Sustainability
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2025
·Vol. 17
·期 8
·3359
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IF 3.3
Zhiqi Lu,Mengzhe Zhao,Xianglong He,Hongjing Li
Perfluorooctanoic acid (PFOA), an emerging organic contaminant frequently detected in wastewater, inhibits biological nitrogen removal processes, posing challenges to sustainable wastewater treatment. Mitigating the adverse effects of PFOA while enhancing total nitrogen (TN) removal efficiency remains a critical concern. In this study, three sequencing batch biofilm reactors (SBBRs) were operated under low-oxygen conditions with a C/N ratio of 4.0 to investigate enhanced nitrogen removal under PFOA stress using biochar. Compared to the 78.1% TN removal efficiency in the control reactor (SBBR-0) with an initial TN concentration of 50 mg/L, the addition of PFOA decreased TN removal by 2.3% in SBBR-1, while the combined addition of PFOA and biochar increased it by 3.2% in SBBR-2. Biochar, acting through its electron-donating surface functional groups, mitigated PFOA-induced reactive oxygen species accumulation and increased adenosine triphosphate production. These effects promoted the generation of quorum sensing (QS) signaling molecules, facilitating microbial communication and cooperation. Consequently, the relative abundance of key nitrogen-removing bacteria, such asThauera(from 7.90% to 9.92%) andNitrosomonas(from 1.42% to 5.75%), increased, leading to enhanced nitrogen removal efficiency. A metagenomic analysis revealed that biochar significantly reduced the production of antibiotic resistance genes without promoting their dissemination. These findings provide new insights into mitigating the negative effects of PFOA and improving TN removal through QS promotion, offering a potential approach for enhancing the sustainability of wastewater treatment systems.
研究领域:
环境科学
·
微生物学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Jiaxin Zhu,Yihua Chen,Yurong Gu,Hang Ma,Mingyue Hu,Xinlei Gao,Tongzhou Liu
The discharge of widely used per- and poly-fluorinated compounds (PFCs) leads to their environmental prevalence, bioaccumulation and biotoxicity; and attracts researches focusing on their treatment in wastewater. Electrochemical reductive treatment is a promising alternative due to its milder reaction conditions and easy operation. The feasibility of electrochemical reductive decomposition of PFOA using a Rh/Ni cathode was explored. The Rh/Ni cathode was fabricated by coating Rh 3+ on Ni foil through electrodeposition . The Rh coating was primarily elemental and in a Rh(111) crystalline form. PFOA decomposition and defluorination were observed when using the Rh/Ni cathode where DMF was the solvent and the cathode potential was −1.25 V. A hydrodefluorination reaction was considered having occurred. Because possessing d electrons and empty d orbitals, the Rh coating enhanced PFOA adsorption onto the cathode surface and facilitated C F bond activation through Rh···F interactions. Moreover, the Rh(111) crystal helped chemisorb the generated H* and supply it participating in PFOA decomposition. With the continuous interaction of cathode-supplied electrons, C F bond would ultimately dissociate and transform to C H bond by H* substitution. Adding FeCp 2 * as a supporting electrolyte enhanced PFOA decomposition by working as the shuttle facilitating PFOA migration to the cathode surface.
研究领域:
环境科学
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电化学
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污染治理
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DOI
PubMed
高影响因子
CHEMOSPHERE
·
2017
·
IF 4.208
Dan Wu,Xukai Li,Yiming Tang,Ping Lu,Weirui Chen,Xiaoting Xu,Laisheng Li
Zinc oxide (ZnO) nanorods were prepared by a directly pyrolysis method and employed as catalyst for perfluorooctanoic acid (PFOA) degradation. Comparative experiments were conducted to discuss the catalytic activity and flexibility of ZnO. After ZnO addition, the best PFOA degradation efficiency (70.5%) was achieved by ZnO/UV/O 3 system, only 9.5% by sole ozonation and 18.2% by UV 254 light irradiation. PFOA degradation was sensitive with pH value and temperature. The better PFOA removal efficiency was achieved at acidic condition. A novel relationship was found among PFOA degradation efficiency with hydroxyl radicals and photo-generated holes. Hydroxyl radicals generated on the surfaces of ZnO nanorods played dominant roles in PFOA degradation. PFOA degradation was found to follow the photo-Kolbe reaction mechanism. C 2 –C 7 shorter-chain perfluorocarboxylic acids and fluoride ion were detected as main intermediates during PFOA degradation process. Based on the results, a proposal degradation pathway was raised.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2020
·
IF 9.13
Ruya Chen,Yuan Zhuang,Ying Yu,Baoyou Shi
Particulate manganese oxide (MnOx) deposition in drinking water distribution systems (DWDS) gives rise to the risk of water discoloration at the consumers’ tap; however, its role in the fate and transport of trace organic pollutants in DWDS is not clear. Perfluorooctanoic acid (PFOA), a persistent organic pollutant frequently detected in natural water, was selected to investigate the potential effect of MnOx on its transportation behavior under DWDS conditions through laboratory batch experiments. The results show that PFOA can be greatly combined with MnOx formed in-situ through a Mn(II) oxidation process by free chlorine. However, the accumulation of PFOA by preformed MnOx was negligible. It was found that 1 mg/L Mn captured over 50% of PFOA with an initial concentration of 50 ng/L during oxidation. The water compositions of actual water could contribute to the effect of PFOA accumulation to a certain extent. Characterization of the solid products revealed that PFOA is homogenously embedded into MnOx. The combination of PFOA with MnOx occurs through a bridging effect of Mn(II) between the surface hydroxyls of MnOx and the -COOH group of PFOA. The resulting MnOx-PFOA particles were more inclined to agglomerate, enabling possibly easy deposition onto the pipe wall than ordinary MnOx particles. This study provides insights into the co-occurrence of metal deposits with PFOA and the potential risks posed by PFOA accumulation to consumers through the water distribution process.
