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Performance comparison of silicone and low-density polyethylene as passive samplers in a global monitoring network for aquatic organic contaminants
2022
Sobotka, Jaromír | Smedes, Foppe | Vrana, Branislav
Contamination with hydrophobic organic compounds (HOCs) such as persistent organic pollutants negatively affects global water quality. Accurate and globally comparable monitoring data are required to understand better the HOCs distribution and environmental fate. We present the first results of a proof-of-concept global monitoring campaign, the Aquatic Global Passive Sampling initiative (AQUA-GAPS), performed between 2016 and 2020, for assessing trends of freely dissolved HOC concentrations in global surface waters. One of the pilot campaign aims was to compare performance characteristics of silicone (SSP) and low-density polyethylene (PE) sheets co-deployed in parallel under identical conditions, i.e. at the same site, using the same deployment design, and for an equal period. Individual exposures lasted between 36 and 400 days, and samples were collected from 22 freshwater and 40 marine locations. The sampler inter-comparability is based on a rationale of common underlying principles, i.e. HOC diffusion through a water boundary layer (WBL) and absorption by the polymer. In the integrative uptake phase, equal surface-specific uptake in both samplers was observed for HOCs with a molecular volume less than 300 ų. For those HOCs, transport in the WBL controls the uptake as mass transfer in the polymer is over 20-times faster. In such a case, sampled HOC mass can be converted into aqueous concentrations using available models derived for WBL-controlled sampling using performance reference compounds. In contrast, for larger molecules, surface-specific uptake to PE was lower than to SSP. Diffusion in PE is slower than in SSP, and it is likely that for large molecules, diffusion in PE limits the transport from water to the sampler, complicating the interpretation. Although both samplers provided mostly well comparable results, we recommend, based on simpler practical handling, simpler data interpretation, and better availability of reliable polymer-water partition coefficients, silicone-based samplers for future operation in the worldwide monitoring programme.
Show more [+] Less [-]Adsorptive removal of propranolol under fixed-bed column using magnetic tyre char: Effects of wastewater effluent organic matter and ball milling
2022
Feizi, Farzaneh | Sarmah, Ajit K. | Rangsivek, Ropru | Gobindlal, Kapish
We investigated the competitive effects of different fractions of wastewater treatment plant effluent organic matter (EfOM) on adsorption of an organic micro pollutant (OMP), propranolol (PRO), in a fixed bed column packed with magnetic tyre char (MTC). The results showed that the presence of EfOM inhibited PRO adsorption in wastewater leading to decreased PRO adsorption capacity from 5.86 to 2.03 mg/g due to competitive effects and pore blockage by smaller EfOM fractions. Characterization of EfOM using size exclusion chromatography (LC-OCD) showed that the principal factor controlling EfOM adsorption was pore size distribution. Low molecular weight neutrals had the highest adsorption onto MTC while humic substances were the least interfering fraction. Effect of important parameters such as contact time, linear velocity and bed height/diameter ratio on MTC performance was studied in large-lab scale columns. Linear velocity and contact time were found to be effective in increasing adsorption capacity of PRO on MTC and delaying breakthrough time. Increase in linear velocity from 0.64 cm/min to 1.29 cm/min increased mass transfer and dispersion, resulting in considerable rise of adsorbed amount (5.86 mg/g to 22.58 mg/g) and increase in breakthrough time (15.8–62.7 h). Efficiency of non-equilibrium Hydrus model considering dispersion and mass transfer mechanism was demonstrated for real wastewater and scale up purposes. Ball milling for degradation of adsorbed PRO and regeneration of MTC resulted in 79% degradation of PRO was achieved after 5 h milling (550 rpm), while the addition of quartz sand increased the efficiency to 92%.
