CHEMICAL ENGINEERING JOURNAL
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2024
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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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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Yuqian Li,Haomin Chen,Wei Li,Beidou Xi,Caihong Huang
The remediation of sites co-contaminated with polycyclic aromatic hydrocarbons (PAHs) and heavy metals (HMs) poses challenges for efficient and ecofriendly restoration methods. In this study, three strains ( Pseudomonas sp. PDC-1, Rhodococcus sp. RDC-1, and Enterobacter sp. EDC-1) were isolated from sites contaminated with PAHs and HMs. The constructed bacteria consortium was then immobilized using biochar, bentonite, and peat. The immobilized bacteria consortium (IBC) demonstrated efficient removal ability of phenanthrene (58.1 %-73.4 %) and benzo[ a ]pyrene (69.6 %-83.5 %) during 60 days. Additionally, the IBC decreased soil bacterial richness and diversity, but increased the relative abundance of Proteobacteria phylum and Ochrobactrum genus, which were capable of degrading PAHs. Soil microbial co-occurrence network with IBC was classified into three main modules, and 14 genera were identified as keystone taxa linked to PAHs degradation and HMs resistance. The IBC enhanced the dioxygenase metabolic pathways for PAHs degradation, including phthalic acid and salicylic acid pathways, which became the main driving factor affecting PAHs removal efficiency based on the structural equation modeling analysis. This study confirmed the potential application of the constructed IBC in the bioremediation of soil co-contaminated with PAHs-HMs, and provides insights into key removal mechanism and main driving factor of the enhanced elimination of PAHs.
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TALANTA
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2014
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IF 3.511
Man Wang,Shihai Cui,Xiaodi Yang,Wentao Bi
An easy preparation of g-C 3 N 4 /Fe 3 O 4 nanocomposites by chemical co-precipitation has been demonstrated. The as-prepared materials were characterized by X-ray diffraction, transmission electron microscopy , Fourier transform infrared spectroscopy and thermogravimetric analysis . The high affinity of g-C 3 N 4 toward polycyclic aromatic hydrocarbons and the magnetic behavior of Fe 3 O 4 were combined to provide an efficient and simple magnetic solid phase extraction (MSPE). The adsorption and desorption of polycyclic aromatic hydrocarbons on g-C 3 N 4 /Fe 3 O 4 were examined. Different factors affecting the magnetic solid phase extraction of polycyclic aromatic hydrocarbons were assessed in terms of adsorption, desorption, and recovery. Under the optimized conditions, the proposed method showed good limits of detection (LOD, S/N=3) in the range of 0.05–0.1 ng mL −1 and precision in the range of 1.8–5.3% (RSDs, n =3). This method was also successfully applied to the analysis of real water samples; good spiked recoveries over the range of 80.0–99.8% were obtained.
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ENVIRONMENTAL POLLUTION
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2024
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IF 7.6
Shuai Zhang,Shuyuan Wang,Jiating Zhao,Lizhong Zhu
Thermal desorption (TD) remediation of polycyclic aromatic hydrocarbon (PAH)-contaminated sites is known for its high energy consumption and cost implications. The key to solving this issue lies in analyzing the PAHs desorption process, defining remediation endpoints, and developing prediction models to prevent excessive remediation. Establishing an accurate prediction model for remediation efficiency, which involves a systematic consideration of soil properties, TD parameters, and PAH characteristics, poses a significant challenge. This study employed a machine learning approach for predicting the remediation efficiency based on batch experiment results. The results revealed that the extreme gradient boosting (XGB) model yielded the most accurate predictions (R 2 = 0.9832). The importance of features in the prediction process was quantified. A model optimization scheme was proposed, which involved integrating features based on their relevance, importance, and partial dependence. This integration not only reduced the number of input features but also enhanced prediction accuracy (R 2 = 0.9867) without eliminating any features. The optimized XGB model was validated using soils from sites, demonstrating a prediction error of less than 30%. The optimized XGB model aids in identifying the most optimal conditions for thermal desorption to maximize the remediation efficiency of PAH-contaminated sites under relative cost and energy-saving conditions.
