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Activation of peroxydisulfate by ball-milled α-FeOOH/biochar composite for phenol removal: Component contribution and internal mechanisms 全文
2022
Zhao, Ling | Zhang, Hui | Zhao, Beibei | Lyu, Honghong
Persulfate-based advanced oxidation process is considered as a promising technology for the degradation of phenol, where efficient, cost effective, and green methods with high peroxydisulfate (PS) activation capacity is of increasing demand. In this work, an in-situ liquid phase precipitation combined with ball milling method was applied for the synthesized of α-FeOOH/biochar, as be the PS activator for phenol degradation. Results showed that the ball-milled α-FeOOH and red pine wood biochar prepared at 700 °C (BM-α-FeOOH/PBC700) exhibited the highest catalytic property with PS for phenol oxidation (a phenol removal rate of 100%), compared with the BM-α-FeOOH (16.0%) and BMPBC700 (66.3%). The presence of intermediate products such as hydroquinone and catechol, and total organic carbon (TOC) removal rate (88.9%) proved the oxidation of phenol in the BM-α-FeOOH/PBC700+PS system. The characterization results showed that the functional groups (e.g., CO, C–O, Fe–O, and Si–O), the dissolved organic matter (DOM) in biochar, the loading of Fe element, and higher degree of graphitization and defect structures, contributed to the activation of PS to form free radicals (i.e., SO₄·⁻, ·OH, ·O₂⁻, and hVB⁺) for phenol oxidation, of which, SO₄·⁻ and ·OH account for 72.1% of the phenol removal rate. The specific contribution to the PS activation for phenol oxidation by each part of the materials was calculated based on the “whole to part” experiment. The contribution of DOM, acid-soluble substance, and carbon matrix and basal part in BM-α-FeOOH/PBC700 were 6.0%, 40.9%, and 53.1%, respectively. The reusability experiments of BM-α-FeOOH/PBC700 demonstrated that the composite was relatively stable after four cycles of reuse. Among three co-existing anions (NO₃⁻, Cl⁻, and HCO₃⁻), HCO₃⁻ played the most significant inhibition effects on phenol removal through reducing the phenol removal rate from 89.6% to 77.9%. This work provides guidance for the design of high active and stable carbon materials that activate PS to remove phenol.
显示更多 [+] 显示较少 [-]Spatial distribution, homologue patterns and ecological risks of chlorinated paraffins in mangrove sediments along the South China Coast 全文
2022
Chen, Hui | Han, Xu | Liang, Bowen | Deng, Man | Du, Bibai | Zeng, Lixi
The spatial distribution, homologue patterns, and ecological risks of chlorinated paraffins (CPs) were investigated in sediments from sixteen mangrove wetlands along the South China Coast (SCS). The total concentrations of CPs in mangrove sediments from Guangdong, Fujian, Guangxi, and Hainan were in the range of 933–4760, 619–2300, 375–1550, and 271–658 ng/g dry weight, respectively. The contamination levels and spatial distribution of short-chain and medium-chain CPs (SCCPs and MCCPs, respectively) in mangrove sediments were mainly affected by local population scale and CP industries. The dominant CP patterns in sediments were C₁₀–₁₁Cl₆₋₈ and C₁₄Cl₇₋₉ for SCCPs and MCCPs, respectively. Redundancy analysis, based on CP levels and several potential influencing factors showed that MCCPs/SCCPs ratio was the main factor affecting the accumulation of CPs in mangrove sediments. Additionally, MCCP concentrations were significantly correlated with total organic carbon (TOC), indicating that TOC might affect MCCP accumulation in mangrove sediments. Risk assessments indicated that CPs would pose medium ecological risks to sediment dwelling organisms in nearly one-third of the sampling sites. This is the first comprehensive report of the sedimentary SCCPs and MCCPs in mangrove wetlands along the SCS and highlights the need for more sediment toxicity data for CPs.
