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JOURNAL OF MOLECULAR STRUCTURE · 2022 · IF 3.841

Two Keggin-type polyoxometalates used as adsorbents with high efficiency and selectivity toward antibiotics and heavy metals

Hao Zhang,Min Li,Zhiliang Liu,Xiangchao Zhang,Chunfang Du

Two Keggin-type polyoxometalates ammonium phosphomolybdate (NH 4 -PMo) and ammonium phosphotungstate (NH 4 -PW) were simply synthesized and used as adsorbents for removing various antibiotics and heavy metals from water system. The effects of adsorbent dosage, initial concentration of pollutants, temperature and pH value on the adsorption efficiencies of tetracycline (TC) and Ni 2+ over both NH 4 -PMo and NH 4 -PW were systematically investigated. The adsorption process of TC molecules can be described by the Langmuir isothermal adsorption model. In terms of kinetic model, the adsorption process of TC can be described by the pseudo first-order kinetics for NH 4 -PMo and pseudo second-order kinetic model for NH 4 -PW. The results of adsorption experiments pointed out that the adsorption efficiency of NH 4 -PMo was higher than that of NH 4 -PW toward various antibiotics, dyes and heavy metals. The more negative surface charges and higher specific surface area contributed to the superior adsorption efficiency of NH 4 -PMo.

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DESALINATION · 2022 · IF 11.211

Antibiotics separation from saline wastewater by nanofiltration membrane based on tannic acid-ferric ions coordination complexes

Long-Fei Ren,Siqi Zhang,Zhongbao Ma,Yangbo Qiu,Diwen Ying,Jinping Jia,Jiahui Shao,Yiliang He

Excessive discharge of saline antibiotics wastewater into aquatic ecosystem is one crucial environmental issue facing the world today. Herein, an eco-friendly nanofiltration (NF) membrane was fabricated based on coordination complexes of tannic acid and ferric ions (TA-Fe) to selectively separate antibiotic and monovalent salt. Optimal membrane with Fe/TA molar ratio of 3/1 and coordination time of 60 s exhibited Zeta potential of −26.0 mV (pH = 7), water contact angle of 45.5 o and pore radius of 0.36 nm. Consequently, TA-Fe@M3-T60 membrane showed high ciprofloxacin/NaCl rejection ratio of ~5.9 and considerable water permeability of 20.6 ± 1.2 LMH. Besides, relatively high rejection rates were obtained for ofloxacin (94.1 ± 2.2 %) and ciprofloxacin (91.9 ± 2.5 %), while rejection rate for trimethoprim was much lower (68.2 ± 4.1 %). Effects of static/dynamic membrane adsorption of antibiotics on subsequent removal performance were investigated for the first time. Rejection rate improvements of 7.4–15.2 % were observed on pristine membrane compared with pre-adsorbed membrane in short-term NF process. Electrostatic shielding experiment and rejection rate prediction further distinguished the contributions of steric hindrance , electrostatic interaction and membrane adsorption on antibiotics removal, especially antibiotics in zwitterionic form at pH = 7. The findings of this work imply that this newly developed NF membrane has great potential for efficient treatment of antibiotics-contaminated wastewater.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Enhanced photo-Fenton degradation of fluoroquinolones in water assisted by a 3D composite sponge complexed with a S-scheme MoS2/Bi2S3/BiVO4 ternary photocatalyst

Boqiang Gao,Yu Pan,Hu Yang

A constructed MoS 2 /Bi 2 S 3 /BiVO 4 ternary photocatalyst(MBB) mainly with a S-scheme heterostructure was loaded on a 3D lignosulfonate modified poly(vinyl formal) sponge to obtain a novel composite sponge(PLS-MBB) with an enhanced performance in synergistic adsorption and photo-Fenton degradation of various fluoroquinolones(FQs) in water. The synergistic adsorption and photocatalysis of PLS-MBB notably improved the applicable pH from 2.0 to 9.0 and reduced the dosage of Fe 2+ to 0.014 mmol/L in Fenton reaction , which could achieve the degradation efficiency of 92.8 % for FQs within 60.0 min at pH 6.0. The photo-generated electrons by MBB and the redox transformation of Mo(IV)/Mo(VI) and Bi(III)/Bi(V) accelerated the conversion of Fe 3+ to Fe 2+ ; besides, the efficient adsorption of FQs on the sponge carrier promoted the surface degradation in solution, thereby causing an enhanced photo-Fenton reaction. This work provided a novel strategy to improve photo-Fenton reaction and accordingly fabricated a talented material for effective removal of organic contaminants in water.

