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Cross-linked sulfydryl-functionalized graphene oxide as ultra-high capacity adsorbent for high selectivity and ppb level removal of mercury from water under wide pH range
2021
Bao, Shuangyou | Wang, Yingjun | Yu, Yongsheng | Yang, Weiwei | Sun, Yinyong
It is highly desirable but remains extremely challenging to develop a facile strategy to prepare adsorbent for dealing with heavy metal pollution in water. Here, we report a facile approach for preparing sulfydryl-functionalized graphene oxide (S-GO) by cross-linking method with an unprecedented adsorption capacity and ultrahigh selectivity for efficient Hg(II) removal. The adsorbents exhibit a prominent performance in capturing Hg(II) from wastewater with a record-high adsorption capacity of 3490 mg/g and rapid kinetics to reduce Hg(II) contaminants below the discharge standard of drinking water (2 ppb) within 60 min under a wide pH range even in the coexistent of other interfering metal ions. In addition, the adsorbents can be also easily recycled and reused multiple times with no apparent decline in removal efficiency. Considering the broad diversity, we developed also a magnetic Fe₃O₄/S-GO adsorbent by a simple chemical cross-linking reaction to achieve rapid separation of S-GO from their aqueous solution. In addition, the adsorbents were successfully applied in dealing with the practical industrial wastewater. The results indicate the potential of rationally designed sulfydryl-functionalized graphene oxide for high performance Hg(II) removal.
Show more [+] Less [-]Ammonium removal and recovery from sewage water using column-system packed highly selective ammonium adsorbent
2021
Tanaka, Hisashi | Fujimoto, Masayuki | Minami, Kimitaka | Takahashi, Akira | Parajuli, Durga | Hiwatari, Takehiko | Kawakami, Masami | Kawamoto, Tohru
One of the strategies to realize a nitrogen cycle society, we attempted to recover ammonium ions from industrial wastewater, especially sewage water with adsorbent materials. We have developed an adsorbent with high ammonium selectivity based on copper hexacyanoferrate and granulated it as pellets. Using a compact column system filled with this granule adsorbent, ammonium ions were recovered from sewage containing 1000–1500 mg-NH₄⁺/L ammonium ions. Despite the coexistence of many metal ions, the adsorbent selectively and stably adsorbed ammonium ions. Furthermore, it was shown that the saturated adsorbent can be regenerated by flowing a potassium ion solution through a column adsorbent to desorb ammonium ions. In other words, the column can be used repeatedly, and there was almost little deterioration in adsorption even after 250 cycles. In addition, it was shown that by increasing the number of stages of this column, it is possible to sufficiently reduce the ammonium in the adsorbent solution and recover the concentrated ammonium solution.
Show more [+] Less [-]Tracing riverine sulfate source in an agricultural watershed: Constraints from stable isotopes
2021
Liu, Jinke | Han, Guilin
The sulfate pollution in water environment gains more and more concerns in recent years. The discharge of domestic, municipal, and industrial wastewaters increases the riverine sulfate concentrations, which may cause local health and ecological problems. To better understand the sources of sulfate, this study collected water samples in a typical agricultural watershed in East Thailand. The source apportionment of sulfide was conducted by using stable isotopes and receptor models. The δ³⁴SSO₄ value of river water varied from 1.2‰ to 16.4‰, with a median value of 8.9‰. The hydrochemical data indicated that the chemical compositions of Mun river water were affected by the anthropogenic inputs and natural processes such as halite dissolution, carbonate, and silicate weathering. The positive matrix factorization (PMF) model was not suitable to trace source of riverine sulfate, because the meaning of the extracted factors seems to be vague. Based on the elemental ratio and isotopic composition, the inverse model yielded the relative contribution of sulfide oxidation (approximately 46.5%), anthropogenic input (approximately 41.5%), and gypsum dissolution (approximately 12%) to sulfate in Mun river water. This study indicates that the selection of models for source apportionment should be careful. The large contribution of anthropogenic inputs calls an urgent concern of the Thai government to establish effective management strategies in the Mun River basin.
Show more [+] Less [-]Structural control of the non-ionic surfactant alcohol ethoxylates (AEOs) on transport in natural soils
2021
Espeso, M Botella | Corada-Fernández, C. | García-Delgado, M. | Candela, L. | González-Mazo, E. | Lara-Martín, P.A. | Jiménez-Martínez, J.
