Journal of Environmental Sciences
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2022
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IF 6.796
Hao-Jie Cui,Yaqi Ning,Cong Wu,Wei Peng,Dong Cheng,Lichu Yin,Weijun Zhou,Wenjuan Liao
It has been documented that organic contaminants can be degraded by hydroxyl radicals (•OH) produced by the activation of H 2 O 2 by Fe(II)-bearing clay. However, the interfacial electron transfer reactions between structural Fe(II) and H 2 O 2 for •OH generation and its effects on contaminant remediation are unclear. In this study, we first investigated the relation between •OH generation sites and sulfamethoxazole (SMX) degradation by activating H 2 O 2 using nontronite with different reduction extents. SMX (5.2–16.9 µmol/L) degradation first increased and then decreased with an increase in the reduction extent of nontronite from 22% to 62%, while the •OH production increased continually. Passivization treatment of edge sites and structural variation results revealed that interfacial electron transfer reactions between Fe(II) and H 2 O 2 occur at both the edge and basal plane. The enhancement on basal plane interfacial electron transfer reactions in a high reduction extent rNAu-2 leads to the enhancement on utilization efficiencies of structural Fe(II) and H 2 O 2 for •OH generation. However, the •OH produced at the basal planes is less efficient in oxidizing SMX than that of at edge sites. Oxidation of SMX could be sustainable in the H 2 O 2 /rNAu-2 system through chemically reduction. The results of this study show the importance role of •OH generation sites on antibiotic degradation and provide guidance and potential strategies for antibiotic degradation by Fe(II)-bearing clay minerals in H 2 O 2 -based treatments.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2026
·
IF 6.6
Zhicong Yan,Xiaocong Cao,Jia Tang,Kai Tang,Zhaoqun Liu,Zhi Zhou
SMX exposure activates immune and antioxidant responses in coral. • SMX exposure induces broad functional shifts in bacterial communities in coral. • Low-concentration SMX (0.1 µg L −1 ) exposure interrupts energy reservation and allocation in coral and their symbiotic Symbiodiniaceae. The overuse of antibiotics in aquaculture causes severe contamination in the coral reef environments, leading to the degradation of this vulnerable ecosystem. In the present study, 16S rRNA, transcriptomic and physiological approaches were employed to reveal the impacts of sulfamethoxazole (SMX), one of the common and widely distributed antibiotics in South China Sea, on the keystone sclerectinian coral Pocillopora damicornis holobiont. It was revealed that low-concentration SMX exposure (0.1 µg L −1 ) induced immune responses in coral hosts by activating the tumor necrosis factor (TNF) signaling pathway, and the synthesis of heat shock proteins. The symbiotic Symbiodiniaceae also enhanced their stress resistance by up-regulating oxygen metabolism and translation-related genes. Low-concentration SMX could also increase energy reserve and suppress energy allocation in the coral host. Moreover, results from 16S rRNA sequencing suggested that SMX exposure caused broad functional shifts in bacterial communities, including microbial infection, degradation of environmental pollutants, cyanoamino acid metabolism, carbon storage and glutathione metabolism. These findings illustrate that coral holobionts are highly sensitive to SMX exposure, which alters bacterial symbiont community to disturb energy metabolism, triggers immune responses, and ultimately affects corals’ survival.
