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Assessing the potential to use CDOM as an indicator of water quality for the sediment-laden Yellow river, China النص الكامل
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.
اظهر المزيد [+] اقل [-]Light absorption properties of elemental carbon (EC) and water-soluble brown carbon (WS–BrC) in the Kathmandu Valley, Nepal: A 5-year study النص الكامل
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.
اظهر المزيد [+] اقل [-]Significant restructuring and light absorption enhancement of black carbon particles by ammonium nitrate coating النص الكامل
2020
Yuan, Zheng | Zheng, Jun | Ma, Yan | Jiang, Youling | Li, Yilin | Wang, Ziqiong
Field observations have suggested that particulate nitrate can promote the aging of black carbon (BC), yet the mechanisms of the aging process and its impacts on BC’s light absorption are undetermined. Here we performed laboratory simulation of internal mixing of flame-generated BC aggregates with ammonium nitrate. Variations in particle size, mass, coating thickness, effective density, dynamic shape factor, and optical properties were determined online by a suite of instruments. With the development of coatings, the particle size initially decreased until reaching a coating thickness of ∼10 nm and then started increasing, accompanied by an increase in effective density and a decrease in dynamic shape factor, reflecting the transformation of BC particles from highly fractal to near-spherical morphology. This is partially attributable to the restructuring of BC cores to more compact forms. Exposing coated particles to elevated relative humidity (RH) led to additional BC morphology changes, even after drying. Particle light absorption and scattering were also amplified with ammonium nitrate coating, increasing with coating thickness and RH. For BC particles with a 17.8 nm coating, absorption and scattering were increased by 1.5- and 7.9-fold when cycled through 70% RH (5-70-5% RH), respectively. The irreversible restructuring of the BC core caused by condensation of ammonium nitrate and water altered both absorption and scattering, with a magnitude comparable to or even exceeding the effects of increased coating. Results show that ammonium nitrate is among the most efficient coating materials with respect to modifying BC morphology and optical properties compared with other inorganic and organic species investigated previously. Accordingly, mitigation of nitrate aerosols is necessary for the benefits of both air pollution control and reducing the impacts of BC on visibility impairment and radiative forcing on climate change. Our results also pointed out that the effect of BC core restructuring needs to be considered when evaluating BC’s light absorption enhancement.
اظهر المزيد [+] اقل [-]Vertical distribution of smoke aerosols over upper Indo-Gangetic Plain النص الكامل
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.
اظهر المزيد [+] اقل [-]Light absorption of organic carbon and its sources at a southeastern U.S. location in summer النص الكامل
2019
Xie, Mingjie | Chen, Xi | Holder, Amara L. | Hays, Michael D. | Lewandowski, Michael | Offenberg, John H. | Kleindienst, Tadeusz E. | Jaoui, Mohammed | Hannigan, Michael P.
Light-absorbing organic carbon (OC), also referred to as “brown carbon” (BrC), has been intensively investigated in atmospheres impacted by biomass burning. However, other BrC sources (e.g., secondary formation in the atmosphere) are rarely studied in ambient aerosols. In the current work, forty-five PM₂.₅ filter samples were collected in Research Triangle Park (RTP), NC, USA from June 1st to July 15th, 2013. The bulk carbonaceous components, including OC, elemental carbon (EC), water soluble OC (WSOC), and an array of organic molecular markers were measured; an ultraviolet/visible spectrometer was used to measure the light absorption of methanol extractable OC and WSOC. The average light absorption per OC and WSOC mass of PM₂.₅ samples in summer RTP are 0.36 ± 0.16 m² gC⁻¹ and 0.29 ± 0.13 m² gC⁻¹, respectively, lower than the ambient aerosol samples impacted by biomass burning and/or fossil fuel combustion (0.7–1.6 m² gC⁻¹) from other places. Less than 1% of the aqueous extracts absorption is attributed to the light-absorbing chromophores (nitroaromatic compounds) identified in this work. To identify the major sources of BrC absorption in RTP in the summer, Positive Matrix Factorization (PMF) was applied to a dataset containing optical properties and chemical compositions of carbonaceous components in PM₂.₅. The results suggest that the formation of biogenic secondary organic aerosol (SOA) containing organosulfates is an important BrC source, contributing up to half of the BrC absorption in RTP during the summertime.
