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Generation of novel n-p-n (CeO2-PPy-ZnO) heterojunction for photocatalytic degradation of micro-organic pollutants
2022
Rajendran, Saravanan | Hoang, Tuan K.A. | Trudeau, Michel L. | Jalil, A.A. | Naushad, Mu | Awual, Md Rabiul
Recently, hetero junction materials (p-n-p and n-p-n) have been developed for uplifting the visible light activity to destroy the harmful pollutants in wastewater. This manuscript presents a vivid description of novel n-p-n junction materials namely CeO₂-PPy-ZnO. This novel n-p-n junction was applied as the photocatalyst in drifting the mobility of charge carriers and hence obtaining the better photocatalytic activity when compared with p-n and pure system. Such catalyst's syntheses were successful via the copolymerization method. The structural, morphological and optical characterization techniques were applied to identify the physio-chemical properties of the prepared materials. Additionally, the superior performance of this n-p-n nanostructured material was demonstrated in the destruction of micro organic (chlorophenol) toxic wastes under visible light. The accomplished ability of the prepared catalysts (up to 92% degradation of chlorophenol after 180 min of irradiation) and their profound degradation mechanism was explained in detail.
Show more [+] Less [-]Assessing the potential to use CDOM as an indicator of water quality for the sediment-laden Yellow river, China
2021
Li, Dianbao | Pan, Baozhu | Han, Xu | Li, Junhua | Zhu, Qingwei | Li, Ming
Chromophoric dissolved organic matter (CDOM) in rivers is mainly affected by natural conditions and human activities and can reflect the watershed pollution status to a certain extent. The Yellow River is one of the largest contributors to the global riverine sediment flux from the land to ocean, and there is a paucity of information on how the optical properties of CDOM have the potential to serve as an indicator of water quality for the sediment-laden Yellow River. In this study, a three-dimensional fluorescence parallel factor (PARAFAC) analysis method was applied to investigate the seasonal and spatial variations in CDOM fluorescence components and spectral characteristics from the source region to the estuary in the mainstream of Yellow River. The relationships of CDOM with water quality indicators and trophic state were also analyzed. Six PARAFAC components (C1–C6) were identified and grouped into two categories: humic-like components (C1–C4), which accounted for 85.8 %, and protein-like components (C5 and C6), which accounted for only 14.2 %. The CDOM components, spectral parameters, and their clear correlations with the main ions (Na⁺ and Cl⁻) all indicated that the humic-like components may be primarily derived from nonpoint source erosion, and the protein-like components were mainly derived from point source discharges in the watershed. The combination of the CDOM absorption coefficient at 254 nm (a(254)), spectral slope ratio (SR), specific UV absorbance SUVA₂₅₄, and fluorescence index (FI) had a good predictive ability for the key water quality indicators (total nitrogen (TN), dissolved total nitrogen (DTN), total phosphorus (TP), dissolved total phosphorus (DTP), and chlorophyll a (Chl a)) and trophic state index (TSI). Therefore, some fluorophores and UV spectral parameters of CDOM in the Yellow River can be used for rapid water quality monitoring and pollution source indication, especially pollutants related to nitrogen and phosphorus nutrients in the basin.
Show more [+] Less [-]Synthesis and photocatalytic degradation activities of phosphorus containing ZnO microparticles under visible light irradiation for water treatment applications
2020
Saffari, Reyhaneh | Shariatinia, Zahra | Jourshabani, Milad
A series of phosphorus containing ZnO (P–ZnO) photocatalysts with various percentages of phosphorus were successfully synthesized using the hydrothermal method. The structural, physical and optical properties of the obtained microparticles were investigated using diverse techniques such as X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, ultraviolet–visible diffusion reflectance spectroscopy (UV–Vis DRS), photoluminescence (PL) spectroscopy, transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDS) and N₂ adsorption-desorption analysis. The photocatalytic activities of the pure and P–ZnO samples were evaluated for the degradation of Rhodamine B (RhB) under visible light irradiation. The parameters such as pH, catalyst dosage, contaminant concentration and effect of persulfate as an oxidant were studied. It was found that the P–ZnO1.8% photocatalyst could destroy 99% of RhB (5 ppm) in 180 min at pH = 7; furthermore, it degraded ∼100% of 5 and 10 ppm of the RhB pollutant in 120 and 180 min, respectively, only by adding 0.01 g of persulfate into the reaction solution. To determine the photocatalytic mechanism, 2-propanol, benzoquinone and EDTA were used and it was indicated that hydroxyl radicals, superoxide ions and holes, all had major roles in the photocatalytic degradation but the hydroxyl radical effect was the most significant. The phenol degradation was also investigated using the P–ZnO1.8% optimum photocatalyst which could destroy 53% of the phenol (5 ppm) in 180 min. According to the reusability test, it was proved that after 5 cycles, the catalyst activity was not highly changed and it was potentially capable of pollutant degradation.
