SCIENCE OF THE TOTAL ENVIRONMENT
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2024
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IF 8.2
Qian Zhang,Xinyan Xu,Chenzhuo Song,Dengke Zhang,Yi Kong,Xinyi Cui
Tire wear particles (TWP), as an emerging type of microplastics, are a significant source of contaminants in roadside soils due to their high concentration of pollutants, including polycyclic aromatic hydrocarbons (PAHs). This study explored the impact of ultraviolet (UV) exposure and natural aging on the in vitro bioaccessibility of PAHs associated with TWP in soil on a China-wide scale. Our findings suggested that UV exposure amplified the negative charge of TWP by 75 % and increased the hydrophobic groups on the particle surface. The bioaccessibility of 3- and 4-ring PAHs in TWP was significantly ( p < 0.05) heightened by UV exposure. After 20 types of soils containing 2 % UV-exposed TWP underwent natural aging, the bioaccessibility of PAHs saw a significant decrease ( p < 0.05) to 16–48 %, compared to 28–96 % in the unaged group. Soil pH and electrical conductivity (EC) were the two primary soil properties positively influencing the reduction of in vitro PAHs concentration and PAHs bioaccessibility. According to the prediction results, soils in southern China presented the highest potential region for the release of bioaccessible PAHs from TWP, highlighting the regional specificity of environmental impact. Our study provides valuable insights into the biological impact of PAHs associated with TWP on a regional scale, and offers scientific evidence for targeted soil risk management strategies.
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JOURNAL OF CHROMATOGRAPHY A
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2024
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IF 3.8
Yibo Yan,Ruilin Yang,Yanan Wang,Yinan Wu,Xiaofei Gu,Xiaoqiang Qiao
Styrene-maleic acid (SMA) copolymer has received much attention for its excellent solubilization characteristics. In this work, SMA copolymer brush-based chromatographic stationary phases were exploited and developed for the first time. First, SMA copolymer brush was in situ grown on the surface of spherical silica via living/controlled reversible addition-fragmentation chain transfer (RAFT) polymerization method. Subsequently, as a proof-of-concept demonstration, the copolymer was esterified by diethylene glycol mono-2-ethylhexyl ether (DGME) and 2-(2-ethylhexyloxy) ethanol (EHOE), respectively. The obtained Sil-SMA-DGME and Sil-SMA-EHOE copolymer-brush chromatographic stationary phases were characterized by transmission electron microscopy, Fourier transform infrared spectrometer, X-ray photoelectron spectroscopy, and thermogravimetric analysis, respectively. The chromatographic retention mechanism indicated that both the two packed columns exhibited hydrophilic/reverse mixed-mode retention modes. The maximum column efficiency was up to 71,000 N/m. The chromatographic separation performance evaluation indicated that the novel kind of stationary phases had excellent separation capabilities for hydrophilic, hydrophobic compounds and phospholipid standards. In addition, by combination with mass spectrometry identification, the Sil-SMA-DGME column was further exploited for separation and identification of phospholipids in human lung cancer cells. Totally, 9 classes including 186 phospholipid species were successfully identified. The results demonstrated the promising application prospects of the novel kind of SMA copolymer-brush chromatographic stationary phases.
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Chemosensors
·
2024
·Vol. 12
·期 10
·220
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IF 3.7
Ting Hu,Yitao Xia,You Wang,Li Lin,Rong An,Ling Xu,Xiangdong Qing
Polycyclic aromatic hydrocarbons (PAHs) are a group of organic compounds that are both toxic and hazardous to human health and ecological systems. In recent work, a novel analytical strategy based on the chemometric-assisted HPLC-DAD method was proposed for the quantification and source apportionment of eight PAHs in PM10 samples. Compared to traditional chromatographic methods, this approach does not require the purification of complex PM10 samples. Instead, it utilizes a mathematical separation method to extract analytes’ profiles from overlapping chromatographic peaks, enabling precise quantification of PAHs in PM10. Firstly, 40 PM10 samples collected in Loudi city during two sampling periods were used for analysis. Subsequently, the second-order calibration method based on alternating trilinear decomposition (ATLD) was employed to handle the three-way HPLC-DAD data. Finally, the pollution sources of PAHs were analyzed by the feature component analysis method according to the obtained relative concentration matrix. For the validation model, the average recoveries of eight PAHs were between (88.8 ± 7.6)% and (105.6 ± 7.5)%, and the root-mean-square errors of prediction ranged from 0.03 μg mL−1to 0.47 μg mL−1. The obtained limits of quantification for eight PAHs were in the range of 0.0050 μg mL−1to 0.079 μg mL−1. For actual PM10 samples, results of the feature component analysis indicated that the main source of PAHs in PM10 may be traffic emissions and coal combustion. In summary, the proposed method provided a new and rapid analysis method for the accurate determination and source apportionment of PAHs in atmospheric aerosols.
