JOURNAL OF MOLECULAR STRUCTURE
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2023
·
IF 3.8
Xin Yan,Na Zhang,Zhiliang Liu,Chunfang Du
In this paper, 1T/2H mixed-phase MoS 2 /g-C 3 N 4 composites (1T/2H-MG) were successfully synthesized by a simple two-step calcination method and used for Cr(VI) removal from aqueous environment. A series of characterization methods were used to characterize the microstructure and surface morphology of the prepared materials. The experiment results showed that 1T/2H-MG (1:12) composite with good pH and temperature adaptability could completely remove Cr(VI) (100 mg∙L –1 ) within 50 min and showed an excellent adsorption capacity of 342.06 mg∙g –1 . The presence of abundant sulfur defects in 1T/2H-MG composite could provide more adsorption and reduction active sites, which was the main reason for the enhanced removal efficiency of 1T/2H-MG in comparison with pure MoS 2 and g-C 3 N 4 . This work not only contributes an excellent adsorbent for the wastewater treatment, but also provides evidences for the defects engineering.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Nguyen Quang Tung,Do Thi Cam Van,Dam Xuan Thang,Nguyen Thi Kim An,Tran Thi Trang,Bui Dinh Nhi,Nguyen Phuong Thao,Le The Son,Nguyen Nhat Huy,Nguyen Trung Dung
In this study, the CuCoFe-LDH catalyst was synthesized by hydrothermal method and applied to degrade levofloxacin (LFX) by peroxymonosulfate (PMS) activation. The physicochemical properties of the synthesized samples were analyzed by X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), Brunauer-Emmett-Teller (BET), X-ray photoelectron spectroscopy (XPS), and thermogravimetric analysis (TGA). The influence of various factors such as catalyst system, pH, catalyst content, PMS , pH, and coexisting ions on the degradation of LFX was systematically investigated. The results showed that after 10 min, 94.57 % of LFX was decomposed under the conditions of 200 mg/L of catalyst, 500 mg/L of PMS, 10 mg/L of LFX, and pH 7.0. Besides, the CuCoFe-LDH/PMS system can effectively remove LFX over a wide pH range from 3.5 to 9.0. Both radical superoxide (O 2 •- ) and non-radical singlet oxygen ( 1 O 2 ) were major reactive oxygen species in the CuCoFe-LDH/PMS system. Mass spectrometry identified 16 major degradation products of LFX, and 38.43 % of LFX was mineralized after 30 min of reaction. Besides, the CuCoFe-LDH/PMS system had the ability to effectively degrade different groups of antibiotics (e.g., fluoroquinolone, tetracycline , and sulfonamide). The mechanism of PMS activation by CuCoFe-LDH and the LFX degradation pathway were proposed. Finally, testing the reusability of CuCoFe-LDH in LFX degradation showed that a decrease of nearly 7 % occurred after five consecutive cycles, suggesting its stability for practical applications.
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JOURNAL OF MOLECULAR STRUCTURE
·
2023
·
IF 3.8
Qi He,Dandan Wang,Jing Shao,Yi Li,Ming Cheng,Lihui Dong,Yunhui Li,Jianwei Zhu,Hongji Li
A novel imprinting membrane (Ag/CuO/CNTs/Eggshell membrane -Molecularly Imprinted polymeric Membrances, ACCE-MIMs) based on surface enhanced Raman scattering (SERS) is successfully synthesized for the specific detection of spiramycin (SP). Firstly, CNTs and CuO are successively loaded on eggshell membrane (ESM) to increase the uniformity and sensitivity by virtue of the unique reticular structure of CNTs and excellent chemical enhancement of CuO. Through the abundant amino and carboxyl groups on ESM, Ag nanoparticles (Ag NPs) are anchored and growth on the surface of membrane by two in-situ reduction process and form a three-dimensional (3D) architecture. Eventually, the ACCE-MIMs are synthetized by silicon-based sol-gel method. With the help of imprinted polymers, the ACCE-MIMs present anti-interference performance during selective detection. The sensor presents a great liner relationship (R 2 = 0.9965) between SP concentration and the Raman peak intensity when the concentration of SP ranges between 1 × 10 −6 M ∼1 × 10 −12 M. The limit of detection concentration is 1 × 10 −12 M and the enhancement factor (EF) is 0.2956 × 10 7 . The ACCE-MIMs exhibits sensitive detection property and this procedure provides a promising future for detection process.