显示更多 [+] 显示较少 [-]Light absorption potential of water-soluble organic aerosols in the two polluted urban locations in the central Indo-Gangetic Plain 全文
2022
Rajeev, Pradhi | Choudhary, Vikram | Chakraborty, Abhishek | Singh, Gyanesh Kumar | Gupta, Tarun
PM₂.₅ (particulate matter having aerodynamic diameter ≤2.5 μm) samples were collected during wintertime from two polluted urban sites (Allahabad and Kanpur) in the central Indo-Gangetic Plain (IGP) to comprehend the sources and atmospheric transformations of light-absorbing water-soluble organic aerosol (WSOA). The aqueous extract of each filter was atomized and analyzed in a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Water-soluble organic carbon (WSOC) and WSOA concentrations at Kanpur were ∼1.2 and ∼1.5 times higher than that at Allahabad. The fractions of WSOC and secondary organic carbon (SOC) to total organic carbon (OC) were also significantly higher ∼53% and 38%, respectively at Kanpur compared to Allahabad. This indicates a higher abundance of oxidized WSOA at Kanpur. The absorption coefficient (bₐbₛ₋₃₆₅) of light-absorbing WSOA measured at 365 nm was 46.5 ± 15.5 Mm⁻¹ and 73.2 ± 21.6 Mm⁻¹ in Allahabad and Kanpur, respectively, indicating the dominance of more light-absorbing fractions in WSOC at Kanpur. The absorption properties such as mass absorption efficiency (MAE₃₆₅) and imaginary component of refractive index (kₐbₛ₋₃₆₅) at 365 nm at Kanpur were also comparatively higher than Allahabad. The absorption forcing efficiency (Abs SFE; indicates warming effect) of WSOA at Kanpur was ∼1.4 times higher than Allahabad. Enhancement in light absorption capacity was observed with the increase in f44/f43 (fraction of m/z 44 (f44) to 43 (f43) in organic mass spectra) and O/C (oxygen to carbon) ratio of WSOA at Kanpur while no such trend was observed for the Allahabad site. Moreover, the correlation between carbon fractions and light absorption properties suggested the influence of low-volatile organic compounds (OC3 + OC4 fraction obtained from thermal/optical carbon analyzer) in increasing the light absorption capacity of WSOA in Kanpur.
显示更多 [+] 显示较少 [-]Concentrations, homolog profiles, and risk assessment of short- and medium-chain chlorinated paraffins in soil around factories in a non-ferrous metal recycling park 全文
2022
Weng, Jiyuan | Zhang, Peixuan | Gao, Lirong | Zhu, Shuai | Liu, Yang | Qiao, Lin | Zhao, Bin | Liu, Yin | Xu, Ming | Zheng, Minghui
Chlorinated paraffins (CPs) are used as additives in metal processing in the metal smelting industry. Data on CPs in the environment near metal smelting plants are limited. The objectives of this study were to investigate the concentrations and congener profiles of CPs in soil around factories in a non-ferrous metal recycling park located in Hebei, China, and to investigate human exposure to CPs in the soil. The concentrations of short-chain CPs (SCCPs) and medium-chain CPs (MCCPs) were determined by two-dimensional gas chromatography with electron capture negative ionization mass spectrometry. The SCCP and MCCP concentrations in the soil samples were 121–5159 ng/g and 47–6079 ng/g, respectively. Generally, the CP concentrations in soils around the factories were relatively high compared with those near other contaminated sites and in rural and urban areas. There were significant correlations between the MCCP concentrations, some SCCP carbon homologs, and the total organic carbon content (p < 0.05). The major SCCP and MCCP congener groups were C₁₀Cl₆–₇ and C₁₅–₁₆Cl₅, respectively. Hierarchical cluster analysis and principal component analysis indicated that SCCPs and MCCPs in the soil might originate from extreme pressure additives containing CP-42 and CP-52 and CP-containing waste material from the factories. The concentrations in two samples collected near a metal recycling factory posed a moderate risk according to a risk assessment conducted using risk quotients. Further risk assessment showed that the CPs concentrations in soil did not pose significant health risks to either children or adults.