Show more [+] Less [-]Vertical distribution of smoke aerosols over upper Indo-Gangetic Plain
2020
Attenuated backscatter profiles retrieved by the space borne active lidar CALIOP on-board CALIPSO satellite were used to measure the vertical distribution of smoke aerosols and to compare it against the ECMWF planetary boundary layer height (PBLH) over the smoke dominated region of Indo-Gangetic Plain (IGP), South Asia. Initially, the relative abundance of smoke aerosols was investigated considering multiple satellite retrieved aerosol optical properties. Only the upper IGP was selectively considered for CALIPSO retrieval based on prevalence of smoke aerosols. Smoke extinction was found to contribute 2–50% of the total aerosol extinction, with strong seasonal and altitudinal attributes. During winter (DJF), smoke aerosols contribute almost 50% of total aerosol extinction only near to the surface while in post-monsoon (ON) and monsoon (JJAS), relative contribution of smoke aerosols to total extinction was highest at about 8 km height. There was strong diurnal variation in smoke extinction, evident throughout the year, with frequent abundance of smoke particles at lower height (<4 km) during daytime compared to higher height during night (>4 km). Smoke injection height also varied considerably during rice (ON: 0.71 ± 0.65 km) and wheat (AM: 2.34 ± 1.34 km) residue burning period having a significant positive correlation with prevailing PBLH. Partitioning smoke AOD against PBLH into the free troposphere (FT) and boundary layer (BL) yield interesting results. BL contribute 36% (16%) of smoke AOD during daytime (nighttime) and the BL-FT distinction increased particularly at night. There was evidence that despite travelling efficiently to FT, major proportion of smoke AOD (50–80%) continue to remain close to the surface (<3 km) thereby, may have greater implications on regional climate, air quality, smoke transport and AOD-particulate modelling.
Show more [+] Less [-]Light absorption properties of elemental carbon (EC) and water-soluble brown carbon (WS–BrC) in the Kathmandu Valley, Nepal: A 5-year study
2020
Chen, Pengfei | Kang, Shichang | Tripathee, Lekhendra | Ram, Kirpa | Rupakheti, Maheswar | Panday, Arnico K. | Zhang, Qianggong | Guo, Junming | Wang, Xiaoxiang | Pu, Tao | Li, Yizhong
This study presents a comprehensive analysis of organic carbon (OC), elemental carbon (EC), and particularly the light absorption characteristics of EC and water-soluble brown carbon (WS–BrC) in total suspended particles in the Kathmandu Valley from April 2013 to January 2018. The mean OC, EC, and water-soluble organic carbon (WSOC) concentrations were 34.8 ± 27.1, 9.9 ± 5.8, and 17.4 ± 12.5 μg m⁻³, respectively. A clear seasonal variation was observed for all carbonaceous components with higher concentrations occurring during colder months and lower concentrations in the monsoon season. The relatively low OC/EC ratio (3.6 ± 2.0) indicates fossil fuel combustion as the primary source of carbonaceous components. The optical attenuation (ATN) at 632 nm was significantly connected with EC loading (ECS) below 15 μg cm⁻² but ceased as ECS increased, reflecting the increased influence of the shadowing effect. The derived average mass absorption cross-section of EC (MACEC) (7.0 ± 4.2 m² g⁻¹) is comparable to that of freshly emitted EC particles, further attesting that EC was mainly produced from local sources with minimal atmospheric aging processes. Relatively intensive coating with organic aerosols and/or salts (e.g., sulfate, nitrate) was probably the reason for the slightly higher MACEC during the monsoon season, whereas increased biomass burning was a major factor leading to lower MACEC in other seasons. The average MACWS₋BᵣC at 365 nm was 1.4 ± 0.3 m² g⁻¹ with minimal seasonal variations. In contrast to MACEC, biomass burning was the main reason for a higher MACWS₋BᵣC in the non-monsoon season. The relative light absorption contribution of WS-BrC to EC was 9.9% over the 300–700 nm wavelength range, with a slightly higher ratio (13.6%) in the pre-monsoon season. Therefore, both EC and WS-BrC should be considered in the study of optical properties and radiative forcing of carbonaceous aerosols in this region.
