trans ; 47(35): 12406-12413, 2018 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-30128445

RESUMO

Crystalline materials with multi-catalytic applications are of great value to both fundamental research and practical applications. The platform of metal-organic frameworks (MOFs) is utilized to fabricate a microporous versatile catalyst with high stability. Self-assembly of a flexible ligand, 4-(4-carboxybenzylamino)benzoic acid (H2CBBA), with Co(ii) resulted in a 3D framework, CBBA-Co, with Co3O clusters exposed in the zigzag channels. Upon in situ activation, CBBA-Co exhibited multiple heterogeneous catalytic activities. Theoretical calculations were carried out to give insights into the catalytic process. In addition, CBBA-Co also showed promising potential in optical sensing by virtue of its catalytic activity. The luminol chemiluminescence was greatly enhanced by CBBA-Co, and linear determination of the concentration of H2O2 in the range of 0-30% was established. The successful implementation of CBBA-Co indicates the feasibility and promising future of employing MOFs as an efficient platform for the fabrication and study of multifunctional catalysts, both experimentally and theoretically.

14.
Bioresour Technol ; 241: 1003-1011, 2017 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-28637158

RESUMO

The silage quality and anaerobic digestion performance of Pennisetum purpereum with molasses-processed wastewater addition were assessed. The silage samples with molasses-processed wastewater addition obtained higher lactic acid concentration of 15.18-23.38mg/g FM, lower pH value of 3.96-4.45 and lower NH3-N content of 0.47-0.64mg/g FM. No obvious difference was observed in the dominant phyla and genus, but the relative abundance of Lactobacillus reached up to 77.39%, increased by 84% compared to the silage samples without molasses-processed wastewater addition. Combined the silage quality and bacterial community, the decreased in pH value of fresh material caused by molasses-processed wastewater addition was the main reason for improving the silage quality. Meanwhile, the increased in COD concentration is beneficial for improving the specific methane yield and the maximum specific methane yield of 259±5.75mL/g VS was obtained with adding 20g/kg molasses-alcoholic wastewater. Molasses-processed wastewater is an alternative additive for silage.


Assuntos
Melaço , Silagem , Águas Residuárias , Fermentação , Pennisetum
15.
Chemistry ; 23(16): 3931-3937, 2017 Mar 17.
Artigo em Inglês | MEDLINE | ID: mdl-28120461

RESUMO

A 3D metal-organic framework (ADA-Cd=[Cd2 L2 (DMF)2 ]⋅3 H2 O where H2 L is (2E,2'E)-3,3'-(anthracene-9,10-diyl)diacrylic acid) constructed from diacrylate substituted anthracene, sharing structural characteristics with some frequently employed anthraquinone-type dye sensitizers, was introduced as an effective sensitizer for anatase TiO2 to achieve enhanced visible light photocatalytic performance. A facile mechanical mixing procedure was adopted to prepare the co-catalyst denoted as ADA-Cd/TiO2 , which showed enhanced photodegradation ability, as well as sustainability, towards several dyes under visible light irradiation. Mechanistic studies revealed that ADA-Cd acted as the antenna to harvest visible light energy, generating excited electrons, which were injected to the conduction band (CB) of TiO2 , facilitating the separation efficiency of charge carriers. As suggested by the results of control experiments, combined with the corresponding redox potential of possible oxidative species, . O2- , generated from the oxygen of ambient air at the CB of TiO2 was believed to play a dominant role over . OH and h+ . UV/Vis and photoluminescence technologies were adopted to monitor the generation of . O2- and . OH, respectively. This work presents a facile strategy to achieve a visible light photocatalyst with enhanced catalytic activity and sustainability; the simplicity, efficiency, and stability of this strategy may provide a promising way to achieve environmental remediation.

16.
Biosens Bioelectron ; 90: 276-282, 2017 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-27923190

RESUMO

The first two-photon fluorescent probe (PC) for selectively detecting biological Cu (Ⅱ) and pyrophosphate (PPi) has been developed based on 7-substituted coumarin in this study. The probe presented excellent selective two-photon "on-off-on" detection signal for Cu(II) /PPi in aqueous solution. The two-photon detection ensemble (PCCu) can detect PPi released from DNA amplification after the polymerase chain reactions (PCR). The probe showed low cytotoxicity and good biocompatibility, and therefore can be applied for imaging Cu(II)/PPi in living cells under two-photon excitation. Furthermore, the ensemble probe (PCCu) was also used to image PPi in deep living rat tissues (~100µm) and in 5-days old zebrafish.