显示更多 [+] 显示较少 [-]Fate, source and mass budget of sedimentary microplastics in the Bohai Sea and the Yellow Sea 全文
2022
Zhang, Mingyu | Lin, Yan | Booth, Andy M. | Song, Xikun | Cui, Yaozong | Xia, Bin | Gu, Zhangjie | Li, Yifan | Liu, Fengjiao | Cai, Minggang
As reservoirs for pollutants transported via the Yangtze and Yellow Rivers, the Bohai Sea (BS) and Yellow Sea (YS) play an important role in transporting microplastics (MPs) to the Pacific Ocean. The fate, sources and mass budget of MPs in the BS and the YS were investigated by Pearson correlation, principal component analysis-multilinear regression analysis (PCA-MRLA) and a mass balance model to sedimentary MPs data. Average MP abundances were 137 and 119 items kg⁻¹ in the Bohai and Yellow Seas, respectively. MPs <1000 μm exhibited similar distribution patterns to total organic carbon and fine-grained sediments, while MPs >1000 μm were confined in the BS and exhibited a strong positive correlation with chlorophyll-a and polyethylene terephthalate, suggesting that larger MPs might deposit faster due to biofouling or when comprised of high density polymers. PCA-MLRA analysis indicated land-based inputs (packing materials, textile material and daily commodities) were dominant in the BS, while maritime activities (fishing and mariculture) were the main source of MPs in the YS. The mass balance model revealed that the total MP input and output to the BS and the YS was 3396.92 t yr⁻¹ and 3814.81 t yr⁻¹, respectively. The major input pathway of MPs to the BS and the YS were river discharge and air deposition, respectively. Notably, 94% of MPs in the BS and the YS were deposited to sediments. This study revealed that BS and YS sediments play an important role in preventing MPs from being further transported to the Pacific Ocean, thus more attention should be paid to local ecological risk assessment.
显示更多 [+] 显示较少 [-]Modern lake sedimentary record of PAHs and OCPs in a typical karst wetland, south China: Response to human activities and environmental changes 全文
2021
Cheng, Cheng | Hu, Tianpeng | Liu, Weijie | Mao, Yao | Shi, Mingming | Xu, An | Su, Yewang | Li, Xingyu | Xing, Xinli | Qi, Shihua
The sedimentary history of polycyclic aromatic hydrocarbons (PAHs) and organochlorine pesticides (OCPs) over the past 140 years in a lake sediment core from Huixian karst wetland was reconstructed. The total PAHs and OCPs concentrations ranged from 40.0 to 210 ng g⁻¹ and 0.98 to 31.4 ng g⁻¹, respectively. The vertical distribution of PAHs and OCPs in different stages was great consistent with the history of regional socio-economic development and the usage of OCPs. As the indicators of socio-economic development, gross domestic product (GDP), population, energy consumption, highway mileage, and private vehicles correlated with the PAHs concentrations, indicating the impact of human activities on PAHs levels. The PAHs and OCPs concentrations were also affected by environmental changes in the wetland, as reconstructed by total organic carbon (TOC), sand, silt, clay, quartz, and calcite in sediments. Redundancy analysis (RDA) results showed TOC was the dominant factor to explain the concentrations of PAHs and OCPs with the explanation of 86.7% and 43.5%, respectively. In addition, TOC content had significantly positive correlation with PAHs (0.96, p < 0.01) and OCPs (0.78, p < 0.01). In particular, the significantly positive correlation (p < 0.05) between calcite and PAHs and OCPs inferred that karstification might play an important role in the migration of PAHs and OCPs in the karst area. Therefore, the lake in Huixian wetland tended to be a sink more than a source of PAHs and OCPs influenced by the increasing TOC content and karstification under climate warming.