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TALANTA
·
2023
·
IF 6.1
Chang Liu,Hong Lin,Limin Cao,Kaiqiang Wang,Jianxin Sui
The third generation of genetic engineering antibodies, single-domain antibodies, have been widely reported as potential biomaterials in recognizing small molecular hazards. In this study, a shark-derived single-domain antibody was used as the recognition element for the first time to detect enrofloxacin (ENR), one of the most representative hazards in aquaculture. An ENR-specific clone named 2E6 was isolated by phage display technology. Experimental results proved that 2E6 ssdAb showed high affinity to ENR-PEI complete antigen, with the highest OD 450 value of 1.348 in binding ELISA . Through icELISA, it was determined that the IC 50 of 2E6 ssdAb to ENR was 19.230 ng/mL, while the IC 10 was 0.975 ng/mL, with rare recognition to other fluoroquinolones, which showed high sensitivity and specificity to ENR. The 2E6 ssdAb also performed excellently in fish matrix immunoassay . Results showed that the ENR-negative fish matrix did not seriously interfere with the recognition of 2E6 ssdAb to ENR-OVA, with the matrix index between 4.85% and 11.75%, while the results of icELISA in ENR-spiked fish matrix showed that 2E6 ssdAb could recognize the target ENR in different ENR-spiked concentrations of the fish matrix (10–1000 ng/mL), with the recovery between 89.30% and 126.38% and the RSD between 1.95% and 9.83%. This study broadens the application scenario of shark-derived single-domain antibodies as small molecule recognition biomaterials, providing a new recognition element on ENR detection for immunoassay.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Junyang Pan,Dan Hua,Yiping Hong,Xi Cheng,Fangsong Guo,Kok Bing Tan,Ziqi Zhong,Guowu Zhan
Photocatalytic membranes with concurrent catalytic oxidation and separating functions possess promising potentials for the degradation of organic pollutants in wastewater treatment. Herein, we designed a hybrid photocatalytic membrane ( viz. , g-C 3 N 4 /GO/MCE) by vacuum-filtration-assisted assembling method, consisting of graphitic carbon nitride (g-C 3 N 4 ) nanosheets as a top layer, graphene oxide (GO) nanosheets as an interlayer, and commercial mixed cellulose ester (MCE) as a substrate layer. The microstructures, chemical compositions, and physicochemical properties of the designed g-C 3 N 4 /GO/MCE membranes were systematically characterized by a series of characterization techniques. Particularly, photocatalysis-filtration reactor cells were designed for the evaluation of the simultaneous separation and photocatalytic degradation performance in a single unit using both organic dyes and antibiotics as modeling pollutants in wastewater. Four parameters were adopted to represent the integrated photocatalysis-filtration performance of our designed photocatalytic membranes, including permeance ( P ), rejection ( R’ , filtration alone), removal ( R , combined photocatalysis-filtration under light-irradiation), and degradation rate ( D ). The hybrid membranes showed superior permeance and solute removal under visible-light irradiation (300 W, λ > 420 nm), in which the permeance was 20% higher than that of no-irradiation conditions. In addition, 10 consecutive cycling tests and light-on/off cycles of the as-prepared g-C 3 N 4 /GO/MCE membrane toward RhB showed quite stable permeance in the range of 268.9 to 352.9 L h −1 m −2 bar −1 , and the removal was maintained in the range of 88.4% to 95.4%, indicating excellent long-term stability. Remarkably, it also exhibited good removal performance of antibiotics ( e.g. , ofloxacin, norfloxacin, sulfamethoxazole, erythromycin, and roxithromycin). Accordingly, the designed hybrid g-C 3 N 4 /GO/MCE photocatalytic membranes with excellent photocatalytic activity and photocatalysis-filtration performance are promising for wastewater treatment and water purification applications.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Baokang Xu,Xiao Zhang,Yue Zhang,Shiwen Wang,Peng Yu,Yongjun Sun,Xi Li,Yanhua Xu
The nonradical pathway selectively oxidizes pollutants with less interference from environmental factors, which can effectively improve the environmental suitability of peroxymonosulfate (PMS) activation. Herein, a Co-doped nanotubular carbon nitride catalyst (Co-CNNT) based on CoN x sites was constructed for stable and efficient PMS activation with a better specific surface area, number of CoN x sites, and electron transfer capability than Co-doped lamellar carbon nitride catalyst (Co-CN). Co-CNNT improved PMS utilization efficiency (∼50%) and enhanced the contribution of the electron transfer pathway to tetracycline (TET) degradation. The enhanced ability of Co-CNNT to adsorb PMS leads to Co-CNNT–PMS* generated by PMS at the CoN x site, which raises the Co-CNNT surface potential and allows PMS to be activated in a manner that captured electrons. Thus, the Co-CNNT/PMS system could effectively destroy electron-rich or low-potential pollutants within 24 min. The stronger environmental adaptability allows it to maintain catalytic activity in complex aqueous matrices, achieving effective oxidation of diluted tetracycline-based pharmaceutical wastewater. This paper reveals the effects of carbon nitride morphology control strategies on the properties of CoN x active sites and PMS activation mechanisms, providing new insights into the induction of nonradical PMS activation pathways.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
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2023
·
IF 4.3
Zhendong Yu,Bolong Liang,Zhe Zhao,Shumin Lin,Hongbin He,Shu-Xuan Liang
