ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Zhen Cao,Hao Li,Gregory V. Lowry,Xiaoyang Shi,Xiangcheng Pan,Xinhua Xu,Graeme Henkelman,Jiang Xu
Groundwater contamination by halogenated organic compounds, especially fluorinated ones, threatens freshwater sources globally. Sulfidized nanoscale zero-valent iron (SNZVI), which is demonstrably effective for dechlorination of groundwater contaminants, has not been well explored for defluorination. Here, we show that SNZVI nanoparticles synthesized via a modified post-sulfidation method provide rapid dechlorination (∼1100 μmol m–2 day–1) and relatively fast defluorination (∼6 μmol m–2 day–1) of a halogenated emerging contaminant (florfenicol) under ambient conditions, the fastest rates that have ever been reported for Fe0-based technologies. Batch reactivity experiments, material characterizations, and theoretical calculations indicate that coating S onto the metallic Fe surface provides a highly chemically reactive surface and changes the primary dechlorination pathway from atomic H for nanoscale zero-valent iron (NZVI) to electron transfer for SNZVI. S and Fe sites are responsible for the direct electron transfer and atomic H-mediated reaction, respectively, and β-elimination is the primary defluorination pathway. Notably, the Cl atoms in florfenicol make the surface more chemically reactive for defluorination, either by increasing florfenicol adsorption or by electronic effects. The defluorination rate by SNZVI is ∼132–222 times higher with chlorine attached compared to the absence of chlorine in the molecule. These mechanistic insights could lead to new SNZVI materials for in situ groundwater remediation of fluorinated contaminants.
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
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Junjing Li,Han Yu,Yongjiao Ding,Liang Wang
In order to improve the metal utilization of the noble metal Pd and the catalytic activity of the reaction, a novel and efficient Pd/Ti 4 O 7 /Ti electrode was prepared by introducing a Ti 4 O 7 intermediate layer for electrocatalytic hydrodechlorination (EHDC) of chlorinated pharmaceuticals and personal care products (PPCPs). The presence of oxygen vacancies (Ov) on the Ti 4 O 7 surface was confirmed by electron paramagnetic resonance (EPR). The results showed that the introduction of Ti 4 O 7 increased the electrochemical active surface area electrode (ECSA) of the Pd/Ti 4 O 7 /Ti electrode, accelerated the electron transfer rate on the catalyst surface, and promoted the generation of electron-rich Pd, which in turn improved the dechlorination efficiency. The Pd/Ti 4 O 7 /Ti electrode had a removal efficiency of 99.6% for florfenicol (FLO) within 180 min. Meanwhile, the removal efficiency of the Pd/Ti 4 O 7 /Ti electrode was still above 95% in seven cycles, which significantly improved the catalytic activity and stability compared with that of the Pd/Ti electrode. In addition, the reaction pathway for the electrocatalytic hydrodechlorination process of FLO at Pd/Ti 4 O 7 /Ti electrode was proposed. The ecotoxicity of the pollutants was also evaluated by the Toxicity Estimation Software Tool (T.E.S.T) model. In this study, an efficient electrocatalyst for EHDC was explored, and the Pd/Ti 4 O 7 /Ti electrode provided strong support for pollutant removal.