Show more [+] Less [-]Adhesion of CdTe quantum dots on model membranes and internalization into RBL-2H3 cells
2017
Zhang, Mengmeng | Wei, Xiaoran | Ding, Lei | Hu, Jingtian | Jiang, Wei
Quantum dots (QDs) have attracted broad attention due to their special optical properties and promising prospect in medical and biological applications. However, the process of QDs on cell membrane is worth further investigations because such process may lead to harmful effects on organisms and also important for QD application. In this study, adhesion of amino- and carboxyl-coated CdTe QDs (A-QDs and C-QDs) on cell membrane and the subsequent internalization are studied using a series of endocytosis-free model membranes, including giant and small unilamellar vesicles, supported lipid bilayers and giant plasma membrane vesicles (GPMVs). The adhered QD amounts on model membranes are quantified by a quartz crystal microbalance. The CdTe QD adhesion on model membranes is governed by electrostatic forces. Positively charged A-QDs adhere on GPMV surface and passively penetrate the plasma membrane via endocytosis-free mechanism, but negatively charged C-QDs cannot. Rat basophilic leukemia (RBL-2H3) cells are exposed to CdTe QDs to monitor the QD internalization process. Both A- and C-QDs are internalized by RBL-2H3 cells mainly via endocytosis. CdTe QDs do not accumulate on the plasma membrane of living cells due to the fast endocytosis and the weakened electrostatic attraction in biological medium, resulting in low chance of passive penetration. The suspended cells after trypsin digestion take more QDs than the adherent cells. A-QDs cause lower cell viability than C-QDs, probably because the approach of positively charged QDs to cells is favored and the smaller aggregates of A-QDs.
Show more [+] Less [-]Traceability of fluorescent engineered nanomaterials and their fate in complex liquid waste matrices
2016
Part, Florian | Zaba, Christoph | Bixner, Oliver | Zafiu, Christian | Hann, Stephan | Sinner, Eva-Kathrin | Huber-Humer, Marion
The number of products containing engineered nanomaterials (ENMs) has increased due to their high industrial relevance as well as their use in diverse consumer products. At the end of their life cycle ENMs might be released to the environment and therefore concerns arise regarding their environmental impact. In order to track their fate upon disposal, it is crucial to establish methods to trace ENMs in complex environmental samples and to differentiate them from naturally-occurring nanoparticles. The goal of this study was to distinctively trace ENMs by (non-invasive) detection methods. For this, fluorescent ENMs, namely quantum dots (QDs), were distinctively traced in complex aqueous matrices, and were still detectable after a period of two months using fluorescence spectroscopy. In particular, two water-dispersible QD-species, namely CdTe/CdS QDs with N-acetyl-l-cysteine as capping agent (NAC-QDs) and surfactant-stabilized CdSe/ZnS QDs (Brij®58-QDs), were synthesized to examine their environmental fate during disposal as well as their potential interaction with naturally-occurring substances present in landfill leachates. When QDs were spiked into a leachate from an old landfill site, alteration processes, such as sorption, aggregation, agglomeration, and interactions with dissolved organic carbon (DOC), led to modifications of the optical properties of QDs. The spectral signatures of NAC-QDs deteriorated depending on residence time and storage temperature, while Brij®58-QDs retained their photoluminescence fingerprints, indicating their high colloidal stability. The observed change in photoluminescence intensity was mainly caused by DOC-interaction and association with complexing agents, such as fulvic or humic acids, typically present in mature landfill leachates. For both QD-species, the results also indicated that pH of the leachate had no significant impact on their optical properties. As a result, the unique spectroscopic fingerprints of QDs, specifically surfactant-stabilized QDs, allowed distinctive tracing in complex aqueous waste matrices in order to study their long-term behavior and ultimate fate.
