CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Shuhui Huo,Xiaohui Deng,Nan Yang,Mengya Qin,Xiaonan Zhang,Xiaoqiang Yao,Cuixiang An,Pengxin Zhou,Xiaoquan Lu
In this study, a durable hydrophobicity hydrazone covalent organic framework (BTCH-PTA-COF) has been developed as fiber coating, which was applied to solid-phase microextraction (SPME) of polycyclic aromatic hydrocarbons (PAHs). The hydrophobic and π-π packing interactions between BTCH-PTA-COF and PAHs were confirmed by contact angle experiments and Van der Waals surface electrostatic potential analysis. Further, large specific surface area, good chemical and thermal stability have positive promoting effect on extraction. The method of wide linearity (0.25–300 µ g·L −1 ), low detection limits (0.03–0.05 µ g·L −1 ) and high enrichment factors (767–1411) for the detection of PAHs is explored, coupling BTCH-PTA-COF based SPME with gas chromatography with hydrogen flame detector (GC-FID). The relative standard deviations (RSDs) for inter-day and intra-day extractions of PAHs are ranging from 4.1 % to 9.6 % and 2.9 % to 6.4 %, respectively. The method successfully detected and quantified trace PAHs in tea beverages and river water samples with recoveries from 88.5 % to 104.8 %. The BTCH-PTA-COF coated fiber is ultra-stable in recycled extraction and reused at least 120 times, which could surpass published and commercial SPME fiber.
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Reaction Chemistry & Engineering
·
2024
·
IF 3.4
Hui Jin,Mengyu Cui,Peiwen Liu,Zhuo Wang,Tongxia Jin,Yonghui Yang,Weiping Zhu,Xuhong Qian
Heterogeneous palladium catalysts are widely used in catalytic hydrogenation, oxidation, reduction, and coupling reactions due to their good stability, recyclability, and reusability. Based on the palladium ion fluorescent probe, a novel magnetically recyclable heterogeneous palladium catalyst Fe3O4@FSM@Pd was constructed and characterized, which is highly efficient and reusable for the Suzuki–Miyaura cross-coupling reaction. The subsequent series of Maitlis' filtration test, catalyst concentration–yield kinetic experiments, and phase trajectory experiments further demonstrated that Fe3O4@FSM@Pd catalyzed through a heterogeneous mechanism under selected reaction conditions. In addition, Fe3O4@FSM@Pd was applied to catalyze the synthesis of five intermediates of active pharmaceutical ingredients (APIs): valsartan, sonidegib, erdafitinib, tubulin inhibitor, and lumacaftor. Importantly, the palladium residue in the API intermediates synthesized with Fe3O4@FSM@Pd as catalyst was less than 1 ppm. Furthermore, Fe3O4@FSM@Pd is stable and can be reused at least 5 times without losing activity.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Xudong Zhang,Yang Deng,Yanhua Liu,Fan Yang,Yugao Wang,Jun Shen
Carbazole is a highly value-added compound derived from crude anthracene. Deep eutectic solvents (DESs) have been extensively used as promising green solvents for the separation of target compounds from mixture. In this work, 135 acidic DESs, formed by combining 9 quaternary ammonium salts with 15 common acids, were screened based on the conductor-like screening model for real solvents (COSMO-RS) model. The four top-ranked DESs, including tetraethylammonium chloride (TEAC)/2 acetic acid (AA), TEAC/2 propionic acid (PA), tetrapropylammonium chloride (TPAC)/2AA, and TPAC/2PA were identified as suitable extractants for carbazole separation based on their performance index (PI). Among them, TEAC/2AA had the best separation performance for carbazole due to its highest PI value (1448.19). Liquid–liquid extraction experiments were performed, and the results were in good accordance with those predicted by COSMO-RS calculations. Therefore, TEAC/2AA was determined as the most promising DES for the carbazole separation. The extraction conditions of TEAC/2AA were optimized. The extraction efficiency (EE) and selectivity (SE) of carbazole were 97.67 % and 66.64 %, respectively, under the optimal extraction conditions (25 ℃, 5 min of extraction time, DES-oil mass ratio of 1:5, initial carbazole concentration of 5000 ppm). Additionally, the deionized water was employed to regenerate the DES and recovery of carbazole. The recycling performance of promising DES was also investigated. Finally, quantum chemical calculations and Fourier Transform Infrared spectroscopy (FT-IR) analysis were conducted to explore the separation mechanism. The results indicated that the separation of carbazole by DESs were predominantly dominated by hydrogen bonds and van der Waals interaction. This work provided a valuable reference for the selection and design of DES extractants to separate other high value-added components from mixture.