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ANALYTICA CHIMICA ACTA
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2024
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IF 5.7
Yiwen Han,Aikun Han,Yaqiong Qin,Yuan Tian,Bin Peng,Lijun He,Wenfen Zhang,Wenjie Zhao,Shusheng Zhang
Background Edible oils are susceptible to contamination with polycyclic aromatic hydrocarbons (PAHs) throughout production, storage, and transportation processes due to their lipophilic nature. The necessity of quantifying PAHs present in complex oil matrices at trace levels, which bind strongly to impurities in oil matrices, poses a major challenge to the accurate quantification of these contaminants. Therefore, the development of straightforward and effective methods for the separation and enrichment of PAHs in oil samples prior to instrumental analysis is paramount to guaranteeing food safety. Results A pyrazine embedded hyper-crosslinked porous polymer, HCP Pz-TPB , was synthesized via a Friedel-Crafts reaction, utilizing triphenylbenzene (TPB) as the monomer and 2,5-dibromomethylpyrazine as the cross-linking reagent. The material was combined with polydimethylsiloxane (PDMS) using the sol-gel method, and applied as a coating to a dumbbell-shaped stir bar prepared in-house. Using stir bar sorptive extraction (SBSE) combined with gas chromatography-mass spectrometry (GC-MS), 15 PAHs in edible oils were successfully quantified. Optimal conditions for the extraction of PAHs were experimentally investigated, with factors such as stirring rate, extraction time, extraction temperature, desorption solvent, and desorption time systematically optimized. The final method demonstrated a broad linear range (0.12–150 ng g −1 ), and low limits of detection (0.04–0.28 ng g −1 ). The recoveries of PAHs in real edible oil samples ranged from 83.14 % to 128.01 %, with relative standard deviations (RSDs) below 13.47 %. Significance This method simplifies PAH extraction by eliminating steps such as saponification, liquid-liquid extraction, drying, and re-dissolution, thus reducing potential analyte loss and errors associated with the inclusion of multiple pretreatment steps typical of conventional methods reported in the literature. Notably, the adsorbent materials prepared in this study can be reused up to 30 times, underscoring its sustainability. The proposed research broadens the diversity of coating choices for SBSE applications while offering a streamlined, cost-effective, and greener alternative for PAH determinations in edible oils via SBSE/GC-MS.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Sitao Wang,Xiaolan Zhang,Qingqing Zhou,Zhimin Liu,Zhigang Xu
Polycyclic aromatic hydrocarbons (PAHs) have long been globally distributed, and almost worldwide people are exposed to varying degrees of PAHs. Aqueous medium is an important transmission route of PAHs, but the detection of PAHs in aqueous environment has been a challenge. Herein, a magnetic hypercrosslinked polymer microsphere (Fe 3 O 4 @SiO 2 -PS@HCP) was developed for the effective detection of PAHs. Under the effect of multiple factors (hydrophilicity, intermolecular force and molecular volume), Fe 3 O 4 @SiO 2 -PS@HCP shows excellent performance on the enrichment of five PAHs in aqueous environment. Fe 3 O 4 @SiO 2 -PS@HCP was used to capture PAHs in city river of plateau lake. In-depth data analysis showed that factory activities and traffic emissions are the main pollution sources of PAHs. Ecological, carcinogenic and non-carcinogenic risks are almost within the safe range. The carcinogenic and non-carcinogenic risks of PAHs in children are higher than adults, which needs to be taken seriously. This method breaks the dilemma that it is difficult to enrich weakly hydrophilic pollutants in aqueous media, and complements important pathways for tracing sources of pollutants and assessing associated risks. It brings methodological enlightenment into the development of environmental pollution and human health risk assessment methodology.
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APPLIED CLAY SCIENCE
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2024
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IF 5.3
Yun Li,Xuechi Liu,Meng Han,Zhouhua Wang,Ruixin Shi,Haoqi Liao,Bao Yuan,Pengfei Wang,Songbai Han,Jinlong Zhu
To understand the occurrence of natural gas hydrates in seabed sediments, it is crucial to examine the mechanisms of methane (CH 4 ) hydrate formation in sodium montmorillonite (Na-Mt) systems in the presence of amino acid. Accordingly, this study employed kinetics experiments and molecular dynamics simulations to investigate CH 4 hydrate nucleation and growth in an Na-Mt system containing alanine (Ala), leucine (Leu), and phenylalanine (Phe), respectively. Kinetics and Raman experiments showed that, compared with Ala, Leu and Phe enhanced hydrogen bonding between water molecules surrounding Na-Mt. This enhancement was due to the long carbon chain of Leu and the phenyl ring of Phe and facilitated CH 4 hydrate formation. Moreover, in the Na-Mt system, Ala reduced CH 4 consumption, whereas Leu and Phe increased CH 4 consumption. Molecular dynamics simulations revealed that the strength of electrostatic interactions between the negatively charged Na-Mt surface and the functional groups of amino acids affected the distribution of amino acids, thereby altering CH 4 aggregation and CH 4 hydrate nucleation processes. The strong interaction between Na-Mt and Ala significantly disrupted interfacial interactions between Na-Mt and water molecules. In contrast, the weaker interactions between Na-Mt and Leu and Phe, respectively, meant that these amino acids affected CH 4 hydrate nucleation in the bulk-like solution by influencing the arrangement of water molecules. These findings indicate that interfacial interactions between Na-Mt and amino acids play a crucial role in CH 4 hydrate formation. Overall, this study generated insights into the formation kinetics and nucleation properties of CH 4 hydrates in clay mineral–amino acid complexes that may increase understanding about the occurrence of natural gas hydrates in marine sediments.