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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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CARBON
·
2024
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IF 10.5
Aiying Song,Rong Liu,Xinghe He
A novel strategy for fabricating deeply reduced three-dimensional inter-porous graphene oxide (drtdipGO)-coated solid-phase microextraction (SPME) fibers was developed. The reduced graphene oxide (rGO) coating was initially immobilized onto a stainless steel wire (SSW) through natural contraction from water loss during the drying process. This was achieved via deoxygenation of graphite oxide using ascorbic acid in an aqueous medium. To enhance the hydrophobicity, surface area, and adhesion strength between the coating and SSW, the rGO coating was calcined and further deoxidized in an H 2 /Ar atmosphere at 1100 °C. The as-fabricated fiber exhibited a homogeneous and wrinkled surface, high Brunauer-Emmett-Teller (BET) surface area (520 m 2 g −1 ), increased hydrophobicity, and unique three-dimensional inter-porous structure. The drtdipGO-coated fibers were employed for sensitive headspace solid-phase microextraction (HS-SPME) of petroleum hydrocarbons (PHCs) in water samples. Enrichment factors ranging from 1.2 to 32.1 were achieved for PHCs. The extraction efficiency per unit volume of the drtdipGO coating for all 31 PHCs was higher than that of five commercial SPME fiber coatings (1.5–1275.0-fold improvement). The proposed method exhibited a linear range of 5–500 μg L −1 (R ≥ 0.990), with limits of detection and quantification ranging from 0.71 to 14.4 μg L −1 and 2.4–48.0 μg L −1 , respectively. Recoveries (C10–C26) of 83%–108 % were obtained for water samples sourced from river, sewage, lake, and artificial water samples.
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JOURNAL OF CHROMATOGRAPHY A
·
2025
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IF 4
Zhihao Li,Dihong Zhong,Haipeng Lin,Peiyin Li,Yongyi Li,Qingmei Huang,Lingzhi Yang,Xueji Zhang
Solid-phase microextraction (SPME) is essential for analyzing ultra-low concentration samples, such as trace drugs and environmental pollutants. Among various formats, pipette tip-based SPME (PT-SPME) stands out for its advantages in efficiency, automation, and flexibility. However, PT-SPME faces challenges such as material loss, high synthesis costs, and environmental impact. To address these issues, we developed a novel PT-SPME device by synthesizing Schiff-base covalent organic frameworks (COFs) in situ on diatomaceous earth (DE), which served as both a matrix and support. This approach significantly improved stability and reduced COFs consumption by 93.7 %. The DE@COFs were packed into pipette tips with a sandwich-like structure and used to extract polycyclic aromatic hydrocarbons (PAHs), with detection achieved through high-performance liquid chromatography coupled with fluorescence detection (HPLC-FLD). The method exhibited excellent sensitivity, with limits of detection (LODs) ranging from 2.05 to 52.5 pg/mL and limits of quantification (LOQs) from 15.0 to 159 pg/mL. It also demonstrated high accuracy, with recoveries between 87.05 % and 115.86 %, and strong repeatability, making it suitable for trace pollutant analysis in complex matrices This cost-effective and environmentally friendly PT-SPME system enhances extraction efficiency while reducing material usage, providing a practical and innovative solution for trace pollutant analysis in pharmaceutical and environmental applications.