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 THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 8
·B654
·
IF 3.12
Ya-Mu Xia,Wen Zhang,Meng-Ying Li,Meng Xia,Li-Jia Zou,Wei-Wei Gao
In this paper, a highly effective electrochemical sensor based on graphene (Gr)/copper phthalocyanine (CuPc) nanocomposites was successfully designed and achieved. The morphology of Gr/CuPc nanocomposites was characterized by UV-vis, IR, Raman spectra and scanning electron microscopy (SEM). Gr/CuPc nanocomposites were gathered on the surface of the glassy carbon electrode (GCE), and the performence of Gr/CuPc/GCE toward chloramphenicol (CAP) and florfenicol (FF) was investigated by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). The Gr/CuPc/GCE presented good electrochemical properties, stability, reproducibility, excellent anti-interference ability and satisfying recovery rate in real samples for the detection of CAP and FF. The performance of Gr/CuPc/GCE exhibited a linear ranging from 1.0 × 10−7 to 2.0 × 10−5 M with a detection limit of 2.7 × 10−8 M (−0.652 V vs. Hg/Hg2Cl2, S/N = 3) toward CAP. For FF, it exhibited a linear ranging from 1.0 × 10−6 to 3.0 × 10−5 M with a detection limit of 7.5 × 10−7 M (−0.863 V vs. Hg/Hg2Cl2, S/N = 3). Furthermore, it is for the first time that FF is determined by electrochemical sensor through nanocomposites modified electrode. This proposed electrochemical sensor can provide an opportunity for convenient and reliable determination of CAP or FF.
研究领域:
分析化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Selvendiran Periyasamy,Xiaochang Lin,Soliu O. Ganiyu,Sathish-Kumar Kamaraj,Abdoulaye Thiam,Dezhao Liu
Antibiotics in the environment provoke serious consequences on living beings and can be effectively remediated by prominent advanced oxidation process . In this study, electrochemical advanced oxidation treatment in a lab-scale reactor for the degradation of florfenicol (FLO) was studied with the aid of boron-doped diamond anode (BDD). The results exhibited that the FLO degradation follows pseudo-first-order kinetics. As the current intensity rose from 60 mA to 250 mA, the FLO removal efficiency increased and the corresponding reaction rate constant increased from 0.0213 to 0.0343 min −1 , which was likely due to the more efficient participation of free hydroxyl radical ( • OH) generated at the BDD anode. Faster degradation and higher mineralization of electrolyzed FLO solution were achieved at higher current intensity as well as in higher SO 4 2− concentration medium, as a consequence of catalytic participation of oxidants (free • OH as well as sulfate radical (SO 4 •− ) and persulfate (S 2 O 8 2− )). The increase in FLO concentration from 30 to 50 mg L −1 resulted in a reaction rate constant decrease (from 0.0235 to 0.0178 min −1 ). Eight transformation by-products ( m/z = 372.99, 359.8, 338.0, 324.04, 199.00, 185.02, 168.99 and 78.989) and three inorganic ions (NO 3 − , Cl − and F − ) were analyzed by UPLC‒Q‒TOF‒MS/MS and Ion‒chromatography, respectively. The Vibrio fischeri bioluminescence inhibition revealed an increase of toxicity during the electrochemical oxidation that could be attributed mostly to the generated organic chlorinated by-products ( m / z = 372.99, 359.8) and inorganic species (ClO 2 − and ClO 3 − ).
研究领域:
环境科学
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电化学工程
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毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2018
·
IF 3.849
Huaxuan Zhao,Yinhai Lang
A magnetic reed biochar (MRBC) was synthesized through chemical co-precipitation firstly and subsequently pyrolysis. The MRBC and reed biochar (RBC) were characterized by SEM, XRD, FTIR and VSM and were used for the adsorption of florfenicol (FF). Batch experiment results showed that the FF adsorption on MRBC exhibited a pronounced pH-dependent pattern and presented a bell curve. However, the FF adsorption on RBC decreased gradually with the increasing pH values. Ionic strength initially inhibited and then promoted the FF adsorption and the multivalent co-existing anions significantly increased the FF adsorption on MRBC. The FF adsorption was non-spontaneous, exothermic and entropy-decreasing on MRBC and was of a non-spontaneous, endothermic and entropy-increasing nature on RBC. The pseudo second-order model presented better fittings for the FF adsorption kinetic data. Langmuir and Freundlich models can well describe FF adsorption on MRBC and RBC, respectively. The FF adsorption on RBC may be controlled by pore-filling effect and π–π EDA interaction, while hydrogen bonding, pore-filling effect and π–π EDA interaction contributed to the FF adsorption on MRBC. The adsorption–regeneration cycles confirmed that the MRBC was a highly efficient and reusable adsorbent for the removal of FF from aqueous solution.