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Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Yezi He,Jerosha Ifthikar,Lie Yang,Zhuqi Chen
A cross-linked chitosan-modified birch sawdust biochar (CS@BSBC) was prepared and applied for the simultaneous elimination of vanadium (Ⅴ) and sulfamethoxazole (SMX) from livestock wastewater. The adsorption capacity of V(V) reached 110 mg/g alone while this value was promoted to 150 mg/g for the simultaneous removal of SMX and V(V), and the adsorption effect is optimal at pH 3. The adsorption capacity of SMX reached about 30 mg/g alone, while the SMX’s adsorption capacity droped to 25 mg/g for the simultaneous removal of SMX and V(V). The mechanism studies disclosed that redox reactions occur on the surface of CS@BSBC. As revealed by the XPS spectra, 63 % of V(V) was reduced to V(IV) concurrently pyrolic nitrogen and C−O terminals were oxidized to nitrogen oxide and C O. The treatment mechanism of CS@BSBC described above can provide a reference for the subsequent treatment of livestock wastewater with complex composition and high vanadium content.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
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IF 9.028
Mengyuan Qi,Bin Liang,Long Zhang,Xiaodan Ma,Lei Yan,Wenchen Dong,Deyong Kong,Liying Zhang,Haizhen Zhu,Shu-Hong Gao,Jiandong Jiang,Shuang-Jiang Liu,Philippe F.-X. Corvini,Aijie Wang
Microbial communities are believed to outperform monocultures in the complete catabolism of organic pollutants via reduced metabolic burden and increased robustness to environmental challenges; however, the interaction mechanism in functional microbiomes remains poorly understood. Here, three functionally differentiated activated sludge microbiomes (S1: complete catabolism of sulfamethoxazole (SMX); S2: complete catabolism of the phenyl part of SMX ([phenyl]-SMX) with stable accumulation of its heterocyclic product 3-amino-5-methylisoxazole (3A5MI); A: complete catabolism of 3A5MI rather than [phenyl]-SMX) were enriched. Combining time-series cultivation-independent microbial community analysis, DNA-stable isotope probing, molecular ecological network analysis, and cultivation-dependent function verification, we identified key players involved in the SMX degradation process. Paenarthrobacter and Nocardioides were primary degraders for the initial cleavage of the sulfonamide functional group (−C–S–N– bond) and 3A5MI degradation, respectively. Complete catabolism of SMX was achieved by their cross-feeding. The co-culture of Nocardioides, Acidovorax, and Sphingobium demonstrated that the nondegraders Acidovorax and Sphingobium were involved in the enhancement of 3A5MI degradation. Moreover, we unraveled the internal labor division patterns and connections among the active members centered on the two primary degraders. Overall, the proposed methodology is promisingly applicable and would help generate mechanistic, predictive, and operational understanding of the collaborative biodegradation of various contaminants. This study provides useful information for synthetic activated sludge microbiomes with optimized environmental functions.
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ARCHIVES OF ENVIRONMENTAL CONTAMINATION AND TOXICOLOGY
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2021
·Vol. 81
·期 1
·155-165
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IF 2.804
Kong Fanxing,Xu Xia,Xue Yingang,Gao Yu,Zhang Ling,Wang Liping,Jiang Shanqing,Zhang Qiuya
In this study, three different types of microplastics were aged by the thermal activation K 2 S 2 O 8 method to investigate the adsorption behavior for sulfamethoxazole (SMX) in aqueous solution. The effects of pH, salinity and humic acid (HA) on adsorption behavior were also investigated. At the same time, the morphology and functional groups of microplastics before and after adsorption were characterized. As the aging time increased, the adsorption capacity of the microplastics also increased significantly. Whether it was pristine or aged, polylactic acid (PLA) had the highest adsorption capacity. The adsorption capacity of microplastics was the largest under acidic conditions, and its adsorption capacity decreased significantly in alkaline solutions. The presence of salinity inhibited the adsorption of SMX on polyethylene terephthalate (PET) and PP, but the adsorption capacity of PLA increases when salinity was above 10‰. The adsorption of SMX on microplastics was promoted by HA. When the concentration of HA was 20 mg/L, the adsorption capacity of PLA and PET decreased. Kinetic and isotherm fits were applied to the adsorption process. The increase in sorption capacity was related to the development of holes and cracks and the enhanced number of surface oxygen-containing functional groups. The adsorption kinetics to pristine microplastics conformed to a pseudo-first-order kinetic model, while the kinetics of the aged microplastics conformed to a pseudo-second-order kinetic model. It implies that the adsorption of SMX by aging microplastics involves multiple processes. The adsorption isothermal adsorption process of SMX by microplastics accorded with Freundlich model, belonging to multi-layer adsorption.