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Catalysts
·
2024
·Vol. 14
·期 5
·311
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IF 3.8
Changzhao Chen,Zhe Yuan,Shenshen Sun,Jiacai Xie,Kunfeng Zhang,Yuanzheng Zhai,Rui Zuo,Erping Bi,Yufang Tao,Quanwei Song
Soil contamination by polycyclic aromatic hydrocarbons (PAHs) has been an environmental issue worldwide, which aggravates the ecological risks faced by animals, plants, and humans. In this work, the composites of nanoscale zero-valent iron supported on carbonylated activated carbon (nZVI-CAC) were prepared and applied to activate persulfate (PS) for the degradation of PAHs in contaminated soil. The prepared nZVI-CAC catalyst was characterized by scanning electron microscopy (SEM), X-ray diffractometer (XRD), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). It was found that the PS/nZVI-CAC system was superior for phenanthrene (PHE) oxidation than other processes using different oxidants (PS/nZVI-CAC > PMS/nZVI-CAC > H2O2/nZVI-CAC) and it was also efficient for the degradation of other six PAHs with different structures and molar weights. Under optimal conditions, the lowest and highest degradation efficiencies for the selected PAHs were 60.8% and 90.7%, respectively. Active SO4−•and HO•were found to be generated on the surface of the catalysts, and SO4−•was dominant for PHE oxidation through quenching experiments. The results demonstrated that the heterogeneous process using activated PS with nZVI-CAC was effective for PAH degradation, which could provide a theoretical basis for the remediation of PAH-polluted soil.
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JOURNAL OF CHROMATOGRAPHY A
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2018
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IF 3.716
Xue Xiong,Meiling Qi
This work describes the separation performance of utilizing hexagonal boron nitride (h-BN) as the stationary phase for capillary gas chromatography (GC). The statically coated h-BN column showed moderate polarity and achieved column efficiencies of 3455 plates/m and 3800 plates/m for naphthalene and n -dodecane, respectively. With temperature-dependent structure properties, the h-BN stationary phase exhibited stronger retention for polycyclic aromatic hydrocarbons (PAHs) over phthalic acid esters (PAEs) and showed advantageous separation performance over the g-C 3 N 4 and commercial polysiloxane stationary phases. Moreover, it displayed preferential retention for halogenated analytes and high resolution performance for structural and positional isomers. In addition, the h-BN column showed good column repeatability with relative standard deviation (RSD) values of 0.03%–0.07% for run-to-run, 0.31%–0.71% for day-to-day and 2.6%–5.3% for column-to-column, respectively, and thermal stability up to 260 °C.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Wang Kai Tong,Chaomeng Dai,Jiajun Hu,Mei Ru Yue,Yun Dong Liu,Bu Li,Jia Jie Zou,Jia Wang,Han Tang,Min-tian Gao,Yucang Liang,Wenjuan Wang,Jixiang Li
Hydrophobic organic contaminants (HOCs) threaten human health and ecosystems. The most economical and low-carbon remediation method employs surfactants to mobilize HOCs, followed by separation using carbon-based materials. A carbon-structure superimposition strategy (CSSS) was developed to prepare interface selectivity-based colloidal biochar (CBC-AO). In a solution with a pollutant concentration of 2.5 mg/L phenanthrene, a 99 % removal efficiency was achieved, and a 100 % recovery rate was obtained for common anionic surfactants. Notably, CSSS offers a unique approach to using lignocellulose-based biomass (LB)-derived biochar as an alternative to activated carbon (AC). The uniqueness of CSSS lies in revealing the carbon structure transfer mechanism, where cellulase pretreatment converts LB into aromatic carbon substrates, followed by air oxidation and colloidal treatment to transform unfavorable carbon structures into those beneficial for selective adsorption. This modification grants biochar selectivity and stability, addressing the challenge of balancing different carbon structures and functions. CBC-AO achieved a 90 % reuse rate after six cycles. Compared with traditional biochar, its acute biological toxicity was reduced by 77 %, and its environmental friendliness was further increased. In terms of carbon emissions and cost, CBC-AO outperforms AC, reducing emissions by 0.62 tons of CO 2 per year, whereas AC increases emissions. CSSS overcomes traditional biomass selection limitations, broadening biomass options and providing efficient, economical, and carbon-negative alternatives to conventional carbon-based materials. Furthermore, integrating CSSS with biofuel production results in biochar performance comparable to commercial AC, potentially advancing both industries.