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JOURNAL OF CHROMATOGRAPHY A
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2025
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IF 4
Zichen Zhao,Ruiyang Ma,Juntao Wang,Qing Zhang,Miao Jing,Chun Wang,Qiuhua Wu,Zhi Wang
A boric acid functionalized hyper-crosslinked polymer (HCP), designated as NPCBA/TBM-HCP, was successfully synthesized via Friedel-Crafts reaction by copolymerizing N-phenylcarbazole-2-boronic acid (NPCBA) and 2,4,6-Tris(bromomethyl)mesitylene (TBM). The NPCBA/TBM-HCP showed a large surface area and a good adsorption property for phenylurea herbicides (PUHs). A method with NPCBA/TBM-HCP based solid phase extraction and high-performance liquid chromatographic detection was developed for the simultaneous analysis of PUHs in lake water, green tea drink and tomato samples. Under the optimized experimental conditions that the amount of the NPCBA/TBM-HCP was 30 mg, sample solution was 100 mL, sample loading rate was 4 mL min -1 , and eluent was 0.3 mL acetonitrile, the linear response for the PUHs was in the range of 0.06–80.0 ng mL -1 , 0.6–80.0 ng mL -1 and 0.9–200 ng g -1 for lake water, green tea drink and tomato samples, respectively, with a good linearity (the coefficients of determination ( r 2 ) ≥ 0.9916). The detection limits (S/N = 3) for lake water, green tea drink and tomato samples were 0.02–0.03 ng mL -1 , 0.2 ng mL -1 and 0.3–0.5 ng g -1 , respectively. The method recoveries for spiked samples were 80.0 %-119.1 % and RSDs were lower than 9.9 % for the determination. The method provides a new and feasible approach for the determination of phenylurea herbicide in real samples.
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Journal of Analysis and Testing
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2025
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IF 7
Li Han,Cui Yuanyuan,Zhen Changqing,Lin Xiaohui,Li Ke,Yang Chengxiong
Microporous organic network (MON) has emerged as efficient stationary phases for high-performance liquid chromatographic (HPLC) separation. Nevertheless, the inherent superhydrophobic networks made their applications limited in the reversed-phase (RP) mode. In this work, a novel amino acid L-cysteine (L-Cys) modified core-shelled microsphere MON@SiO 2 -L-Cys was synthesized via the efficient thiol-yne “click” reaction for hydrophilic interaction chromatography /reversed-phase liquid chromatography (HILIC/RPLC) mixed-mode chromatographic separation. Baseline separation of various hydrophilic and hydrophobic compounds including aromatic ketones, phthalate esters, alkylbenzenes, amines, polycyclic aromatic hydrocarbons, phenols, nucleosides, nucleic acid bases, sulfonamides, water-soluble vitamins, cephalosporin antibiotics, and estrogens was realized on MON@SiO 2 -L-Cys packed column based on the predesigned mixed-mode retention mechanisms. The MON@SiO 2 -L-Cys packed column also exhibited higher selectivity compared to bare SiO 2 , MON@SiO 2 without L-Cys, and C 18 packed columns, revealing the synergistic interactions of MON’s networks and the modified L-Cys molecules. This work provided a feasible way to construct a novel amphipathic MON-based stationary phase, broadened the application scope of MON for hydrophilic analytes, and uncovered the prospects of MON in mixed-mode HPLC.