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JOURNAL OF CHROMATOGRAPHY A
·
2024
·
IF 3.8
Xiaomin Li,Mingxia Sun,Yang Feng,Yanming Liu,Yanli Wang,Juanjuan Feng,Min Sun
A covalent organic framework (COF) was gown on porous silica with 1,3,5-tri(4-aminophenyl)benzene and 2,5-divinyl-1,4-phenyldiformaldehyde as monomers, and two ionic liquids were grafted to COF by a click reaction. The materials before and after the modification of ionic liquids were separately packed into solid-phase extraction columns (10 × 4.6 mm, i.d.), which were coupled with liquid chromatography to construct online analysis systems. The extraction mechanisms of polycyclic aromatic hydrocarbons, bisphenols, diphenylalkanes and benzoic acids were investigated on these materials. There were π-π, hydrogen-bond and electrostatic interactions on ionic liquid-functionalized sorbents. After the comparison among these materials, the best sorbent was used, and the analytical method was established and successfully applied to the detection of some estrogens from actual samples. For the analytical method, the detection limit was as low as 0.005 μg L −1 , linear range was as wide as 0.017–10.0 μg L −1 , and enrichment ratio was as high as 3635. The recoveries in actual samples were 70 %-129 %.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xiao Wang,Bingcheng Lin,Jian Wang,Yunfeng Ma,Rong Jin,Guorui Liu,Minghui Zheng
Four inhibitors (CaO, CaS, CH 4 N 2 S, and (NH 4 ) 2 SO 4 ) were employed to inhibit the formation of multiple unintentional persistent organic pollutants (POPs) and environmentally persistent free radicals (EPFRs) using anthracene as a precursor, with CuCl 2 serving as both a transition metal catalyst and chlorine source. The inhibition mechanisms were elucidated in terms of chlorine immobilization, catalyst deactivation, and free radical regulation. The inhibition efficiency of the four inhibitors on polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), polychlorinated biphenyls (PCBs), and polychlorinated naphthalenes (PCNs) ranged from 64.7 % to 98.4 %, with the corresponding inhibition rates on toxic equivalency quantity ranging from 86.3 % to 99.7 %. The distribution of homologs shifted towards less chlorinated species, indicating effective suppression of chlorination. Calcium- and nitrogen-containing compounds consumed chlorine sources by forming CaCl 2 , CaClOH, and NH 4 Cl, while sulfur-containing compounds deactivated catalysts by forming CuSO 4 . EPFRs derived from anthracene were identified as carbon-centered anthracene-type and anthraquinone-type radicals. Positive correlations were observed between POPs and EPFRs concentrations, suggesting the pivotal role of organic free radicals as intermediates in POPs formation. Anthraquinones derived from anthracene underwent decomposition, recombination and chlorination, leading to the formation of PCDD/Fs and PCBs. The addition of inhibitors reduced EPFRs concentrations by 74.2–95.1 %. Sulfur- and nitrogen-containing inhibitors generated radicals that attacked POPs precursors and intermediates, forming heteroatomic compounds and inhibiting POPs formation. These findings enhanced the understanding of the source control mechanisms of POPs and provided theoretical and technical support for the synergistic inhibition of POPs and EPFRs in industrial thermal processes.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Dongni Liu,Peng Cui,Fangfang Zhang,Hao Ren,Lilin Fang,Xiaosi Sun,Haiyan Ji,Wenshuai Zhu,Zhichang Liu
Ionic liquid is an ideal candidate in the extraction of aromatic compounds. The design and construction of ionic liquids with high extraction efficiency and selectivity towards to the specific aromatics remain crucial question. In this paper, with the aid of orthogonal array experiment, the imidazolium-based ionic liquids with long alkyl chain on the cations were determined to possess high aromatics extraction efficiency. Furthermore, the Lewis acid anion was introduced into the ionic liquid to form 1-dodecyl-3-methylimidazolium ferric chloride ([C 12 mim][FeCl 4 ]) and performed 62 % and 100 % extractant efficiency of naphthalene (NAP) and anthracene (ANT), respectively. Then the porous carbon materials (P1-1000) derived from hyper-crosslinked porous polymers (HCP) which possessed high BET surface area (1186 m 2 /g) was dispersed in [C 12 mim][FeCl 4 ] to form porous ionic liquid. The single extraction efficiency of NAP improved from 62 % to 77 %. The great single extraction efficiency was attributed to the high porosity, additional adsorption sites provided by the Lewis acid anions and the hydrophobic long alkyl chain on the cations. After three times extraction, the concentration of NAP dropped down to 0. The porous ionic liquids also showed good recycle performance. The construction of porous ionic liquids provided an efficient approach for extraction of polycyclic aromatic hydrocarbons from aliphatic hydrocarbon.