研究领域:
环境科学
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水处理工程
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Yuancai Lv,Shiyu He,Shuting Liu,Zhendong Yu,Yanting Jiang,Yihui Hu,Yifan Liu,Chunxiang Lin,Xiaoxia Ye,Guifang Yang,Minghua Liu
Doping polymetals on Fe-based catalysts is proved to be an effective way to improve the performance on activating persulfate. In this paper, a highly efficient persulfate activation catalyst (FeCo@MoS 2 ) was successfully synthesized by introducing MoS 2 onto the surface of FeCo nanoboxes. During the activation of PMS the introduced of MoS 2 effectively promoted the formation of free radicals (∙OH, SO 4 · - ), 1 O 2 and Fe(IV). Due to the synergistic effects between Mo and Fe, FeCo@MoS 2 has better catalytic activity (2.01 times larger of defluorination efficiency and 3.91 times larger of the apparent rate constant ( k obs )) than FeCo. Under the optimal conditions (catalyst dosage of 0.2 g L −1 , PMS dosage of 1.0 g L −1 and initial pH 4.0), the perfluorooctanoic acid (PFOA, 10 mg L −1 ) could be degraded in 60 min, with 90.26 ± 2.64% of the defluorination efficiency. The LC- MS results showed that under the attack of free radicals (∙OH, SO 4 · - ), 1 O 2 and Fe(IV), the PFOA underwent step-by-step defluorination process. In addition, the ECOSAR results showed that during the whole degradation of PFOA in FeCo@MoS 2 /PMS system, no highly toxic intermediates was accumulated, suggesting a green degradation process. This work showed new ideas and strategies for studying the influence of polymetallic doping on the catalytic process of PMS multiphase catalytic system.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2025
·Vol. 91
·期 5
·609-625
·
IF 2.6
Li Shuilian,Zhang Lishan,Zhong Shan,Zhu Jiayan,Wei Zengxian
View large Download slide View large Download slide Close modal This study reports the preparation of granular ternary micro-electrolysis materials and their effectiveness in removing the emerging contaminant PFOA. Al/nZVI/C@F granules were synthesized using a liquid-phase reduction method combined with high-temperature calcination. By comparing the removal of methylene blue dye by granules, the optimum preparation conditions were determined as follows: Fe:C = 5:1, fly ash = 50%, calcination temperature = 800 °C, and holding time = 1 h. Static batch experiments revealed that under optimal conditions (PFOA concentration = 25 mg/L, solid–liquid ratio = 30 g/L, pH = 3, reaction temperature = 15 °C), Al/nZVI/C@F achieved a PFOA removal rate of 97.83%. The removal efficiency of Al/nZVI/C@F (93.90%) was significantly higher than that of commercial iron-carbon (12.75%). After 45 days of dynamic column experiments, the removal efficiency of nZVI/C@F and Al/nZVI/C@F for PFOA (50 mg/L) remained above 60%, demonstrating strong practical application potential. Further adsorption–desorption experiments revealed that nZVI/C@F and Al/nZVI/C@F primarily removed 50 mg/L PFOA through adsorption. For a lower PFOA concentration of 0.5 mg/L, the defluorination rates were 53.2% for nZVI/C@F and 68.9% for Al/nZVI/C@F. High-performance liquid chromatography-tandem mass spectrometry was used to analyze the intermediates formed during PFOA removal, leading to a proposed degradation pathway. Developed Al/nZVI/C via liquid-phase reduction and high-temperature calcination. Proven efficacy in PFOA removal from water using fly ash-Al/nZVI/C@F granules. Identified adsorption as the primary mechanism for over 50% PFOA removal. Degradation of PFOA to form short-chain fluorinated intermediates. The materials hold promise for PFOA removal in water treatment applications.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Fengjie Chen,Anen He,Yarui Wang,Wanchao Yu,Haoze Chen,Fanglan Geng,Zhunjie Li,Zhen Zhou,Yong Liang,Jianjie Fu,Lixia Zhao,Yawei Wang