In this study, magnetic polystyrene polymers (Fe 3 O 4 @PLS) with both hydrophilic and hydrophobic groups were synthesized for magnetic solid-phase extraction. Experimental parameters, including solution pH, adsorption time, elution solvent, elution volume and elution time, were optimized. A magnetic solid-phase extraction method using Fe 3 O 4 @PLS as adsorbent for three fluoroquinolones (FQs), including enrofloxacin , ofloxacin and ciprofloxacin , in milk substrates was established with high-performance liquid chromatography. Under the optimized experimental conditions, the limits of detection of the three FQs were 0.41–0.45 µg/kg and the limits of quantitation of the three FQs were 1.37–1.51 μg/kg. The recoveries of three FQs in milk samples were 96.5–118.6%. The method was successfully applied to the detection of three FQs in 20 kinds of milk. The results showed that the proposed method had the advantages of easy operation, rapid and efficient enrichment and separation of analytes, which proved its reliability and applicability. The adsorption property of Fe 3 O 4 @PLS was significantly improved compared with ProElut polystyrene polymers (PLS), which provided a new idea for the development of magnetic polymer materials and expanded the application of magnetic polymers in the pretreatment of complex samples.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Ding Liu,Zhenkun Su,Bo Han,Kaisheng Xia,Chenggang Zhou,Qiang Gao
Cobalt–aluminum oxide clusters-embedded γ-Al 2 O 3 nanosheets (CAO@AO) were facilely fabricated and developed for peroxymonosulfate (PMS) activation. Interestingly, the Al–OH-rich amphiphilic surface of CAO@AO endowed the catalyst with unique interfacial pH-buffering property, which stabilized the reaction media at nearly neural level and thus prevented the cobalt sites from leaching. Moreover, the presence of Al–OH groups around the Co−Al oxide clusters facilitated the activation of PMS and the redox cycle of Co 2+ /Co 3+ , which resulted in a boosted catalytic activity. Consequently, the CAO@AO exhibited zero leaching of cobalt and high efficacy for PMS activation, enabling complete and ultrafast removal of metronidazole with a significantly higher turnover frequency (TOF, 1.83 min −1 ) than that of Co 3 O 4 (0.004 min −1 ). It was also demonstrated that introducing suitable foreign metal into CAO@AO could further enhance the catalytic activity (e.g., TOF of Mn(40%)-CAO@AO: 5.80 min −1 ). Furthermore, Mn(40%)-CAO@AO-decorated granular support was synthesized that dominated a continuous-flow degradation in column reaction system.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Peng Xu,Xiang Li,Rui Wei,Chunyan Yang,Tianyao Shen,Peng Wang,Guangshan Zhang
The adaptability and stability of catalysts guarantee efficient catalytic performance. Hence, we fabricated FeCo 2 O 4 /diatomite for efficient peroxymonosulfate (PMS) activation. Distinct from stacked FeCo 2 O 4 , FeCo 2 O 4 /diatomite possessed a 1.2-fold larger specific surface area (94.84 m 2 g −1 ), achieving 100% ATZ removal within 10 min at 0.2 g L −1 PMS and 0.1 g L −1 FeCo 2 O 4 /diatomite. The system could adapt to a broad pH range (3–11) and complex water matrices, efficiently removing multiple contaminants. High removal performance (>92%) and mineralization (>57%) were maintained after six cycles with minimal leached Co (0.10 mg L −1 ). The conversion between ≡Fe(III)/≡Fe(II) and ≡Co(III)/≡Co(II) could trigger PMS persistently, producing abundant active species, in which SO 4 •− was dominant. Then, intermediates and degradation pathways were proposed based on DFT calculations and ESI-QTOF-MS/MS data. Toxicity analysis showed that most intermediates were more eco-friendly than ATZ. This study developed FeCo 2 O 4 /diatomite with superior catalytic performance, high adaptability, and stability for eliminating refractory organic pollutants.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Roujia Du,Qianxin Zhang,Frank Leresche,Mengmeng Zhong,Ping Chen,Jun Huang,Shubo Deng,Fernando L. Rosario-Ortiz,Gang Yu
To determine and predict the reaction rate between 3 DOM* and PPCPs in various water bodies, this study defines a reaction rate coefficient ( α 3 DOM ∗ ) to describe the reaction between 3 DOM* and PPCPs. As the values also included the inhibition effect of DOM's antioxidant moieties, the calculation of α 3 DOM ∗ is inconsistent with that of a bimolecular rate constant via the steady-state kinetic method. The α 3 DOM ∗ values of 12 selected PPCPs were determined in two DOM solutions and ten DOM-containing water samples collected from typical surface water bodies in Beijing. The Pearson coefficients between nine predictors including the absorbance ratio (E2/E3), specific absorption coefficient at 254 nm (SUVA 254 ), fluorescence index (FI), biological index (BIX), humification index (HIX), pH, total organic carbon (TOC), total fluorescence intensity (TFI) and TOC normalized TFI (TFI/TOC) and α 3 DOM ∗ were examined. Correlation patterns for sulfonamides, β-blockers and diclofenac supported the electron transfer pathway, and was distinctly different from those appeared for FQs where quenching effect played a main part. TFI and TFI/TOC were recognized as the most useful surrogates in empirically predicting α 3 DOM ∗ . For PPCPs that went through the electron transfer pathway, α 3 DOM ∗ could be well fit to the Rehm-Weller model assuming a proportional relationship between TFI and △G et . For FQs, α 3 DOM ∗ was found to linearly correlated with TFI/TOC. The α 3 DOM ∗ values determined in this study enrich the database of PPCPs photolysis parameters, and the correlation analysis provides reference for forecasting PPCPs fate in the aquatic environment.