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
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2023
·Vol. 24
·期 5
·4412
·
IF 5.6
Xinping Guo,Ziang Qian,Qiqi Pan,Yuqing Hu,Wangxin Mei,Xiumei Xing,Shaowu Yin,Jie Ji,Kai Zhang
Excessive use of antibiotics in aquaculture causes residues in aquatic animal products and harms human health. However, knowledge of florfenicol (FF) toxicology on gut health and microbiota and their resulting relationships in economic freshwater crustaceans is scarce. Here, we first investigated the influence of FF on the intestinal health of Chinese mitten crabs, and then explored the role of bacterial community in FF-induced intestinal antioxidation system and intestinal homeostasis dysbiosis. A total of 120 male crabs (48.5 ± 4.5 g) were experimentally treated in four different concentrations of FF (0, 0.5, 5 and 50 μg/L) for 14 days. Responses of antioxidant defenses and changes of gut microbiota were assessed in the intestine. Results revealed that FF exposure induced significant histological morphology variation. FF exposure also enhanced immune and apoptosis characteristics in the intestine after 7 days. Moreover, antioxidant enzyme catalase activities showed a similar pattern. The intestinal microbiota community was analyzed based on full-length 16S rRNA sequencing. Only the high concentration group showed a marked decrease in microbial diversity and change in its composition after 14 days of exposure. Relative abundance of beneficial genera increased on day 14. These findings illustrate that exposure to FF could cause intestinal dysfunction and gut microbiota dysbiosis in Chinese mitten crabs, which provides new insights into the relationship between gut health and gut microbiota in invertebrates following exposure to persistent antibiotics pollutants.Keywords:florfenicol;gut barrier;apoptosis;gut microbiota;crab
研究领域:
水产养殖
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毒理学
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微生物学
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动物健康
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产品关联
DOI
PubMed
高影响因子
Journal of Saudi Chemical Society
·
2024
·
IF 5.8
Zhengjie Li,Miao Liu,Chunxia Fang,Huanshu Zhang,Tianyi Liu,Yixian Liu,Heli Tian,Jilong Han,Zhikun Zhang
The widespread use and subsequent accumulation of florfenicol (FFC), a common antibiotic, through the food chain poses significant risks to aquatic ecosystems and human health, necessitating effective strategies for its removal from water bodies. To solve the challenge, herein, we developed a novel aluminum-based metal–organic framework CAU-1, engineered for the efficient adsorption of FFC. CAU-1 contains the plentiful –NH 2 and μ-OH groups with the positively charged on the surface. In the adsorption process, CAU-1 perform hydrogen bonding interactions with FFC’s functional groups (−F, –OH, −Cl, –NH–, and −SO 2 –). Furthermore, the positively charged surface of CAU-1 enhances FFC adsorption via electrostatic attraction together. FFC adsorption equilibrium on CAU-1 is attained within 180 min with a monolayer adsorption capacity of 386 mg/g at 303 K, surpassing most of the reported adsorbents. The exothermic FFC adsorption process on CAU-1 remains largely unaffected by coexisting ions. Additionally, CAU-1 can be efficiently regenerated using a mixed solution of 0.1 M HCl and ethanol–water as an eluent. This work highlights CAU-1’s potential as an effective adsorbent for FFC removal, emphasizing the importance of tuning or designing surface functional groups on adsorbents to boost their adsorption capabilities.