Surfactants, after use, enter the environment through diffuse and point sources such as irrigation with treated and non-treated waste water and urban and industrial wastewater discharges. For the group of non-ionic synthetic surfactant alcohol ethoxylates (AEOs), most of the available information is restricted to the levels and fate in aquatic systems, whereas current knowledge of their behavior in soils is very limited. Here we characterize the behavior of different homologs (C12–C18) and ethoxymers (EO3, EO6, and EO8) of the AEOs through batch experiments and under unsaturated flow conditions during infiltration experiments. Experiments used two different agricultural soils from a region irrigated with reclaimed water (Guadalete River basin, SW Spain). In parallel, water flow and chemical transport were modelled using the HYDRUS-1D software package, calibrated using the infiltration experimental data. Estimates of water flow and reactive transport of all surfactants were in good agreement between infiltration experiments and simulations. The sorption process followed a Freundlich isotherm for most of the target compounds. A systematic comparison between sorption data obtained from batch and infiltration experiments revealed that the sorption coefficient (Kd) was generally lower in infiltration experiments, performed under environmental flow conditions, than in batch experiments in the absence of flow, whereas the exponent (β) did not show significant differences. For the low clay and organic carbon content of the soils used, no clear dependence of Kd on them was observed. Our work thus highlights the need to use reactive transport parameterization inferred under realistic conditions to assess the risk associated with alcohol ethoxylates in subsurface environments.
Show more [+] Less [-]Co-oxidative removal of arsenite and tetracycline based on a heterogeneous Fenton-like reaction using iron nanoparticles-impregnated biochar
2021
Fu, Dun | Kurniawan, Tonni Agustiono | Li, Heng | Wang, Haitao | Wang, Yuanpeng | Li, Qingbiao
A highly efficient, eco-friendly and relatively low-cost catalyst is necessary to tackle bottlenecks in the treatment of industrial wastewater laden with heavy metals and antibiotic such as livestock farm and biogas liquids. This study investigated co-oxidative removal of arsenite (As(III)) and tetracycline (TC) by iron nanoparticles (Fe NP)-impregnated carbons based on heterogeneous Fenton-like reactions. The composites included Fe NP@biochar (BC), Fe NP@hydrochar (HC), and Fe NP@HC-derived pyrolysis char (HDPC). The functions of N and S atoms and the loading mass of the Fe NP in the Fe NP@BC in heterogeneous Fenton-like reactions were studied. To sustain its cost-effectiveness, the spent Fe NP@BC was regenerated using NaOH. Among the composites, the Fe NP@BC achieved an almost complete removal of As(III) and TC under optimized conditions (1.0 g/L of dose; 10 mM H₂O₂; pH 6; 4 h of reaction; As(III): 50 μM; TC: 50 μM). The co-oxidative removal of As(III) and TC by the Fe NP@ BC was controlled by the synergistic interactions between the Fe NPs and the active N and S sites of the BC for generating reactive oxygen species (ROS). After four consecutive regeneration cycles, about 61 and 95% of As(III) and TC removal were attained. This implies that the spent carbocatalyst still has reasonable catalytic activities for reuse. Overall, this suggests that adding technological values to unused biochar as a carbocatalyst like Fe NP@BC was promising for co-oxidative removal of As(III) and TC from contaminated water.
Show more [+] Less [-]Combining metal and stable isotope analyses to disentangle contaminant transfer in a freshwater community dominated by alien species
2021
Balzani, Paride | Haubrock, Phillip J. | Russo, Francesco | Kouba, Antonín | Haase, Peter | Veselý, Lukáš | Masoni, Alberto | Tricarico, Elena
Freshwater ecosystems are negatively impacted by various pollutants, from agricultural, urban and industrial wastewater, with metals being one of the largest concerns. Moreover, freshwater ecosystems are often affected by alien species introductions that can modify habitats and trophic relationships. Accordingly, the threat posed by metals interacts with those by alien species, since the latter can accumulate and transfer these substances across the food web to higher trophic levels. How metals transfer within such communities is little studied. We analysed the concentration of 14 metals/metalloids (Al, As, Cd, Co, Cr, Cu, Fe, Hg, Mg, Mn, Ni, Pb, Se, Zn, hereafter ‘metal(s)’) of eight fish and three crustacean species co-existing in the Arno River (Central Italy), most of which were alien. To assess the pathway of contaminants within the community, we coupled metal analysis with carbon and nitrogen stable isotope analysis derived from the same specimens. Crustaceans showed higher metal concentration than fish, except for Cd, Hg and Se that were higher in fish. We found evidence of trophic transfer for six metals (Cd, Cr, Hg, Mg, Se, Zn). Additionally, ontogenetic differences and differences among various fish tissues (muscle, liver, and gills) were found in metals concentration. Considerable biomagnification along the trophic chain was found for Hg, while other metals were found to biodilute. Using stable isotopes and Hg as a third diet tracer, we refined the estimations of consumed preys in the diet previously reconstructed with stable isotope mixing models. Alien species reach high biomass and can both survive to and accumulate high pollutants concentrations, potentially posing a risk for their predators and humans. A combined effect of environmental filtering and increased competition may potentially contribute to the disappearance of native species with lower tolerances.