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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Fabrication of 3D lignosulfonate composited sponges impregnated by BiVO4/polyaniline/Ag ternary photocatalyst for synergistic adsorption-photodegradation of fluoroquinolones in water

Boqiang Gao,Koukou Tao,Zhonghua Xi,Mayyada M.H. El-Sayed,Tamer Shoeib,Hu Yang

In this work, a 3D lignosulfonate composited poly(vinyl formal) (PVF) sponge impregnated by BiVO 4 /polyaniline (PANI)/Ag ternary photocatalyst (PLS-BiVO 4 /PANI/Ag) was designed and fabricated. The synergistic adsorption-photodegradation of five fluoroquinolones (FQs) antibiotics onto PLS-BiVO 4 /PANI/Ag was investigated. Incorporating lignosulfonate as a carrier on PVF sponge improved its structural properties and enhanced its adsorption performance toward FQs. The BiVO 4 /PANI/Ag ternary photocatalyst was well-dispersed and tightly bound to the composited sponge, thus it efficiently degraded the adsorbed FQs through surface photodegradation. PLS-BiVO 4 /PANI/Ag achieved >90% removal efficiency for all examined FQs within 2.0 h in a batch system, while it maintained a steady 80% removal efficiency for 30.0 h in a continuous dynamic treatment system. Photoelectric characterizations and ESR results showed that BiVO 4 /PANI/Ag was consistent with the type II heterostructure and effectively improved the utilization of visible light and the separation of photogenerated electron-hole pairs. The hole was the dominant active species in the degradation of FQs, while the main degradation pathways included defluorination, decarboxylation and destruction of piperazine ring. The prepared composited sponge is thus characterized by its high performance, convenient operation, eco-friendliness, and practicality in real water treatment systems since it undergoes self-purification and is easily recovered from water without mass loss.

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ANALYTICA CHIMICA ACTA · 2022 · IF 6.911

Copper doped zinc sulfide quantum dots as ratiometric fluorescent probes for rapid and specific detection of tetracycline residues in milk

Jian Zhang,Zhijun Bao,Jingjing Qian,Haibo Zhou,Kui Zhang

In this work, copper-doped zinc sulfide quantum dots (ZnS:Cu QDs) were developed as ratiometric fluorescent probes to detect tetracycline (TC) in milk. With the increasing of TC concentration, the fluorescence at 578 nm of ZnS:Cu QDs was quenched, while a new fluorescence at 520 nm was significantly enhanced due to the formation of a green-emitting complex of Zn 2+ and TC on the surface of probes. The fluorescence intensity ratio (I 520 /I 578 ) have a good linear relationship (R 2  = 0.98) with the concentration of TC in the range of 0.2–2.0 μM. The detection limit was calculated to 149 nM, which is lower than the allowable level of TC (about 180 μM) in milk set by the US Food and Drug Administration (FDA). Finally, the fluorescent test papers have been also prepared using ZnS:Cu QDs as ink by painting on a piece of filter paper. With the addition of TC, the orange test paper produced green spots that became more and more obvious with a dose-discerning ability as low as 2 μM. This work demonstrated a great potential of ratiometric fluorescent probe for the easy and visual detection of TC in complicated real samples.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Separation Science Plus · 2022 ·Vol. 5 ·期 8 ·337-348 · IF 0

Hollow magnetic molecularly imprinted polymer based on metal-organic framework for capture of ciprofloxacin