Show more [+] Less [-]Volatility of Springtime ambient organic aerosol derived with thermodenuder aerosol mass spectrometry in Seoul, Korea
2022
Kang, Hyun Gu | Kim, Youngjin | Collier, Sonya | Zhang, Qi | Kim, Hwajin
The volatilities of ambient organic aerosol (OA) components are important to forecasting OA formation with models. However, providing the OA volatility distribution inputs for models is challenging, and models often rely on measurements from chamber experiments. We measured the volatility of submicron ambient OA in Seoul during May/June of 2019 by connecting a thermodenuder to an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (AMS). We calculated a volatility basis set (VBS) of the organic aerosol with a thermodenuder mass transfer model and data from the thermodenuder set to various temperatures (30–200 °C). We found a large discrepancy between the measured ambient VBS and a reference VBS used in air quality models, with the ambient organics being less volatile. The results suggest that a modeling study that tries to account for this discrepancy may be needed to identify the impact it has on modeling outcomes. Chamber experiments aiming to determine VBSs for specific chemical systems should address limitations caused by wall losses and incomplete modeling parameters.
Show more [+] Less [-]Rapid narrowing of the urban–suburban gap in air pollutant concentrations in Beijing from 2014 to 2019
2022
Li, Xue | Zhang, Fang | Ren, Jingye | Han, Wenchao | Zheng, Bo | Liu, Jieyao | Chen, Lu | Jiang, Sihui
Understanding the spatial patterns of atmospheric pollutants in urban and suburban areas is important for evaluating their effects on regional air quality, climate, and human health. The analyses of pollutant monitoring data of the China National Environmental Monitoring Center revealed that the differences in the concentrations of ambient O₃, PM₂.₅, NO₂, SO₂, and CO between urban and suburban areas rapidly decreased from 2014 to 2019 in Beijing. Considering the negligible urbanization and interannual meteorological changes during the study period, the results reveal a quick response of the urban-to-suburban difference (ΔUᵣbₐₙ₋Sᵤbᵤᵣbₐₙ) in the ambient pollutants concentrations to emission reduction measures implemented in China in 2013. However, owing to the efficient O₃ formation in summer in urban areas in recent years, we observed a more rapid decrease in the ΔUᵣbₐₙ₋Sᵤbᵤᵣbₐₙ in O₃ concentration in summer (64.8%) than in winter (16.1%). In addition, the ΔUᵣbₐₙ₋Sᵤbᵤᵣbₐₙ in daytime summer O₃ changed from negative in 2014–2018 to positive in 2019, indicating that the daytime O₃ concentration in urban areas exceeded that in suburban areas. Furthermore, instantaneous changes in ΔUᵣbₐₙ₋Sᵤbᵤᵣbₐₙ in air pollutants were more sensitive to meteorological variations in 2014 than in 2019. The results indicate a less significant role of regional air mass transport in the spatial variability of pollutants under a future scenario of strong emission reduction in China.
Show more [+] Less [-]High time-resolved variations of proteins in PM2.5 during haze pollution periods in Xi'an, China
2022
Yanpeng, Li | Haoyue, Zhang | Aotang, Li | Jiali, Zhang | Shengli, Du
Proteinaceous matter is an important component of PM₂.₅, which can cause adverse health effects and also influence the air quality and climate change. However, there is little attention to high time-resolved variations and potential role of aerosol proteins during haze pollution periods. In this study, PM₂.₅ samples were first collected by a medium flow sampler in autumn and winter in Xi'an, China. Then three high time-resolved monitoring campaigns during haze pollution periods were conducted to determine the evolving characteristics of total protein concentration and explore the interactive relationship between protein and other chemical compositions. The results showed that the average protein concentration in PM₂.₅ in Xi'an (5.46 ± 3.32 μg m⁻³) was higher than those in most cities of China, and varied by seasons and air pollution conditions. In particular, the protein concentration in PM₂.₅ increased with the increase of air quality index (AQI). The continuous variations of aerosol proteins during the haze pollution periods further showed that PM₂.₅, atmospheric humidity and long-distance air mass transport exerted the significant impacts on the protein components in aerosols. Based on the present observation, it is suggested that aerosol proteins might affect the generation of secondary aerosols under haze weather conditions. The present results may provide a new possible insight into the variations and the role of aerosol proteinaceous matter during the formation and development of haze pollution.