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Particuology
·
2021
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IF 3.067
Jinbo Ouyang,Jian Chen,Shaoqing Ma,Xiaohong Xing,Limin Zhou,Zhirong Liu,Chuntao Zhang
The adsorption removal of anti-inflammatory drugs from water by diverse materials has drawn great attention. This study investigated the adsorption of sulfamethoxazole (SMX) by two types of materials, UiO-66 and UiO-66-BC composites. Highly porous MOF composites with functional groups were synthesized by combining UiO-66 with corncob-based biochar at different molar ratios. SEM results showed that macroporosity of UiO-66-BC composites was increased by increasing the ratio of biochar. It was found that UiO-66-BC composites displayed highly improved adsorption performance of SMX relative to pristine UiO-66. UiO-66-BC (5%) had the highest SMX adsorption capacity, about 2.4 times those of pristine UiO-66. It was the high surface area of UiO-66 and redundant functional groups of biochar that increased the adsorption performance of composites. Moreover, UiO-66-BC can be reused and displayed the competitive adsorption efficiency after successive adsorption, which made it a potential adsorbent for the removal of SMX from water.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Yingjie Gao,Qi Zhao,Yunhe Li,Yuanqing Li,Jianfeng Gou,Xiuwen Cheng
Advanced Oxidation Processes (AOPs) play a critical role in the elimination of antibiotics, in which it is essential to explore an environmentally friendly, cheap and effective catalyst. In this study, Ag 2 O-g/eggshell catalyst had been synthesized in a simple strategy, combining with peroxymonosulfate (PMS) to simultaneous remove sulfamethoxazole (SMX). Then, physicochemical properties of catalyst were investigated by series of techniques. Results indicated the Ag species was featured with a spherical-like structure and homogeneously distributed on the surface of eggshell. In addition, Ag 2 O-Ag/eggshell exhibited high degradation efficiency of SMX by activation of PMS (94.6%) under the optimized conditions of 0.1 g•L −1 Ag 2 O-Ag/eggshell, 0.16 mM PMS, 10 mg•L −1 SMX and initial pH 6.42. Moreover, several parameters such as the dosage of catalyst, PMS and the effect of pH, co-existing anions, humic acid (HA) and water matrices on SMX degradation were systematically studied. Besides, scavenging experiments were conducted to distinguish the active radicals. Furthermore, to improve the reusability of powder Ag 2 O-Ag/eggshell, corresponding Microporous Filter Membrane had been synthesized. Subsequently, possible reaction mechanism was proposed. Consequently, these results revealed that the waste eggshell was considered as a promising supporting material for the metal catalyst for the catalytic degradation of antibiotics in water.
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ENVIRONMENTAL POLLUTION
·
2021
·
IF 8.071
Chen Sun,Tong Chen,Qunxing Huang,Xiaoguang Duan,Mingxiu Zhan,Longjie Ji,Xiaodong Li,Jianhua Yan
Porous carbons are appealing low-cost and metal-free catalysts in persulfate-based advanced oxidation processes . In this study, a family of porous biochar catalysts (ZnBC) with different porous structures and surface functionalities are synthesized using a chemical activation agent (ZnCl 2 ). The functional biochars are used to activate persulfate for sulfamethoxazole (SMX) degradation. ZnBC-3 with the highest content of ketonic group (C O, 1.25 at%) exhibits the best oxidation efficiency, attaining a rate constant ( k obs ) of 0.025 min −1 . The correlation coefficient of the density of C O to k obs ( R 2 = 0.992) is much higher than the linearity of the organic adsorption capacity to k obs ( R 2 = 0.694), implying that C O is the intrinsic active site for persulfate activation. Moreover, the volume of mesopore ( R 2 = 0.987), and Zeta potential ( R 2 = 0.976) are also positive factors in PS adsorption and catalysis. In the mechanistic study, we identified that singlet oxygen is the primary reactive oxygen species . It can attack the –NH 2 group aligned to the benzene ring to form dimer products which could be adsorbed on the biochar surface to reach complete removal of the SMX. The optimal pH range is 4–6 which will minimize the electrostatic repulsion between ZnBCs and the reactants. The SMX degradation in ZnBC/PS system was immune to inorganic anions but would compete with organic impurities in the real wastewater . Finally, the biochar catalysts are filled in hydrogel beads and packed in a flow-through packed-bed column. The continuous system yields a high removal efficiency of over 86% for 8 h without decline, this work provided a simple biochar-based persulfate catalyst for complete antibiotics removal in salty conditions.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Wenjiao Sang,Zhixuan Li,Mingjie Huang,Xiaohui Wu,Danyi Li,Longjie Mei,Jiaqi Cui
The enhanced peroxomonosulfate (PMS) activation and sulfamethoxazole (SMZ) degradation performances and mechanisms by hydroxylamine (HA) in the presence of three transition metal oxides (M x O y ), hematite (α-Fe 2 O 3 ), cobalt oxide (Co 2 O 3 ) and copper oxide (CuO) were comprehensive investigated. The results showed that proper addition of hydroxylamine (HA) can greatly promote the degradation of SMZ in the three M x O y /PMS systems. The results of electron paramagnetic resonance (EPR) study and quenching experiment suggested that OH was the dominating reactive oxygen species (ROS) in the α-Fe 2 O 3 /HA/PMS and Co 2 O 3 /HA/PMS systems, while in CuO/HA/PMS system, the activated-PMS on the surface of CuO was concluded to be responsible for SMZ degradation instead of free radicals. Furthermore, the intermediates of SMZ in the systems were detected by a high performance liquid chromatography-electrospray ionization-mass spectrometry (HPLC-ESI-MS) and the degradation pathways of SMZ system were inferred, the results indicated that due to the difference of the dominating ROS and the attack order against oxidation sites, SMZ was degraded in different pathways in α-Fe 2 O 3 /HA/PMS, Co 2 O 3 /HA/PMS and CuO/HA/PMS system. α-Fe 2 O 3 , CuO and Co 2 O 3 , could maintain stable catalytic activity in the respective reaction systems and could be efficiently recycled.