显示更多 [+] 显示较少 [-]Ag NPs decorated C–TiO2/Cd0.5Zn0.5S Z-scheme heterojunction for simultaneous RhB degradation and Cr(VI) reduction 全文
2021
Wang, Yuhan | Kang, Chunli | Li, Xinyang | Hu, Qing | Wang, Chao
In this study, heterojunction photocatalysts, XAg@C-TCZ, based on MOF-derived C–TiO₂ and Cd₀.₅Zn₀.₅S decorated with Ag nanoparticles (Ag NPs) were successfully synthesized through hydrothermal and calcination methods. The catalytic effectiveness of XAg@C-TCZ was evaluated by simultaneous photocatalytic degradation of rhodamine B (RhB) and reduction of Cr(VI) under simulated sunlight irradiation. The presence of the Z-scheme heterojunction was demonstrated through trapping experiments, X-ray photoelectron spectroscopy (XPS), time-resolved photoluminescence (PL) investigations, and electron spin resonance (ESR) spectroscopy. With an initial RhB and Cr(VI) concentration of 7 mg L⁻¹ and 5 mg L⁻¹, the catalyst 10Ag@C-TCZ achieved a simultaneous removal of 95.2% and 95.5% within 120 min, respectively. With the same catalyst, the degradation rate of RhB was 2.75 times higher and the reduction rate of Cr(VI) was 9.3 times higher compared to pure Cd₀.₅Zn₀.₅S. Total organic carbon (TOC) analysis confirmed the extent of mineralization of RhB, while the reduction of Cr(VI) was corroborated by XPS. Compared to pure RhB and Cr(VI) solutions, the reaction rates are smaller in the solution containing both contaminants, which is attributed to the competition for ·O₂⁻. 10Ag@C-TCZ also exhibited a stable catalytic performance in tap water and lake water. This work provides a new perspective on the construction of heterojunctions with doped MOF derivatives for the purification of complex pollutant systems.
显示更多 [+] 显示较少 [-]Occurrence and spatial distribution of legacy and novel brominated flame retardants in seawater and sediment of the South China sea 全文
2021
Feng, Hongru | Cheng, Yixue | Ruan, Yuefei | Tsui, Mirabelle M.P. | Wang, Qi | Jin, Jing | Wu, Rongben | Zhang, Haiyan | Lam, Paul K.S.
The occurrence and spatial distribution of polybrominated diphenyl ethers (PBDEs) and novel brominated flame retardants (NBFRs) in seawater and surficial sediment samples (N = 19 and 45, respectively) from the South China Sea (SCS) in 2018 were investigated, and the correlation between BFRs and site parameters (total organic carbon, depth, etc.) were assessed by principal component analysis. The concentration ranges of ΣPBDEs in seawater and sediments were 0.90–4.40 ng/L and 0.52–22.67 ng/g dry weight (dw), respectively, while those of ΣNBFRs were 0.49–37.42 ng/L and 0.78–82.29 ng/g dw, respectively. BDE-209 and decabromodiphenyl ethane were the predominant BFRs, accounting for 38.65% and 36.94% in seawater and 26.71% and 68.42% in sediments, respectively. Notably, tris(2,3-dibromopropyl)isocyanurate and 2,4,6-tris(2,4,6-tribromophenoxy)-1,3,5-triazine, seldomly detected in aquatic matrices worldwide, were detected for the first time in the study area, and their relatively high levels and detection frequencies indicate the ubiquitous application of these NBFRs in the Pearl River Delta. Zhuhai and Jiangmen are the main sources of NBFRs in the SCS. Preliminary risk assessment on NBFRs using hazard quotient indicates low to medium risks to marine organisms at some sites. The occurrence of NBFRs in the SCS highlights the prioritization of more toxicological information on these compounds.