Show more [+] Less [-]Improvement of aerosol optical properties modeling over Eastern Asia with MODIS AOD assimilation in a global non-hydrostatic icosahedral aerosol transport model
2014
Dai, Tie | Schutgens, Nick A.J. | Gotō, Daisuke | Shi, Guangyu | Nakajima, Teruyuki
A new global aerosol assimilation system adopting a more complex icosahedral grid configuration is developed. Sensitivity tests for the assimilation system are performed utilizing satellite retrieved aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS), and the results over Eastern Asia are analyzed. The assimilated results are validated through independent Aerosol Robotic Network (AERONET) observations. Our results reveal that the ensemble and local patch sizes have little effect on the assimilation performance, whereas the ensemble perturbation method has the largest effect. Assimilation leads to significantly positive effect on the simulated AOD field, improving agreement with all of the 12 AERONET sites over the Eastern Asia based on both the correlation coefficient and the root mean square difference (assimilation efficiency). Meanwhile, better agreement of the Ångström Exponent (AE) field is achieved for 8 of the 12 sites due to the assimilation of AOD only.
Show more [+] Less [-]Ultraviolet absorbance as a proxy for total dissolved mercury in streams
2009
Dittman, Jason A. | Shanley, James B. | Driscoll, Charles T. | Aiken, George R. | Chalmers, Ann T. | Towse, Janet E.
Stream water samples were collected over a range of hydrologic and seasonal conditions at three forested watersheds in the northeastern USA. Samples were analyzed for dissolved total mercury (THgd), DOC concentration and DOC composition, and UV₂₅₄ absorbance across the three sites over different seasons and flow conditions. Pooling data from all sites, we found a strong positive correlation of THgd to DOC (r² = 0.87), but progressively stronger correlations of THgd with the hydrophobic acid fraction (HPOA) of DOC (r² = 0.91) and with UV254 absorbance (r² = 0.92). The strength of the UV₂₅₄ absorbance-THgd relationship suggests that optical properties associated with dissolved organic matter may be excellent proxies for THgd concentration in these streams. Ease of sample collection and analysis, the potential application of in-situ optical sensors, and the possibility for intensive monitoring over the hydrograph make this an effective, inexpensive approach to estimate THgd flux in drainage waters. Ultraviolet absorbance measurements are a cost-effective proxy to estimate dissolved mercury concentration in stream water.
Show more [+] Less [-]Predictive role of spectral slope ratio towards 17α-ethynylestradiol photodegradation sensitized by humic acids
2019
Ren, Dong | Ren, Zhaogang | Chen, Fang | Wang, Bin | Huang, Bin
Humic acids (HAs) have been shown to dominate the photodegradation of steroid estrogens in natural waters. Nevertheless, how the photosensitizing ability of HAs relates to their structural and optical characteristics remains largely unknown. In this study, 17α-ethynylestradiol (EE2) was selected as a model compound to study to what extent easily-measurable characteristics of HAs might be used to predict their photosensitization potency. HAs were extracted from sediments of two different sources, and then subjected to structural and optical properties characterization using elemental analyzer, UV–vis spectroscopy and fluorescence spectroscopy. Photochemical experiments show that the HAs from the two sources can effectively meditate EE2 photodegradation. Although with drastically different structural and optical properties, the photosensitizing ability of these HAs towards EE2 can be well described by simple linear regressions using a spectroscopic index, the spectral slope ratio (SR). This optical indicator is correlated with various physicochemical properties of HAs, including the molecular weight, lignin content, charge-transfer interaction potential, photobleaching extent and sources. No universal prediction model could be established for predicting EE2 photodegradation kinetics on the basis of SR, but in specific waters SR could be a powerful indictor for predicting the EE2 photodegradation sensitized by HAs.
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