Show more [+] Less [-]Mass and number concentration distribution of marine aerosol in the Western Pacific and the influence of continental transport
2022
Ma, Yining | Zhang, Xiangguang | Xin, Jinyuan | Zhang, Wenyu | Wang, Zifa | Liu, Quan | Wu, Fangkun | Wang, Lili | Lyu, Yilong | Wang, Qinglu | Ma, Yongjing
We quantify for the first time marine aerosol properties and their differences in the offshore and remote ocean in the mid-latitude South Asian waters, low-latitude South Asian waters, and equatorial waters of the Western Pacific Ocean, based on shipboard cruise observations conducted by the Western Pacific Ocean Scientific Observation Network in winter 2018, and further investigate the effects of long-range transport of continental aerosols on the marine environment. During the overall observation period, the average number concentration of particle matter which aerodynamic diameters<2.5 μm (PM₂.₅N) was 35.1 ± 87.4 cm⁻³ and the mass concentration (PM₂.₅M) was 12.3 ± 9.1 μg/m³. The PM₂.₅N and PM₂.₅M during the continental air mass transport period were 7.2 and 1.3 times higher than those during the non-transport period (109.2 ± 169.3 cm⁻³, 15.9 ± 14.9 μg/m³), respectively. Excluding transport period, the average PM₂.₅N and PM₂.₅M are reduced by 120% and 7%. Coarse mode particle number concentration (PM₂.₅–₁₀N) and mass concentration (PM₂.₅–₁₀M) are not significantly influenced by continental air masses (only a reduction of 7% and 2%). The variation of marine aerosol concentrations in different latitudes zones is greatly influenced by continental aerosol transport. The offshore PM₂.₅M/PM₁₀M was 30%, 21%, and 22% in the mid-latitude sea of South Asia, a low-latitude sea of South Asia, and the equatorial sea, respectively. In comparison, in the remote ocean, the distribution ratio of PM₂.₅M/PM₁₀M tended to be steady (22%–23%), and the background characteristics of marine aerosols were clearly represented. The aerosol concentration decreases with the increase of wind speed during the transport period, and the wind speed reflects the scavenging effect on aerosol. In the non-transport period, the wind speed at the sea surface promotes the generation of marine aerosols, and the impact in wind speed is strongest in the PM₂.₅–PM₅ particle size range.
Show more [+] Less [-]In-stream sorption of azithromycin and levofloxacin in a river receiving sewage treatment plant effluent
2022
Hanamoto, Seiya | Yamamoto-Ikemoto, Ryoko
Modelling natural attenuation is crucial to managing pharmaceuticals. However, little is known about the mechanism behind their in-stream sorption. To better understand the in-stream attenuation of the highly sorptive antibiotics azithromycin (AZM) and levofloxacin (LVF), we monitored them in a 2.1-km stretch of the Asano River under diverse flow conditions. This stretch receives effluent directly from a sewage treatment plant (STP), which was a dominant source of the pharmaceuticals. Average distribution coefficients between dissolved and particulate phases (Kd,SPM) in the outflow river water were 6.3×105 L/kg for AZM and 7.5×104 L/kg for LVF, while those in the STP effluent were 1–2 orders of magnitude lower. Mass balances in the river stretch calculated by considering only dissolved phase (MBw) and both dissolved and particulate phases (MBs) were 8%–52% and 58%–102%, respectively, for AZM, and 58%–71% and 60%–105% for LVF. MBw<MBs is attributed to an increase in suspended particulate matter (SPM)-mediated mass flows in the river stretch, i.e., in-stream sorption to SPM, which was caused mainly by their much higher river Kd,SPM values than those in the effluent. Their river Kd,SPM values increased on higher-flow days with decreasing effluent content in the river water, resulting in the increase of their in-stream SPM sorption. Their in-stream loss from the entire water column (i.e., 100−MBs), which was attributable to their mass transfer from the overlying water to sediment through sorption, was decreased on higher-flow days by hydrological factors. A key finding is that AZM and LVF mostly entered the river stretch in the dissolved phase of STP effluent, whereas they existed substantially in the particulate phase in the outflow river water, especially on high-flow days.