显示更多 [+] 显示较少 [-]In-depth investigation of Sodium percarbonate as oxidant of PAHs from soil contaminated with diesel oil 全文
2021
Cavalcanti, Jorge Vinicius Fernandes Lima | Fraga, Tiago José Marques | Loureiro Leite, Mirella de Andrade | dos Santos e Silva, Daniella Fartes | de Lima, Valmir Félix | Schuler, Alexandre Ricardo Pereira | do Nascimento, Clístenes Williams Araújo | da Motta Sobrinho, Maurício Alves
Sodium percarbonate (SPC, 2Na₂CO₃∙3H₂O₂), is a compound that can be used under multiple environmental applications. In this work, SPC was employed as oxidant in the treatment of soil contaminated with diesel oil. The soil samples were collected during the earthmoving stage of RNEST Oil Refinery (Petrobras), Brazil. Then, the samples were air-dried, mixed and characterized. Subsequently, raw soil was contaminated with diesel and treated by photo-Fenton reaction (H₂O₂/Fe²⁺/UV). SPC played a significant role in the generation of hydroxyl radicals under the catalytic effect of ferrous ions (Fe²⁺), hydrogen peroxide (H₂O₂) and radiation. These radicals provoked the photodegradation of polycyclic aromatic hydrocarbons (PAHs), in the soil remediation. A factorial design 3³ was carried out to assess the variables which most influenced the decrease in total organic carbon (TOC). The study was performed with the following variables: initial concentration of [H₂O₂] and [Fe²⁺], between 190.0 and 950.0 mmol L⁻¹ and 0.0–14.4 mmol L⁻¹, respectively. UV radiation was supplied from sunlight, blacklight lamps, and system without radiation. All experiments were performed with 5.0 g of contaminated soil in 50.0 mL of solution. The initial concentration of Fe²⁺ showed the statistically most significant effect. The oxidation efficiency evaluated in the best condition showed a decrease from 34,765 mg kg⁻¹ to 15,801 mg kg⁻¹ in TOC and from 85.750 mg kg⁻¹ to 20.770 mg kg⁻¹ in PAHs content. Moreover, the sums of low and high molecular weight polycyclic aromatic hydrocarbons (LMW-PAHs and HMW-PAHs) were 19.537 mg kg⁻¹ and 1.233 mg kg⁻¹, respectively. Both values are within the limits recommended by the United Sates Environmental Protection Agency (USEPA) and evidenced the satisfactory removal of PAHs from contaminated soil, being an alternative to classic oxidation protocols.
显示更多 [+] 显示较少 [-]Occurrence and distribution of PAHs and microbial communities in nearshore sediments of the Knysna Estuary, South Africa 全文
2021
Liu, Xinran | Liu, Min | Zhou, Limin | Hou, Lijun | Yang, Yi | Wu, Dianming | Meadows, Michael E. | Li, Zhanhai | Tong, Chunfu | Gu, Jinghua
This study investigated the polycyclic aromatic hydrocarbons (PAHs) occurrence, and their impact on the microbial community and PAH-degrading genera and genes in the Knysna Estuary of South Africa. The results reveal that the estuary exhibits low PAH levels (114.1–356.0 ng g⁻¹). Ignavibacteriae and Deferribacteres, as well as Proteobacteria and Bacteroidetes, are keystone phyla. Among measured environmental factors, total organic carbon (TOC), nutrients such as nitrite and nitrate, metals as Al, Cr, Cu, Ni, Pb and Zn, and environmental properties (pH and salinity) are primary contributors to structuring the bacterial community assemblage. The abundance of alpha subunit genes of the PAH-ring hydroxylating dioxygenases (PAH-RHDα) of Gram-negative bacteria lies in the range of (2.0–4.2) × 10⁵ copies g⁻¹, while that of Gram-positive bacteria ranges from 3.0 × 10⁵ to 1.3 × 10⁷ copies g⁻¹. The PAH-degrading bacteria account for up to 0.1% of the bacterial community and respond mainly to nitrate, TOC and salinity, while PAHs at low concentration are not significant influencing factors. PAH degraders such as Xanthomonadales, Pseudomonas, and Mycobacterium, which play a central role in PAH-metabolization coupled with other biogeochemical processes (e.g. iron cycling), may contribute to maintaining a healthy estuarine ecosystem. These results are important for developing appropriate utilization and protection strategies for pristine estuaries worldwide.
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