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RADIATION PHYSICS AND CHEMISTRY
·
2019
·
IF 1.984
Run Zhuan,Jianlong Wang
Degradation of sulfamethoxazole (SMX) by ionizing radiation combined with goethite (α-FeOOH) catalyzed Fenton-like process were studied under various conditions. The results showed that SMX could be degraded completely at 2 kGy with or without the addition of goethite. This process followed pseudo first-order kinetics model. The presence of goethite promoted the mineralization of SMX, and the mineralization ratio increased with the increase of goethite dosage. The decomposition of SMX in goethite/ionizing radiation system exhibited high activity at pH ranging from about 3.0 to 11.0. Acidic condition was more preferable than alkaline condition for the degradation of SMX. The presence of humic acid inhibited SMX degradation, due to the competition of hydroxyl radical with SMX molecules. The addition of tert butyl alcohol (TBA) resulted in the decrease of SMX removal efficiency, indicating that hydroxyl radical played the main role in this system. This investigation demonstrated that goethite combined with ionizing radiation has potential for enhancing the mineralization of toxic organic pollutants in water and wastewater.
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CHEMOSPHERE
·
2024
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IF 8.1
Peng Yi,Xiao Shu,Chenhui Wang,Mingfu Li,Yu Huang,Min Wu,Lijuan Zhang,Quan Chen
The coexistence of metal cations is often accompanied by organic pollution and could affect the environmental fate of organics by mediating the formation of cation bridges. However, the environmental fate and risk of organics in cation co-existing environments are poorly understood due to the lack of accurate identification of cation bridge formation and stability. In this study, the sorption of sulfamethoxazole (SMX) on montmorillonite (MT) with the coexistence of three different valence metal cations (Na + , Ca 2+ , and Cr 3+ ) was investigated. Ca 2+ and Cr 3+ can significantly promote the sorption of SMX on MT for about 5∼10 times promotion, respectively, while Na + bridges displayed little effect on the sorption of SMX. The sorption binding energy of SMX with MT-Ca (−44.01 kcal/mol) and MT-Cr (−64.57 kcal/mol) bridges was significantly lower than that with MT-Na (−38.45 kcal/mol) and MT (−39.39 kcal/mol), indicating that the sorption affinity of SMX on Cr and Ca bridges was much stronger. The higher valence of the cations also resulted in a more stable adsorbed SMX with less desorption fluctuation. In addition, the relatively higher initial concentration of SMX and the valence of cations increased the bonding density of the cation bridges, thus promoting the apparent sorption of SMX on MT to a certain extent. This work reveals the formation and function of cation bridges in the sorption of SMX on MT. It lays a theoretical foundation for further understanding the environmental fate and risk of organics.
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MOLECULES
·
2024
·Vol. 29
·期 10
·2276
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IF 4.2
Qun Xue,Zhihui Chen,Wenjing Xie,Shuke Zhang,Jie Jiang,Guoxin Sun
Bioelectrochemical systems (BESs) are an innovative technology for the efficient degradation of antibiotics.Shewanella oneidensis(S. oneidensis) MR-1 plays a pivotal role in degrading sulfamethoxazole (SMX) in BESs. Our study investigated the effect of BES conditions on SMX degradation, focusing on microbial activity. The results revealed that BESs operating with a 0.05 M electrolyte concentration and 2 mA/cm2current density outperformed electrolysis cells (ECs). Additionally, higher electrolyte concentrations and elevated current density reduced SMX degradation efficiency. The presence of nutrients had minimal effect on the growth ofS. oneidensisMR-1 in BESs; it indicates thatS. oneidensisMR-1 can degrade SMX without nutrients in a short period of time. We also highlighted the significance of mass transfer between the cathode and anode. Limiting mass transfer at a 10 cm electrode distance enhancedS. oneidensisMR-1 activity and BES performance. In summary, this study reveals the complex interaction of factors affecting the efficiency of BES degradation of antibiotics and provides support for environmental pollution control.
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