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
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2019
·
IF 7.149
Huiling Liu,Jinglong Han,Jili Yuan,Chengbin Liu,Dong Wang,Tian Liu,Meijun Liu,Jinming Luo,Aijie Wang,John C. Crittenden
Efficient elimination of antibacterial activity of halogenated antibiotics by dehalogenation pretreatment is desired for a biochemical treatment process. In this study, crystalline cobalt phosphide nanosheet arrays on a Ti plate (C-CoP/Ti) are fabricated by a simple electrodeposition and phosphorization process. The crystalline structure greatly promotes atomic hydrogen (H*) generation. Moreover, the nanosheet arrays can provide abundant active sites and accelerate electron transfer and mass transport. As a result, the dehalogenation rate of florfenicol (FLO, an emerging organic pollutant) on C-CoP/Ti is 11.1, 2.97, and 13.6 times higher than that on amorphous CoP/Ti, Pd/Ti, and bare Ti, respectively. The C-CoP/Ti electrode achieves 97.4% dehalogenation of FLO (20 mg L–1) within 30 min at −1.2 V (vs Ag/AgCl). Nearly 100% of Cl and 20% of F are broken away within 120 min, showing the highest electrocatalytic defluorination efficiency reported so far. Both experimental results and theoretical calculations reveal that the dehalogenation of FLO on C-CoP/Ti is synergistically accomplished via direct reduction of electron transfer and indirect reduction of H*. This study develops a highly efficient non-noble metal electrode material for dehalogenation of halogenated organic compounds.
研究领域:
环境科学
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材料科学
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化学
✓ 已验证
DOI
PubMed
高影响因子
CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
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2018
·
IF 0.824
Ran LI,Ze-Jia LIN,Jin-Yi YANG,Zhen-Lin XU,Hong WANG,Hong-Tao LEI,Yuan-Ming SUN,Yu-Dong SHEN
A high-affinity polyclonal antibody was prepared by immunizing animals with haptens FFD and FFM. Under the optimal combination of coating antigen and antibody, an indirect competitive enzyme-linked immunosorbent assay (icELISA) for simultaneous detection of florfenicol and thiamphenicol residues in animal meat and urine samples was developed. The icELISA showed an IC 50 value of 1.32 ng mL −1 for florfenicol and 2.13 ng mL −1 for thiamphenicol, respectively. The linear ranges were from 0.31 to 5.61 ng mL −1 with a limit of detection of 0.12 ng mL −1 for florfenicol, and 0.41 to 11.2 ng mL −1 with a limit of detection of 0.15 ng mL −1 for thiamphenicol, respectively. The average recoveries of florfenicol and thiamphenicol in spiked samples ranged from 77.2% to 116.0% with a relative standard deviation of less than 15%. Therefore, this proposed icELISA provided a valid detection method for florfenicol and thiamphenicol residues in animal tissue and urine samples.
研究领域:
免疫学
·
食品安全检测
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jianhui Xu,Xin Fu,Yufeng Liu,Yunfei Zhang,Shenggui Chen,Dan Li,Chunhui Zhang,Jiale Gao,Yibo Fu
Electrocatalytic hydrodechlorination technology provides an attractive strategy to effectively eliminate the biotoxicity of halogenated organic pollutants (HOPs). Herein, we demonstrated a highly dispersed Pd loaded on blue TiO 2 nanotube arrays (Pd x -BTNA) cathode that can achieve efficient dechlorination and detoxification toward florfenicol (FLO). Characterization results indicated that strong interaction between Pd and BTNA was achieved through Pd-O bonds, which facilitated the electron transfer rate. Pd x -BTNA significantly outperformed other cathodes (i.e., BTNA, Pd x -TNA and Pd x -Ti) in the electrocatalytic dechlorination of FLO due to enhanced utilization of active H*. The dechlorination performances of FLO well followed the pseudo-first-order kinetic, and the reaction constant rate on Pd x -BTNA cathode (0.035 min −1 ) was 17.5, 1.94, 7.0 times higher than that on BTNA, Pd x -TNA and Pd x -Ti cathodes, respectively. Quenching experiments and electrochemical characterization indicated that both direct electron transfer and indirect reduction process mediated by H* were involved in the dechlorination of FLO. The optimal dechlorination efficiency of 98.79% was obtained by Pd x -BTNA cathode within 120 min at 1 mM PdCl 2 , applied cathode potential of −1.2 V. In addition, Pd x -BTNA exhibited superior stability and durability with almost no Pd leaching (0.0011 mg/L) during five dechlorination cycles. Our research proposed a novel strategy to design low noble Pd-loaded cathode material for efficient dechlorination and detoxification of HOPs.