Shu Zhou,Jinli Fu,Pengfei Zhao,Sisi Tang,Xiaodan Wu,Zhaoxia Yang,Zhaohui Zhang

The development of a simple and rapid separation and analysis method with high selectivity toward ciprofloxacin is of great importance for environmental protection. Herein, this paper reported a hollow magnetic zeolitic imidazolate framework-67 based molecularly imprinted polymer for selective adsorption and enrichment of ciprofloxacin. The morphology and structural properties of the hollow magnetic molecularly imprinted polymer were characterized by scanning electron microscopy, transmission electron microscopy, infrared spectroscopy, and thermogravimetry, and the results showed that the material has an obvious hollow structure, good thermal stability, and magnetic properties. The hollow magnetic imprinted polymer has a higher adsorption capacity (75.59 mg/g) and shorter adsorption saturation time (50 min) toward ciprofloxacin. Moreover, the hollow magnetic molecularly imprinted polymer showed excellent adsorption ability, stability, and repeatability. The hollow magnetic imprinted polymer was used to detect trace ciprofloxacin in actual samples (river water, human urine, chicken) successfully with the recoveries of 91.4–100.4%. With the advantages of high recovery (91.4–100.4%), high speed (50 min), and high selectivity (selectivity factor > 2.50), the hollow magnetic molecularly imprinted polymer has broad application prospects in the efficient adsorption of ciprofloxacin.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Introduction of cluster-to-metal charge transfer in UiO-66-NH2 for enhancing photocatalytic degradation of bisphenol a in the existence of peroxymonosulfate

Shi-Wen Lv,Xiaoran Wang,Xing Wei,Yi Zhang,Yanqing Cong,Lin Che

Nowadays photocatalysis assisted advanced oxidation processes exhibited a great application prospects in pollution control. Herein, for the first time, a series of transition metal modified UiO-66-NH 2 (namely Fe-UiO-66-NH 2 , Co-UiO-66-NH 2 and Ni-UiO-66-NH 2 ) were synthesized via a simple method. After that, these functional materials were employed as photocatalyst to activate PMS for degrading BPA under visible light irradiation. Significantly, prepared Fe-UiO-66-NH 2 exhibited the highest photocatalytic activity among these samples. More importantly, proposed Fe-UiO-66-NH 2 /PMS/light oxidation system showed excellent degradation ability for various organic pollutants, including BPA, TC, OFX, IBP as well as SMX. Owing to the occurrence of d-d transitions after the coordination of transition metal ions, UiO-66-NH 2 displayed the enhanced utilization efficiency of visible light. Furthermore, introduced Fe ion as a mediator could boost the charge transfer by the cluster-to-metal way, thereby effectively inhibiting the recombination of photogenerated electrons and holes. In addition, embedding cluster-to-metal charge transfer in UiO-66-NH 2 modified the band structure, and both SO 4 −• and OH were major active species in the photocatalytic reaction system. Developed Fe-UiO-66-NH 2 /PMS/light oxidation system with good stability also presented great antibacterial performance. To sum up, current work could provide some novel inspirations for designing the high-efficiency photocatalyst.

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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2022 · IF 5.518

Facile hydrothermal synthesis of co-glycerate as an efficient peroxymonosulfate activator for rhodamine B degradation

Qin Yang,Yujie Zhang,Jie Liang,Yongsong Luo,Qian Liu,Yingchun Yang,Xuping Sun

Sulfate radical based advanced oxidation processes (SR-AOPs) are regarded as a promising technology to degrade organic pollutants in water. Here, hydrothermally synthesized Co-glycerate (Co-G) microspheres are proposed as an efficient heterogeneous catalyst to activate peroxymonosulfate (PMS) for degradation of refractory organic pollutant rhodamine B (RhB) in aqueous solution. The presence of Co-G microspheres enhanced the degradation rate significantly with a short full degradation time (8 min) and a total organic carbon (TOC) removal exceeding 41% (10 min), thus implying the excellent catalytic performance of Co-G microspheres for PMS activation. Furthermore, the effects of PMS and catalyst concentration, initial pH value and co-existing ions on RhB degradation were investigated. Radical quenching and EPR tests identify that active species including SO 4 - ·, HO·, O 2 - · and 1 O 2 are involved in the degradation process. Additionally, a possible reaction mechanism of PMS activation by Co-G microspheres for RhB degradation was suggested. This study can provide a new insight for design of cobalt-based heterogeneous catalysts as activators to activation PMS for pollutants degradation.