Show more [+] Less [-]Migration processes of radioactive cesium in the Fukushima nearshore area: Impacts of riverine input and resuspension
2022
Misonou, Toshiharu | Nakanishi, Takahiro | Tsuruta, Tadahiko | Shiribiki, Takehiko | Sanada, Yukihisa
It is essential to evaluate secondary migration caused by riverine input and resuspension from seabed sediments to estimate the future distribution of radioactive cesium (¹³⁷Cs) in the coastal area off Fukushima Prefecture. In particular, the inflow from rivers cannot be ignored because most of the ¹³⁷Cs inflow from rivers is deposited on the coast without elute into seawater. Two mooring systems were installed near the Ukedo River's mouth (Fukushima Prefecture) from February 2017 to February 2018. The first contained a sediment trap system, collecting sinking particles during the period. The second comprised a turbidity sensor and a current sensor. The contribution of resuspension and inflow from the river to the mass flux was quantitatively evaluated using multiple regression equations. The results showed that resuspension caused 79%–83% of secondary ¹³⁷Cs migration in nearshore areas, whereas the influence of riverine ¹³⁷Cs input on the sediment was only 7% per year.
Show more [+] Less [-]Investigation on a high gravity device for reduction of NOx emission from marine diesel engines
2022
Ni, Peiyong | Xu, Haiyan | Liu, Zhongfei | Zhang, Ziheng | Peng, Chaohua | Wang, Xiangli
High gravity technology, as a process intensification technology, has demonstrated the great advantages in the field of gas purification on account of its excellent mass transfer efficiency and energy-efficient, but it is rarely applied in the field of nitrogen oxides (NOx) purification of marine diesel engine exhaust. In this paper, a high-gravity bowl-shaped-disk rotating bed (HBRB) without catalytic was designed for diesel exhaust after-treatment. A diesel oxidation catalyst (DOC) was installed in the front of the HBRB to regenerate more nitrogen dioxide (NO₂) easily reduced by urea. A bench test of a 6-cylinder marine diesel engine with the HBRB was carried out. The effects of the HBRB speeds, urea concentrations, and engine operating conditions on NOx purification efficiency in engine exhaust were experimentally investigated. The experimental result indicates that the maximum NOx removal efficiency of the HBRB can reach 69.1%. The improvement of the NOx removal efficiency is not obvious at the HBRB speed of over 1500 r/min. The pre-oxidation degree of nitric oxide (NO) and urea concentration largely affect the NOx removal efficiency. The HBRB has great potential in marine diesel engine exhaust denitration.
Show more [+] Less [-]Study of the performance of a cylindrical flow-through electro-Fenton reactor using different arrangements of carbon felt electrodes: effect of key operating parameters
2022
García-Espinoza, Josué Daniel | Robles, Irma | Durán-Moreno, Alfonso | Godínez, Luis A.
In this work, a cylindrical flow-through electro-Fenton reactor containing graphite felt electrodes and an Fe(II) loaded resin was evaluated for the production of the Fenton reaction mixture and for the degradation of amoxicillin (AMX) and fecal coliforms containing aqueous solutions. First, the influence of several factors such as treatment time, current intensity, flow rate, and electrode position was investigated for the electrogeneration of H₂O₂ and the energetic consumption by means of a factorial design methodology using a 2⁴ factorial matrix. Electric current and treatment time were found to be the pivotal parameters influencing the H₂O₂ production with contributions of 40.2 and 26.9%, respectively. The flow rate had low influence on the responses; however, 500 mL min⁻¹ (with an average residence time of 1.09 min obtained in the residence time distribution analysis) allowed to obtain a better performance due to the high mass transport to and from the electrodes. As expected, polarization was also found to play an important role, since for the cathode-to-anode flow direction, lower H₂O₂ concentrations were observed when compared with the anode-to-cathode flow arrangement, indicating that part of the H₂O₂ produced in the cathode was destroyed at the anode. A fluorescence study of hydroxyl radical production, on the other hand, showed that higher yields were obtained using an anode-to-cathode flow direction (up to 3.88 µM), when compared with experiments carried out using a cathode-to-anode flow path (3.11 µM). The removal of a commercial formulation of the antibiotic AMX was evaluated in terms of total organic carbon, achieving up to 57.9% and 38.63% of pollutant mineralization using synthetic and real sanitary wastewater spiked, respectively. Finally, the efficiency of the process on the inactivation of fecal coliforms in sanitary wastewater samples was assessed, reducing 90% of the bacteria after 5 min of electrolysis.
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