Show more [+] Less [-]A bibliometric analysis of industrial wastewater treatments from 1998 to 2019
2021
Mao, Guozhu | Hu, Haoqiong | Liu, Xi | Crittenden, John | Huang, Ning
For the foreseeable future, industrial water demand will grow much faster than agriculture. The demand together with the urgency of wastewater treatment, will pose big challenges for most developing countries. We applied the bibliometric analysis combined with social network analysis and S-curve technique to quantitatively analyze 9413 publications related to industrial wastewater treatment in the Scientific Citation Index (SCI) and Social Sciences Citation Index (SSCI) databases from 1998 to 2019. The results showed that: (1) Publications on industrial wastewater treatment have increased from 120 in 1998 to 895 in 2019 with a steady annual increment rate, and researchers have focused more on the application and optimization of existing technologies. (2) China had the highest number of publications (n = 1651, 19.66% of global output) and was a core country in the international cooperation network, whereas the United States and European countries produced higher quality papers. (3) By analyzing the co-occurrence and clusters of keywords and comparing three wastewater treatment categories (physical, chemical, biological), adsorption (n = 1277), oxidation (n = 1085) and activated sludge process (n = 1288) were the top three techniques. Researchers have shifted their focus to treatment technologies for specific wastewater type, such as textile wastewater, pulp and paper wastewater, and pharmaceutical wastewater. The S-curve from articles indicates that physical and chemical treatment technologies are attached with great potential in the near future, especially adsorption and advanced oxidation, while the biological treatment technologies are approaching to the saturation stage. Different pattern is observed for the S-curve derived from patents, which stressed the limited achievement until now and further exploration in the field application for the three treatment categories. Our analysis provides information of technology development landscape and future opportunities, which is useful for decision makers and researchers who are interested in this area.
Show more [+] Less [-]Occurrence and seasonal distribution of five selected endocrine-disrupting compounds in wastewater treatment plants of the Metropolitan Area of Monterrey, Mexico: The role of water quality parameters
2021
López-Velázquez, Khirbet | Guzmán-Mar, Jorge L. | Saldarriaga-Noreña, Hugo A. | Murillo-Tovar, Mario A. | Hinojosa-Reyes, Laura | Villanueva-Rodríguez, Minerva
Five endocrine-disrupting compounds (EDCs) were determined in four urban wastewater treatment plants (WWTPs) of the Metropolitan Area of Monterrey (MAM) in two seasonal periods (winter and summer). The MAM, one of the most urbanized areas in Mexico, is characterized by high industrial activity and population density, leading to extensive use of several EDCs. In the MAM, ∼90% of urban and industrial wastewater is treated in WWTPs, where EDCs can be partially eliminated. In this work, dissolved levels of 17β-estradiol (E2), 17α-ethinyl estradiol (EE2), bisphenol A (BPA), 4-nonylphenol (4NP), and 4-tert-octylphenol (4TOP) in wastewater were determined. The EDCs’ determination was carried out through solid-phase extraction (SPE) and gas chromatography coupled to mass spectrometry (GC-MS). High EDCs levels (0.4–450 ng/L) were found in the influents of WWTPs, while concentrations in the effluents ranged from 0.2 to 26.8 ng/L, with E2, EE2, and 4TOP being the most persistent. The Spearman correlation analysis revealed the association between E2 and EE2 (r = 0.4835, p < 0.05), and between BPA and 4NP (r = 0.5180, p < 0.05), suggesting that these EDCs have similar sources. Also, E2, BPA, and 4TOP were positively correlated with the chemical oxygen demand (COD), biochemical oxygen demand (BOD), and total suspended solids (TSS) (r = 0.4080–0.5694, p < 0.05), indicating the association of the EDCs with the organic matter in the wastewater. The factor analysis confirmed the significant correlation of COD, BOD, TSS, temperature, and pH with the high occurrence of 4TOP during the summer. It was also confirmed that summer warmer temperatures favored the removal of BPA and 4NP in the studied WWTPs. Finally, the studied sites were classified by cluster analysis in three groups, revealing the impact that seasonality has on the behavior of the selected EDCs.