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MICROCHIMICA ACTA · 2022 ·Vol. 189 ·期 5 ·1-7 · IF 6.408

Self-enhancement photoelectrochemical strategy for kanamycin determination with amino functionalized MOFs

Wang Yang,Jin Daobin,Zhang Xiaoqian,Zhao Jikuan,Hun Xu

Based on the self-enhanced photoelectrochemical quality of Cu-MOF-NH 2 , a photoelectrochemical biosensor for kanamycin detection with a Cu-MOF-NH 2 modified electrode was constructed. This biosensor took full advantage of the low electron hole recombination rate due to the ligand-to-metal charge-transfer mechanism of excited electron transfer in Cu-MOF-NH 2 . The kanamycin aptamer was modified onto Cu-MOF-NH 2 by Schiff base reaction. In the presence of kanamycin, the holes on the amino group in Cu-MOF-NH 2 oxidize kanamycin, making kanamycin itself as a signal enhancement substance, and achieving the effect of self-enhancement. The dynamic monitoring range for kanamycin is 0.5 to 650 nM, and the detection limit is 0.1 nM. The sensor has been successfully applied to the determination of kanamycin in fish with recoveries of 95.7–105.0% and RSD of 1.5–4.0%. This work provides a broad path for the development of self-enhanced photoelectrochemical sensors. Graphical abstract

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APPLIED CLAY SCIENCE · 2022 · IF 5.907

Halloysite nanotubes supported copper oxide composites used as efficient catalysts for bisphenol A removal

Wenyu Zhang,Xin Yan,ZhiliangLiu,Chunfang Du

Copper oxide/ halloysite nanotubes (CuO/HNTs) served as excellent catalysts for bisphenol A (BPA) removal were prepared through a hydrothermal method . The influences of catalyst dosage, peroxymonosulfate (PMS) concentration, pH value, initial BPA concentration, temperature, inorganic anions, and humic acid on the degradation efficiency were investigated. The degradation results indicated that the catalyst 70% CuO/HNTs (70% represented the weight ratio of CuO to HNTs) displayed an extraordinary TOC removal efficiency of 96%, which was 1.2 times higher than that of CuO. The mechanism studies suggested that the abundant hydroxyl groups of HNTs mostly contributed to the superior degradation efficiency of CuO/HNTs. The singlet oxygen ( 1 O 2 ) produced in the CuO/HNTs/PMS system acted as the predominant active specie in the degradation process . Moreover, the formed Cu-O-Al bond constrained the growth of CuO and improved the cycle performance of CuO/HNTs. This work provides an efficient catalyst for contaminant removal and contributes an innovative strategy for constructing functional mineral composites with abundant hydroxyl groups.

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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

A green strategy from waste red mud to Fe0-based biochar for sulfadiazine treatment by peroxydisulfate activation

Dongmei Ma,Jing Wang,Kun Feng,Bingfeng Liu,Guojun Xie,Defeng Xing

Zerovalent iron (Fe 0 )-based biochar (Fe 0 -BC) has attracted wide attention in activating persulfate to eliminate antibiotics. In this study, the waste red mud (RM) was successfully used as an iron precursor to prepare Fe 0 -BC (RMIS 1:1 ) via co-pyrolysis strategy, which was confirmed with remarkable capacity in peroxydisulfate (PDS) activation. The removal efficiency of sulfadiazine (SDZ) was 99.7% in RMIS 1:1 /PDS system in 20 min, with k obs of 0.3001 min −1 . Both free radicals (SO 4 − , OH, and O 2 − ) and non-free radicals ( 1 O 2 ) were responsible for SDZ degradation, in which the SO 4 − and O 2 − played the dominant roles. Four SDZ degradation pathways were provided according to the intermediates identified by Q-TOF-MS. Furthermore, the ECOSAR prediction implied that the intermediates have less eco-toxicity than SDZ. Compared with PDS concentration and RMIS 1:1 dosage, the initial SDZ concentration had stronger effect on its degradation. Co-existed Cl − slightly improved SDZ degradation rate, while other anions (NO 3 – /SO 4 2− /HCO 3 – /CO 3 2– ) and humic acid exhibited different levels of inhibition on SDZ removal. Moreover, RMIS 1:1 /PDS maintained acceptable degradation ability for practical pharmaceutical wastewater. The electrical energy per mass of SDZ was about 2.24 kWh/(g·SDZ) by RMIS 1:1 /PDS, lower than that produced in any other advanced oxidation processes that have been reported so far. In summary, this study reported a green strategy for Fe 0 -BC preparation from RM, which was valuable for both waste resource recycling and environmental remediation.