Assuntos
Cobre/análise , Difosfatos/análise , Corantes Fluorescentes/química , Microscopia de Fluorescência por Excitação Multifotônica/métodos , Imagem Óptica/métodos , Animais , Técnicas Biossensoriais/métodos , DNA/química , Células HeLa , Humanos , Fígado/química , Fígado/ultraestrutura , Camundongos , Peixe-Zebra
17.
J Mater Chem B ; 5(15): 2743-2749, 2017 Apr 21.
Artigo em Inglês | MEDLINE | ID: mdl-32264160

RESUMO

A new two-photon fluorescent probe (MCN) for viscosity imaging was developed based on a 6-substituted quinoline framework. MCN showed an excellent "off-on" fluorescence response (ca. 90-fold enhancement) with viscosity increasing in the glycerol-water viscosity system. MCN showed great sensitivity to viscosity (R2 = 0.98, x = 0.65), which gave rise to cell imaging for micro-viscosity or real-time cell imaging during apoptosis with low cytotoxicity under two-photon excitation (λex = 800 nm). Fluorescence lifetime imaging (FLIM) of living HeLa cells stained with MCN revealed that the intracellular average viscosity value was 73.45 ± 21.55 cP in cytosol. Imaging in living tissue slices indicated that MCN can work in deep tissue (∼130 µM) under two-photon excitation. Moreover, MCN also showed the capacity for in vivo imaging viscosity in zebrafish with obvious fluorescence emission.

18.
Materials (Basel) ; 9(8)2016 Aug 11.
Artigo em Inglês | MEDLINE | ID: mdl-28773809

RESUMO

Monoclinic BiVO4 photocatalysts with porous structures were synthesized by a two-step approach without assistance of any templates. The as-prepared samples were characterized by X-ray diffraction pattern (XRD), scanning electron microscopy (SEM), Brunauer-Emmett-Teller (BET), ultraviolet-visible (UV-vis) diffuse reflectance spectroscopy (DRS), photocurrent responses, and electrochemical impedance spectra (EIS). It is found that the as-prepared BiVO4 samples had a porous structure with aperture diameter of 50-300 nm. Moreover, the BET specific surface area of the porous BiVO4-200 °C sample reaches up to 5.69 m²/g, which is much higher than that of the sample of BiVO4 particles without porous structure. Furthermore, a possible formation mechanism of BiVO4 with porous structure was proposed. With methylene blue (MB) as a model compound, the photocatalytic oxidation of organic contaminants in aqueous solution was investigated under visible light irradiation. It is found that the porous BiVO4-200 °C sample exhibits the best photocatalytic activity, and the photocatalytic rate constant is about three times of that of the sample of BiVO4 particles without porous structure. In addition, the photocurrent responses and electrochemical impedance spectra strongly support this conclusion.

19.
Materials (Basel) ; 9(12)2016 Nov 29.
Artigo em Inglês | MEDLINE | ID: mdl-28774088

RESUMO

Pristine Ag3PO4 microspheres were synthesized by a co-precipitation method, followed by being calcined at different temperatures to obtain a series of calcined Ag3PO4 photocatalysts. This work aims to investigate the origin of activity and stability enhancement for Ag3PO4 photocatalyst after calcination based on the systematical analyses of the structures, morphologies, chemical states of elements, oxygen defects, optical absorption properties, separation and transfer of photogenerated electron-hole pairs, and active species. The results indicate that oxygen vacancies (VO˙˙) are created and metallic silver nanoparticles (Ag NPs) are formed by the reaction of partial Ag⁺ in Ag3PO4 semiconductor with the thermally excited electrons from Ag3PO4 and then deposited on the surface of Ag3PO4 microspheres during the calcination process. Among the calcined Ag3PO4 samples, the Ag3PO4-200 sample exhibits the best photocatalytic activity and greatly enhanced photocatalytic stability for photodegradation of methylene blue (MB) solution under visible light irradiation. Oxygen vacancies play a significantly positive role in the enhancement of photocatalytic activity, while metallic Ag has a very important effect on improving the photocatalytic stability. Overall, the present work provides some powerful evidences and a deep understanding on the origin of activity and stability enhancement for the Ag3PO4 photocatalyst after calcination.

20.
Nanoscale ; 5(6): 2491-504, 2013 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-23411671

RESUMO

A series of Lu6O5F8:20%Yb(3+),1%Er(3+)(Tm(3+)),x%Li(+) (0 ≤ x ≤ 12) nanoparticles with average size from 20 to 320 nm upon increasing Li(+) concentration were prepared by a coprecipitation method. The detailed crystal structure of Lu6O5F8 as a new matrix is firstly analysed via retrieved refinement of the powder X-ray diffraction (XRD). In addition, the corresponding Powder Diffraction File card information was also obtained through indexing the XRD pattern of the host. Upconversion under excitation at 980 nm, downconversion with Xe lamp as excitation source and cathodoluminescence properties of Lu6O5F8:20%Yb(3+),1%Er(3+)(Tm(3+)),x%Li(+) (0 ≤ x ≤ 12) nanoparticles were compared and studied. It is worthwhile pointing out that according to the effects of Li(+) on emission intensity ratio, white UC emission was achieved in the Lu6O5F8:6%Yb(3+),0.3%Er(3+),0.4%Tm(3+),5%Li(+) compared to Li(+) free sample with the same activator concentration. The reasons behind this behavior were presented and discussed. All in all, Li(+) ion would be a wonderful luminescence intensifier for lanthanide ions, and the multifunctional lanthanide ion-doped Lu6O5F8 nanoparticles have potential application in photoluminescence areas and field emission display devices.

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