Show more [+] Less [-]Multi-regional industrial wastewater metabolism analysis for the Yangtze River Economic Belt, China
2021
Han, Dengcheng | Huang, Gordon | Liu, Lirong | Zhai, Mengyu | Gao, Sichen
Enormous wastewater discharges have significantly impeded the sustainable development. As several economic belt has been formed in China, systematic analysis of multi-regional wastewater metabolic system is required for advancing wastewater mitigation effectively and efficiently. In this study, a distributive environmental input-output model (DEIO) is developed for the Yangtze River Economic Belt (YREB) to provide bases for supporting sustainable development from inter-regional and inter-sectoral perspectives. The discharges and flows of wastewater and related pollutants (i.e., chemical oxygen demand (COD) and ammonia nitrogen (AN)) among sectors and regions are analyzed to providing solid bases for wastewater management within the YREB. The results show that the industrial wastewater mitigation in YREB is desired urgently. The industrial wastewater discharges in Jiangsu and Zhejiang provinces are numerous, while Hunan and Yunnan provinces are more inclined to suffer from serious COD and AN pollution. In addition, the manufacture of food, tobacco, chemical materials, and pharmaceutical are the typical sectors with a large amount of direct wastewater discharge, and the tertiary industry is ranked at the first in indirect wastewater discharge. According to the analysis, the implementation of the “Supply-side Structure Reform” and the “Replace Subsidies with Rewards” policy can benefit the wastewater mitigation in the YREB.
Show more [+] Less [-]Endocrine-disrupting chemicals in a typical urbanized bay of Yellow Sea, China: Distribution, risk assessment, and identification of priority pollutants
2021
Lü Shuang, | Lin, Chunye | Lei, Kai | Xin, Ming | Wang, Baodong | Ouyang, Wei | Liu, Xitao | He, Mengchang
Endocrine-disrupting chemicals (EDCs) in water are receiving particular attention as they pose adverse effects on aquatic systems, even at trace concentrations. A comprehensive study was conducted on 14 EDCs (five estrogens and nine household and personal care products (HPCPs)) in the water of the urbanized Jiaozhou Bay in the Yellow Sea during summer and winter. Results showed that the total concentration of 14 EDCs ranged from 100 to 658 ng L⁻¹ and 56.7–212 ng L⁻¹ in the estuarine and bay water, respectively. The average total concentration of five estrogens in summer was significantly (p < 0.05) lower than that in winter due to the higher precipitation dilution and degradations during summer, whereas the average total concentration of nine HPCPs was significantly (p < 0.05) higher during the summer than that during the winter because of the higher usage and emissions during the summer. Estrogens and HPCPs were dominated by 17α-ethinylestradiol and p-hydroxybenzoic acid (PHBA), respectively. High PHBA concentrations may be related to the hydrolysis of parabens. The total concentrations of EDCs were higher in the eastern coastal seawater of the bay due to the strong influence of domestic and industrial wastewater discharge. Estrogens may interfere with the endocrine system of aquatic organisms in the bay because the total estradiol equivalent concentration exceeded 1 ng L⁻¹. 17α-ethinylestradiol was the main contributor to the estrogenic activity. The EDC mixtures posed high risks (RQ > 1) to mollusks, crustaceans, and fish, and low to moderate risks (RQ < 1) to algae. Fish was the most sensitive aquatic taxon to the EDC mixtures. Given the concentration and frequency of EDCs, the optimized risk quotient method revealed that 17α-ethinylestradiol, estrone, triclocarban, triclosan, and 17β-estradiol should be prioritized in ecological management because of their high risks (prioritization index of >1).
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