Photo-induced holes (h + ) oxidation is an efficient approach for perfluorooctanoic acid (PFOA; C 7 F 15 COOH) removal. To maintain a high amount of h + on the surface of photocatalysts participating in the PFOA photodegradation could be a critical issue. Herein, a highly efficient spherical BiOBr-modified nano-TiO 2 (P25) was synthesised and used for PFOA photodegradation through direct oxidation with h + . A high number of h + could be generated and remain on the surface of P25/BiOBr due to the appropriate position of the conduction band (CB) and valence band (VB) levels between P25 and BiOBr. Meanwhile, PFOA molecules were coordinated to the P25/BiOBr's surface via unidentate binding, being directly activated and oxidised by h + , resulting in a decomposition yield of 99.5% (100 mg/L) under simulated solar light irradiation within 100 min, at the initial pH condition (3.5). A stepwise photodegradation pathway was proposed due to the significant intermediates detected as the short-chain perfluorinated carboxylic acids (C2–C7). Reactive oxygen species (ROS) generation, scavenging and trapping analysis indicated that the direct oxidation on h + followed PFOA degradation. In a real aqueous environment of Tangxun lake (adjusted pH 3.5), stable common anions and natural organic matter (NOM) would restrain the PFOA photodegradation. However, adding 10 mg/L of NO 3 − or HA could reduce the inhibition effect of PFOA photodegradation. These findings gave an alternative strategy to drive an h + directly oxidation to treat PFOA contaminated water bodies.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jiaoqin Liu,Chengjie Guo,Nannan Wu,Chenguang Li,Ruijuan Qu,Zunyao Wang,Riya Jin,Yina Qiao,Zengdi He,Jing Lu,Xingqiao Feng,Yufan Zhang,Anlong Wang,Jingshuai Gao
In this work, the kinetics and mechanisms of photocatalytic degradation of perfluorooctanoic acid (PFOA) by nitrogen-doped indium trioxide (N-doped In 2 O 3 or NH 4 NO 3 -In 2 O 3 ) under Xe lamp irradiation were systematically investigated. Nitrogen originating from various inorganic and organic nitrogen compounds was doped into In 2 O 3 to examine the catalytic effect. The NH 4 NO 3 -In 2 O 3 catalyst was characterized by SEM , TEM, FT-IR, UV-DRS, BET surface area, XPS, and XRD , and showed the best catalytic performance. After 18 h of irradiation, PFOA was almost completely degraded with addition of 5 mg catalyst, while it was hardly degraded by simulated sunlight alone. The low photocatalytic degradation efficiency of PFOA was observed in different natural waters, which was due to the inhibitory effect of high pH and common anions like SO 4 2− . The calculation results of Materials Studio showed that a shoulder-to-shoulder π system between nitrogen atom and oxygen atom (NO π*) was formed after nitrogen doping into interstitial sites of In 2 O 3 , therefore resulting in a reduction in band gap energy. Occupied NO π* states were responsible for the red shift, while unoccupied NO π* levels restrained the recombination of electrons (e − ) and holes (h + ). Nitrogen doping reduced the excitation energy for electronic transition, and thus accelerated the reaction. According to mass spectrometry analysis, decarboxylation and elimination were still the main photodegradation pathways of PFOA. To the best of our knowledge, this report is the first to explore the reaction mechanisms of PFOA in an N-doped In 2 O 3 /Xe lamp irradiation system.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Zhiyuan Liu,Fan Yang,Tingting Zhai,Jianwei Yu,Chunmiao Wang,Zhengang Liu,Zhixue Liu,Yingxin Gao,Min Yang
Activated carbon (AC) adsorption is a practical process for the removal of perfluorooctanoic acid (PFOA) in aquatic environments, but the relationship between its pore structure and adsorption performance is not well understood. In this study, the KOH-activated carbons (KACs) with different tailored pore structures were prepared, and presented a 2.61-fold higher adsorption capacity and a 2.21-fold higher adsorption rate than the raw AC. An in situ characterization method and a modified adsorption model were introduced to investigate the impact of pore size, which demonstrated that the ultra-micropores (<1.2 nm) and small mesopores (2.0–3.0 nm) contributed significantly to the adsorption of PFOA, with the highest mean contribution factor ( k ) of 0.45 and the second highest of 0.39, respectively. Molecular dynamics simulations revealed that PFOA molecules tend to attach to the pore walls at various pore sizes. The adsorption of PFOA in the ultra-micropores was dominated by enhanced interactions due to the overlapping potentials of the bilateral pore walls (maximum of −567.32 Kcal·mol −1 ) and hydrophobic interactions. PFOA micelles or hemi-micelles could be formed in the small mesopores, allowing them to function as both the molecule transportation channels and strong adsorption sites. This study would guide the development of activated carbon tailored for the selective adsorption of PFOA from water.