研究领域:
环境科学
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材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROPHORESIS
·
2024
·
IF 3
Weiyan Li,Chuansheng Sun,Haiping Wang,Qingyan Bai,Yi Xu,Chunmiao Bo,Junjie Ou
Detection of florfenicol (FF) residues in animal-derived foods, as one of the most widely used antibiotics, is critically important to food safety. The fluorescent molecularly imprinted polymer (MIP) was synthesized by surface-initiated atom transfer radical polymerization technique with poly(glycidyl methacrylate- co -ethylene glycol dimethacrylate) microspheres, 4-vinylpyridine, ethylene glycol dimethacrylate, and FF as the matrix, functional monomer, crosslinker, and template molecule, respectively. Meanwhile, N–S co-doped carbon dot (CD) was synthesized with triammonium citrate and thiourea as precursors under microwave irradiation at 400 W for 2.5 min and then integrated into FF-MIP to obtain CD@FF-MIP. For comparison, non-imprinted polymer (NIP) without FF was also prepared. The adsorption capacity of CD@FF-MIP to FF reached 53.1 mg g −1 , which was higher than that of FF-MIP (34.7 mg g −1 ), whereas the adsorption capacity of NIP was only 17.3 mg g −1 . The adsorption equilibrium of three materials was reached within 50 min. Particularly, CD@FF-MIP exhibited an excellent fluorescence quenching response to FF in the concentration range of 3–50 µmol L −1 . As a result, CD@FF-MIP was successfully utilized to extract FF in milk samples, which were analyzed by high-performance liquid chromatography. The standard recoveries were 95.8%–98.2%, and the relative standard deviation was 1.6%–4.2%. The method showed the advantages of simple operation, high sensitivity, excellent selectivity, and low cost, and also demonstrated a great application prospect in food detection.
研究领域:
食品安全
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
He Jiang,Haoliang Wei,Xinkai Li,Yijun Zhang,Tingjiang Lu,Feili Li,Shuang Song,Yan Yu,Meilan Pan,Weiting Yu
The widespread discharge of halogenated organic pollutants (HOPs) in wastewater brings significant risks to the environment and human health due to potent high toxicity, antibacterial activity, and strong biodegradation resistance. Adsorbed atomic hydrogen (H* ads )-mediated electrocatalytic hydrodehalogenation (EHDH) has been recognized as an efficient strategy for HOPs removal through selectively breaking carbon-halogen bonds. In this work atomic Pd uniformly anchored on molybdenum disulfide (denoted as Pd-MoS 2 ) was synthesized through a facile hydrothermal method and found with state-of-the-art specific activity in florfenicol (FLO) removal via the H* ads -mediated EHDH process. Pd-MoS 2 completely dehalogenated (∼100 %) FLO within 30 min at a rate constant of 0.15 min −1 , which was 6.0, 6.5 and 33.1 times the value of MoS 2 , Pd/C and carbon paper samples, respectively. Notably, the toxicity of the wastewater was reduced to 1/6 of its original value after the treatment. Moreover, Pd-MoS 2 presented superior catalytic stability in five successive cycles. Furthermore, Pd-MoS 2 was also robust in complex water environment with practical applicability for industrial wastewater treatment. A dual-active-center mechanism with enhanced H* ads production capacity and the improved H* ads utilization efficiency was contributed to the increased EHDH activity on Pd-MoS 2 .
研究领域:
环境科学
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材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）