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Analytical Methods
·
2018
·Vol. 11
·期 4
·507-516
·
IF 2.073
Chang Liu,Diandian Deng,Di Xu,Kang Wu,Hong Yang,Kang Zhao,Jianguo Li,Anping Deng
In this study, a monoclonal antibody (mAb)-based enzyme-linked immunosorbent assay (ELISA) for the determination of chloramphenicol (CAP) in shrimp, feed and milk samples was developed and validated by LC-MS/MS coupled with immunoaffinity clean-up (LC-MS/MS-IAC). Three immunogens were synthesized and used to immunize mice. Spleen cells from the immunized mice with the highest titer were selected for cell fusion. Two lines of hybridoma cells (1B1 and 2D2) secreting specific antibodies against CAP were successfully screened. Under optimal conditions, the values of the 50% inhibitory concentration (IC50) and limit of detection (LOD) of the ELISA in phosphate-buffered saline (PBS) based on 2D2 mAb for the detection of CAP were 0.46 ng mL−1 and 0.06 ng mL−1, respectively. There was no cross-reactivity (CR) of the ELISA with other antibiotics (florfenicol, thiamphenicol, etc.). Shrimp, feed and milk samples were spiked with different contents of CAP and detected by ELISA. The recoveries and coefficients of variation (CVs) of the ELISA for CAP from three spiked samples were 80.6–116.0% and 5.5–15.4% (n = 3), 96.2–111.0% and 7.0–13.5% (n = 3), and 79.7–109.8% and 5.8–13.3% (n = 3), respectively. As the CAP concentrations in spiked samples measured by LC-MS/MS coupled with solid phase extraction (LC-MS/MS-SPE) were significantly lower than those measured by ELISA, we established an immunoaffinity clean-up (IAC) for CAP by covalently immobilizing our mAb against CAP on the CNBr-activated Sepharose-4B gel and directly mixing the mAb-immobilized gel with the spiked samples sufficiently. The recoveries of CAP from the spiked samples measured by LC-MS/MS-IAC were 78.6–106.7% with the CV less than 11.1% (n = 3).
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CHEMOSPHERE
·
2018
·
IF 4.427
Xue Xue Liang,A.M. Omer,Zhao-hong Hu,Yang–guang Wang,Di Yu,Xiao-kun Ouyang
In this study, we prepared a magnetic composite based on amine-functionalized chitosan (aminochitosan; AmCS) and Fe 3 O 4 to remove diclofenac sodium (DS) from water. The fabricated AmCS@Fe 3 O 4 composite was characterized using Fourier-transform infrared spectroscopy, transmission electron microscopy , scanning electron microscopy, vibrating sample magnetometry, X-ray diffraction, and thermogravimetric analysis . Furthermore, we investigated the influence of pH, initial DS concentration, and adsorbent dosage on the adsorption of DS. Through thermodynamic analysis, we found that the data corresponded with the Langmuir adsorption isotherm model. The maximum adsorption capacity reached 469.48 mg g −1 , and the adsorption process followed the pseudo-second-order kinetic model. Finally, the AmCS@Fe 3 O 4 composite retained good adsorption characteristics after four consecutive cycles, with removal efficiency exceeding 70%. Therefore, the developed adsorbent could be used for efficient adsorptive removal of trace drugs and personal care products from water bodies.
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