研究领域:
环境科学
·
水处理
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2022
·
IF 6.796
Wenjing Tang,Yunyi Meng,Bin Yang,Dongyu He,Yan Li,Bojun Li,Zheming Shi,Changwei Zhao
Nanofiltration (NF) process has become one of the most promising technologies to remove micro-organic combined water pollution . Developing a NF membrane material with efficient separation for perfluorooctanoic acid (PFOA) combined pollution is highly desired, this manuscript targets this unmet need specifically. In this work, hydrophilic SiO 2 nanoparticles with various contents blended with carboxylic multiwalled carbon nanotube were used to modify poly (m-phenylene isophthal amide) (SiO 2 /CMWCNT/PMIA) hollow fiber NF membrane. The modified membrane with 0.1 wt% SiO 2 doping exhibits way better fouling resistance with irreversible fouling ratio decreased dramatically from 18.7% to 2.3%, and the recovery rate of water flux increases significantly from 81.2% to 97.7%. The separation experiment results had confirmed that the modified membrane could improve the rejection from 97.2% to 98.6% for perfluorooctanoic acid (PFOA) and its combined pollution with bovine serum albumin (BSA). It is clear that this reported SiO 2 /CMWCNT/PMIA hollow fiber NF membrane potentially could be applied in water treatment . This research also provides a theoretical basis for efficiently removal of PFOA and its combined pollution by NF membrane.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Xiaoyuan Wang,Yinchuan Lv,Xin Qiang,Shumin Liang,Ruosi Li,Jing Zhan,Jiaying Liu
The disruption of per- and polyfluoroalkyl substances (PFASs) on bile acid (BA) homeostasis has raised public concerns, making the evaluation of their effects and underlying mechanisms a high priority. Although the use of perfluorooctanoic acid (PFOA) has been restricted, it remains a widespread legacy PFAS in the environment. Concurrently, the use of its prevalent short-chain alternative, perfluorobutanoic acid (PFBA), is increasing, yet the toxicity assessment of PFBA remains inadequate. In this study, C57BL/6N mice were exposed to PFOA and PFBA (0.4 or 10 mg/kg body weight) by gavage for 28 days. The results showed that both PFOA and PFBA significantly increased hepatic weight, although PFBA exhibited lower bioaccumulation than PFOA in the liver. Targeted metabolomics revealed that PFOA significantly decreased total BA levels and altered their composition. Conversely, PFBA, without significantly altering total BA levels, notably changed their composition, such as increasing the proportion of cholic acid. Further investigations using in vivo and in vitro assays suggested that PFOA inhibited the expression of Cyp7A1, a key BA synthetase, potentially via PPARα activation, thereby reducing BA levels. In contrast, PFBA enhanced Cyp7A1 expression, associated with the inhibition of intestinal Farnesoid X receptor-fibroblast growth factor 15 (FXR-FGF15) pathway. This study evaluated the differences in the BA-interfering effects of PFOA and PFBA and shed light on the potential mechanisms, which will provide new insights into the health risks of legacy PFASs and their alternatives.
研究领域:
毒理学
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环境健康
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代谢组学
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分子生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2020
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IF 3.594
Yang Liu,Jia Bao,Xiao-Min Hu,Gui-Lin Lu,Wen-Jing Yu,Zhen-Hao Meng
Water bodies of numerous countries and regions in the world have been contaminated to various extents with the widespread production and usage of perfluoroalkyl substances (PFASs). Both domestic and industrial wastewaters become one of the important sources for the PFAS contaminations in natural water bodies, due to the incomplete treatment. Usually, the artificial wastewaters are complex and have high concentrations of inorganic salts, which could result in the matrix effects during the process of analysis for PFASs, contributing to quantify the target compounds inaccurately. In order to monitor the concentrations of PFAS contaminants precisely, suitable extraction methods were compared focusing on the matrix effects and characters of green analytical chemistry during the detection of perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) existing with several common inorganic salts in wastewaters. The results showed that the analytical values of PFOA and PFOS were 2.8–3.6 times and 3.0–5.2 times higher than the theoretical values, respectively. The liquid-liquid extraction (LLE) and solid phase extraction (SPE) methods were used to reduce the matrix effects originated from inorganic salts, consequently the SPE method was confirmed as the optimal extraction method, based upon both the recoveries and green procedures. Combined with the application of the best parameters in real industrial wastewaters, indicating the present study would provide an accurate and green quantitative analysis of PFASs in salty wastewaters.
研究领域:
环境科学
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分析化学
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产品关联
DOI
高影响因子