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Chinese Journal of Chromatography · 2022 ·Vol. 40 ·期 5 ·433-442 · IF 0

[Fast screening and confirmation of 73 common prohibited compounds in cosmetics by ultra performance liquid chromatography-quadrupole-time-of-flight high resolution mass spectrometry].

Yangjie LI,Jiaying HUANG,Jihui FANG,Zhiye HUANG

A high throughput screening method based on ultra performance liquid chromatography-quadrupole-time-of-flight high resolution mass spectrometry (UPLC-Q-TOF HRMS) was developed for the simultaneous and rapid confirmation of 73 prohibited compounds in cosmetics. The sample was dispersed in a saturated sodium chloride solution and ultrasonically extracted using acetonitrile containing 0.2% (v/v) formic acid. The resultant solution was centrifuged and then cleaned using dispersive solid phase extraction using a primary secondary amine (PSA) sorbent. The purified solution was centrifuged, and the supernatant was filtered through a 0.22 μm membrane before determination. The optimal pretreatment method was determined by comparing the recovery rates obtained using different extraction solvents and different amounts of purifying agents. The chromatographic separation conditions and mass spectrometry scanning mode were also optimized. Chromatographic separation was performed on an Acquity UPLC HSS T3 column (100 mm×2.1 mm, 1.8 μm) with gradient elution using 0.1% (v/v) formic acid aqueous solution and methanol as mobile phases. The eluent from the column was further detected using Q-TOF HRMS with the high resolution multiple reaction monitoring (MRM HR) scanning mode. Retention time, precise mass of parent ion, isotope abundance ratio, and precise mass of fragment ions were the parameters considered for rapid untargeted screening and confirmation. The matrix effects of water- and cream-based cosmetics were investigated. The matrix effects could be addressed using the matrix matched standard curve method. The correlation coefficients for the 73 prohibited compounds were all >0.99 in the corresponding linear concentration range. The limits of detection (LODs) were in the range of 5-150 μg/kg, and the limits of quantification (LOQs) were in the range of 15-450 μg/kg. Average recoveries were in the range of 60.3%-130.3% at three spiked levels, and the intra-day and inter-day precisions were 0.8%-10.0% ( n =6) and 1.1%-15.0% ( n =3), respectively. A total of 692 cosmetics samples were screened; 16 positive samples were detected, namely, sulfamethoxazole, meprednisone, lincomycin, 4-acetamidophenol, trimethoprim, alfacalcidol, betamethasone 17-valerate, brimonidine, chloramphenicol, chlorpheniramine, clobetasol propionate, crotamiton, econazole, ketoconazole, prednisone 21-acetate, and prednisone, with content in the range of 0.5-1136.1 mg/kg. The optimized method is accurate, fast, and simple, and it is suitable for the routine detection and rapid screening of common prohibited compounds in cosmetics. In addition, a screening and confirmation library was established for the 650 prohibited compounds using SCIEX OS and Library View software, using information-dependent acquisition (IDA)-MS/MS mode for MS data acquisition. The database contains multiple types of information, including formulas, theoretical exact mass, retention time, precise mass of parent ion, isotope abundance ratio, and fragment ion distribution. The library can be used for the simultaneous and rapid confirmation of prohibited compounds in cosmetics.

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