اظهر المزيد [+] اقل [-]Dynamic variations in dissolved organic matter and the precursors of disinfection by-products leached from biochars: Leaching experiments simulating intermittent rain events النص الكامل
2018
Lee, Mi-Hee | Ok, Yong Sik | Hur, Jin
Biochar-leached dissolved organic matter may have a substantial impact on the water quality of receiving water surrounded by biochar-amended fields. In this study, we tracked variations in the spectroscopic characteristics and the disinfection by-products formation potentials of dissolved organic matter (DOM) leached during sequential extraction for three different biochars (BCs), which simulates DOM from BC-amended fields during intermittent rain events. The optical properties of DOM were more dependent on the BC types with different origins (sludge, corn, and rice) rather than on the extraction time. A large amount of DOM was released during the initial period of the extraction (1 day), which was equivalent to 52–60% of the total cumulative organic carbon during 17 days of extraction. The relative contribution of the initial extraction to the total cumulative amounts was greater for the formation potential of trihalomethanes (THMs) per BC (71–82%) compared to those of haloacetic acids (HAAs) or dissolved organic carbon (DOC), suggesting that the leaching behaviors of disinfection byproducts (DBP) precursors from BCs may be different from those of DOC (i.e., bulk DOM). Among the three BCs, corn BC-derived DOM exhibited the highest formation potentials of THMs and HAAs per BC for both the initial and the total cumulative extraction. The specific (or DOC-normalized) THMs formation potential was positively correlated with the ratios of terrestrial humic-like to fulvic-like components, implying condensed aromatic structures could operate as a surrogate for THMs formation of BC-derived DOM. This study provided insight into dynamic leaching behaviors of DOM from BCs and the formation potentials for THMs and HAAs in BC-amended fields under intermittent rainfall.
اظهر المزيد [+] اقل [-]Characteristics and source apportionment of PM2.5 during persistent extreme haze events in Chengdu, southwest China النص الكامل
2017
Li, Lulu | Tan, Qinwen | Zhang, Yuanhang | Feng, Miao | Qu, Yu | An, Junling | Liu, Xingang
Based on detailed data from Chengdu Plain (CP) from 6 January to 16 January, two typical haze episodes were analyzed to clarify the haze formation mechanism in winter. Weather conditions, chemical compositions, secondary pollutant transformation, optical properties of aerosols, the potential source contribution function (PSCF) and source apportionment were studied. The planetary boundary layer (PBL) height decreased distinctly during the haze episodes and restrained air pollutant vertical dispersion. As the haze worsened, the value of PBL × PM2.5 increased notably. The [NO3−]/[SO42−] ratio was 0.61, 0.76 and 0.88 during a non-haze period, episode 1 and episode 2, respectively, indicating that the mobile source of the air pollution is increasingly predominant in Chengdu. Water vapor also played a vital role in the formation of haze by accelerating the chemical transformation of secondary pollutants, leading to the hygroscopic growth of aerosols. The PSCF and backward trajectories of the air masses indicated that the pollution mainly came from the south. The secondary inorganic aerosols, vehicle emissions, coal combustion, biomass burning, industry, and dust contributed 34.1%, 24.1%, 12.7%, 12.3%, 7.6%, and 7.2% to PM2.5 masses in episode 1 and 28.9%, 23.1%, 9.4%, 9.5%, 20.3% and 7.5% in episode 2.
اظهر المزيد [+] اقل [-]Traceability of fluorescent engineered nanomaterials and their fate in complex liquid waste matrices النص الكامل
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.
اظهر المزيد [+] اقل [-]Source profiles of molecular structure and light absorption of PM2.5 brown carbon from residential coal combustion emission in Northwestern China النص الكامل
2022
Zhang, Qian | Li, Ziyi | Shen, Zhenxing | Zhang, Tian | Zhang, Yujie | Sun, Jian | Zeng, Yaling | Xu, Hongmei | Wang, Qiyuan | Hang Ho, Steven Sai | Cao, Junji
Residential coal combustion is a prominent source of brown carbon (BrC) aerosols, but knowledge of their molecular structures and optical absorption were limited, which have notable used in ambient BrC source identification and radiative forcing calculation. In this study, the Fourier transform–ion cyclotron resonance mass spectrometry combined with partial least squares regression analysis as well as Fourier transform infrared spectroscopy analysis were used to insight the molecular compounds and structures of BrC from anthracite and bituminous coal combustions between traditional and improved stoves. The absorption Ångström exponents (AAE) and mass absorption efficiency (MAE) values for the BrC emitted from the combinations of bituminous were both 1.2–2.5 times lower than those of anthracite, interpreting that the BrC from the anthracite emissions had greater light-absorbing capacity. In contrast, the emission factor of light absorption (EFAbₛ) at 365 nm for the bituminous coal combusted in the traditional stove was the highest among all the tested scenarios, which revealed that the incomplete combustion of bituminous coal could emit more BrC. It was noted that primary BrC emitted from the coal combustion with traditional stoves contains higher aromaticity groups of C–C and C=O and higher S containing organics, whereas more aliphatic groups were found in BrC using the improved stoves. N-containing (CHON and CHONS) compounds were dominated in the total molecular formula of BrC, whereas the sum of CHON and CHO groups had high double-bond equivalent (DBE) values contributed 53.5%–87.1% to the total BrC absorption. Moreover, for CHOS, the lowest of estimated molecular absorption, DBE, and DBE/C should attribute to the non-chromophoric or weak absorptive S-containing compounds. This study supplied an effective evaluation method to compare BrC emissions and their absorption for coal combustion on regional scale.
اظهر المزيد [+] اقل [-]Synthesis and photocatalytic degradation activities of phosphorus containing ZnO microparticles under visible light irradiation for water treatment applications النص الكامل
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.
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