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LANGMUIR
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2024
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IF 3.7
Chunyang Liu,Yanrong Cheng,Delan Ge,Ju Xie,Xia Guo
Aqueous two-phase systems (ATPS) are considered a new type of green separation system, but their low selectivity to target molecules limits their practical application. In this study, we used surfactant@MWCNT as an adjuvant to improve the selectivity of PEG/(NH4)2SO4 ATPS. The surfactants used include Triton X-100 (TX-100), Tween 80, sodium dodecyl sulfate (SDS), sodium dodecyl benzenesulfonate (SDBS), and bis(2-ethylhexyl)sulfosuccinate sodium salt (AOT). Nine aromatic compounds, including syringic acid, vanillin, tryptophan, phenylalanine, tyrosine, mandelic acid, theophylline, theobromine, and cephalexin, were selected as model extracts. The results showed that the use of the surfactant@MWCNT composite as an adjuvant significantly improved the selectivity of the ATPS toward syringic acid among the nine extracts. Moreover, the selectivity of the ATPS for syringic acid with the TX-100/MWCNT composite as the adjuvant is better than that with the Tween 80/MWCNT composite as the adjuvant, followed by that with the anionic surfactant/MWCNT composite as the adjuvant. The enhanced selectivity of ATPS by the surfactant/MWCNT composite is ascribed to the spatial effect and the electrostatic and hydrophobic interactions between the extract and the surfactant adsorbed on the MWCNT.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Guangyu Dong,Liushan Jiang,Linchun Nie,Jiawei Liao,Xiaodie Geng,Wenjing Liu,Dejing Meng,Meiling Xu,Na Liu,Qingxiang Zhou,Chunmao Chen
In this study, a magnetic covalent organic framework composite (Fe 3 O 4 @COF-BTCA-TMB) was conceived and synthesized with benzene-1,3,5-tricarbaldehyde and 3,3’,5,5’-tetramethyl benzidine as monomers. The modification of COF endowed the magnetic composite with a large number of functional groups and benzene rings, which exhibited high affinity to polycyclic aromatic hydrocarbons (PAHs) attributed to π-π conjugation and hydrophobic interaction. Based on these properties, it was utilized to conceive a highly efficient magnetic solid phase extraction method to enrich PAHs from water samples prior to high performance liquid chromatography analysis. The key factors that affect the extraction efficiencies of six PAHs in water samples were explored. Under the optimized conditions, six PAHs obtained good linearity in wide concentration ranges of 0.2–80 μg L −1 , 0.2–180 μg L −1 , and 0.2–240 μg L −1 , respectively. The limits of detection (LODs) ranged from 0.03 to 0.09 μg L −1 , and the enrichment factors were in the range of 107–149. The adsorption of PAHs on Fe 3 O 4 @COF was consistent with the quasi-second-order kinetic model, and Freundlich adsorption isotherm model. The conceived method was evaluated with real water samples and satisfactory recoveries (73.8 % ∼ 100.5 %) were obtained, indicating that it was simple, robust and efficient, and could be optioned for monitoring trace PAHs in environment.
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JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Lei Tian,Mengni Pan,Cuiping Ye,Hongbo Hao,Wenying Li
Phenanthrene (Phe) and fluorene (Flu) are crucial chemical intermediates with applications in materials, medicine, and pesticides. However, conventional separation methods struggle to effectively isolate phenanthrene from fluorene due to their similar physical properties. To address this challenge, a reaction–separation coupling technique was employed to convert fluorene into 9-fluorenone (9-Fluo), followed by the separation of phenanthrene from 9-fluorenone using solvent-cooling crystallization. Initially, the relative solubilities of phenanthrene and 9-fluorenone in 2072 solvents were calculated using COSMO-RS for preliminary screening. Among various conventional short-chain aliphatic alcohols and low-carbon saturated hydrocarbons, methanol, and cyclohexane were identified as the most effective solvents based on their solubility selectivity (SS). The molecular interactions between phenanthrene or 9-fluorenone and these solvents were analyzed using theoretical methods such as σ-potential/profile, infinite dilution activity coefficients in COSMO-RS, and Hansen solubility parameters, with further confirmation from FTIR tests. The optimal liquid–solid ratios were determined using both phase diagram measurements and solubility calculations. The reaction conversion of fluorene to 9-fluorenone was complete regardless of the raw material used. Phenanthrene and 9-fluorenone were effectively separated using methanol and cyclohexane with optimum liquid–solid mass ratios of 1.6:1 and 2.8:1, respectively. In the model mixture, the contents of phenanthrene and 9-fluorenone exceeded 98 wt%, with yields above 91 wt%. For anthracene residue, the content of 9-fluorenone reached 93.98 wt% with a yield of 84.52 wt%, while its content was only 76.58 wt% due to the accumulation of other components in phenanthrene.
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危险品化学品经营许可证（带存储）