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ANALYTICA CHIMICA ACTA
·
2015
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IF 4.513
Juan Zheng,Kun Wang,Erlun Luo,Dingcai Wu,Fang Zhu,Ruifen Jiang,Chengyong Su,Chaohai Wei,Gangfeng Ouyang
The monodisperse microporous carbon nanospheres (MMCNSs) were applied in solid phase microextraction for the first time. The MMCNSs-fiber was prepared by sol–gel technique and good repeatability and reproducibility were obtained, due to the excellent monodispersity of the MMCNSs . The sol–gel-MMCNSs fiber exhibited superior extraction ability for polycyclic aromatic hydrocarbons (PAHs) and organochlorine pesticides (OCPs), compared with the commercial polydimethylsiloxane/divinylbenzene (PDMS/DVB) fiber and the fiber prepared with its precursor, the monodisperse microporous polystyrene nanospheres (MMPNSs). Moreover, the fiber has good thermostability and strong acid/base durability. The sol–gel-MMCNSs fiber was then employed to detect PAHs and OCPs in aqueous samples by combining with gas chromatography–mass spectrometer (GC–MS). Under the optimized conditions, the detection limits of the proposed method ranged from 0.10 to 5.5 ng L −1 . Furthermore, the method was successfully utilized for the analysis of PAHs and OCPs in real samples, with satisfactory recoveries in the range of 81.0–120% for the Pearl River water samples and 72.8–118% for the coking wastewater samples.
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JOURNAL OF CHROMATOGRAPHY A
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2015
·
IF 4.169
Shu-Wen Xue,Min-Qiong Tang,Li Xu,Zhi-guo Shi
Magnetic nanoparticles (MNPs) featured with divinylbenzene (DVB) and sulfonate functionalities (Fe 3 O 4 –DVB–SO 3 − ) were prepared via “thiol-ene” click chemistry. The hydrophobic DVB moieties were dedicated for extraction while the hydrophilic sulfonate groups were designed for dispersing the MNPs in aqueous sample solution. Thus, the specially designed material could ensure operational convenience and improve reproducibility during extraction. The application of the material was demonstrated by the extraction of polycyclic aromatic hydrocarbons (PAHs) from environmental water samples followed by gas chromatography–mass spectrometric analysis. The main factors influencing the extraction, including the type of the desorption solvent, the agitation mode, the amount of MNPs, extraction and desorption time and salt addition in sample solution, were investigated in detail. Under the optimized conditions, the proposed method showed satisfactory reproducibility with intra-day and inter-day relative standard deviations less than 16.5% and 21.2%, and low limits of detection of 1.1 pg mL −1 , 0.8 pg mL −1 , 1.1 pg mL −1 , 1.4 pg mL −1 , 0.6 pg mL −1 , 2.1 pg mL −1 and 0.7 pg mL −1 for naphthalene, acenaphthene, fluorine, phenanthrene, anthracene, fluoranthene and pyrene, respectively. The developed method was also successfully used for determination of the PAHs in genuine lake and river environmental water samples by standard addition method. All the studied PAHs were detected in these waters with comparable results by the standard liquid–liquid extraction method. The developed MNPs with dual property of hydrophobicity and hydrophilicity were suitable for the treatment of water samples. The magnetic solid phase extraction based on this material was reliable and convenient. It has great potential in the preconcentration of trace analytes in complex matrix.
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MARINE POLLUTION BULLETIN
·
2025
·
IF 4.9
Ruicong Gao,Jiaqi Lu,Zhixuan Wei,Hao Xu,Siyuan Jing,Minghuo Wu
PAHs, a group of persistent organic pollutants with significant carcinogenic and mutagenic effects, are widely distributed in the environment and can accumulate in sediments, posing potential threats to mangrove ecosystems and human health. This study is one of the most recent studies that presents an analysis of the vertical contamination characteristics of PAHs in mangrove sediments down to a depth of 80 cm, utilizing a combination of solid-phase extraction and gas chromatography–mass spectrometry. The results showed that the mean value of PAHs was 258.82 ng/g (range from 226.41 to 320.07 ng/g) in the studied mangrove areas (Beihai City, Guangxi). The results indicated a decline in PAH concentrations with increasing sediment depth, with values of 259.3 ng/g in surface sediments (0–10 cm), 240.9 ng/g in intermediate sediments (30–40 cm), and 241.1 ng/g in deeper sediments (60–70 cm). This suggests that PAHs not only remain in the surface layer of the sediment, as in previous studies, but also migrate vertically within the sediment. Based on the results, the potential ecological risks of PAHs were also evaluated by the ERL/ERM model. After environmental risk assessment, it was found that among the six PAHs studied, the contents of all except acenaphthene were lower than the ERL, indicating a low ecological risk. This study elucidates the vertical distribution of PAHs in mangrove sediments, offering crucial data for ecological risk assessment and establishing a foundation for future research on PAH transport mechanisms and their ecological impacts, thereby informing environmental management strategies.
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危险品化学品经营许可证（带存储）