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Water
·
2024
·Vol. 16
·期 17
·2537
·
IF 3
Bo Li,Hulong Liu,Xiaona Liu,Li Han,Jing Yang,Lingke Kang,Liuyuan Tang,Tianwei Qian
Bioremediation is a promising technique owing to its effectiveness, low cost, and environmental friendliness. Previous studies have focused on the degradation efficiency of polycyclic aromatic hydrocarbons (PAHs) in soil and water. However, the expression of PAH-catabolic genes in organisms involved in the degradation process has been rarely and unsystematically reported. In this study, a PAH-degrading strain—Pseudomonas aeruginosa(PQ249631)—was successfully isolated from coking-contaminated soil and used for PAH degradation in soil and water. Furthermore, the degradation of PAHs (naphthalene, fluorene, phenanthrene, anthracene, and pyrene) was investigated in single, binary, and mixture systems to explore the interaction of substrates. The results showed that when naphthalene was used as a cometabolite carbon source, the removal rates of fluorene, phenanthrene, anthracene, and pyrene increased from 14.33%, 17.25%, 6.61%, and 4.47% to 72.08%, 100.00%, 15.63%, and 6.63%, respectively. In a PAH mixture, the degradation rate of each PAH was higher when naphthalene, rather than glucose, was used as the cometabolite carbon source. Transcriptome analysis revealed significant differential expression of PAH-catabolic genes and ATP-binding cassette transporter-related genes under naphthalene stress. The enhanced degradation of PAHs could be attributed to the augmentation of the PAH metabolic pathway and membrane transportation, facilitating the transfer of PAHs to bacteria. These findings underscore the effectiveness ofP. aeruginosaas a PAH degrader and provide molecular insights into enhancing PAH degradation.
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ACS Sensors
·
2025
·
IF 9.1
Xing Wang,Shen Shen,Ning Sun,Yong Zhu,Jie Zhang
To enhance the sensitivity, integration, and practicality of the Raman detection system, a deep learning-based dual-functional subregional microfluidic integrated hydrogel surface-enhanced Raman scattering (SERS) platform is proposed in this paper. First, silver nanoparticles (Ag NPs) with a homogeneous morphology were synthesized using a one-step reduction method. Second, these Ag NPs were embedded in N-isopropylacrylamide/poly(vinyl alcohol) (Ag NPs-NIPAM/PVA) hydrogels. Finally, a dual-functional SERS platform featuring four channels, each equipped with a switch and a detection region, was developed in conjunction with microfluidics. This platform effectively allows the flow of the test material to be directed to a specific detection region by sequential activation of the hydrogel switches with an external heating element. It then utilizes the corresponding heating element in the detection region to adjust the gaps between Ag NPs, enabling the measurement of the Raman enhancement performance in the designated SERS detection area. The dual-functional microfluidic-integrated hydrogel SERS platform enables subregional sampling and simultaneous detection of multiple molecules. The platform demonstrated excellent detection performance for Rhodamine 6G (R6G), achieving a detection limit as low as 10–10 mol/L and an enhancement factor of 107, with relative standard deviations of the main characteristic peaks below 10%. Additionally, the platform is capable of simultaneous subarea detection of four real molecules─thiram, pyrene, anthracene, and dibutyl phthalate─combined with fully connected neural network technology, which offers improved predictability, practicality, and applicability for their classification and identification.
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JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Wanting Guo,Christian Marcus Pedersen,Zhihui Liu,Wenbo Dong,Lingyu Jia,Shuwei Chen,Yingxiong Wang,Yan Qiao
Carbazole (CAR) and anthracene (AN) are high value compounds derived from coal tar, but their separation is challenging due to their structural similarity. Promising results, using deep eutectic solvents (DESs) for the separation, have recently been obtained. However, choosing the optimal DESs for the separation of CAR and AN is difficult due to a lack of knowledge about the interaction of DESs with CAR and AN. Herein, the interactions between CAR and AN with seven DESs containing ethylene glycol (EG) as the hydrogen bond donor (HBD) were investigated by nuclear magnetic resonance (NMR). The interaction between CAR and tetrabutylammonium chloride/ ethylene glycol (TBAC/EG) was investigated using various NMR methods such as chemical shift titration, variable temperature NMR (VT-NMR), relaxation time measurements and diffusion-ordered spectroscopy (DOSY). From the chemical shift differences of the N H proton of CAR, a strong interaction between CAR and the DES consisting of TBAC and EG, was revealed. TBAC/EG was therefore proposed as a promising solvent for the separation of CAR and AN. In addition, VT-NMR showed that the hydrogen bonding interaction between CAR and TBAC/EG increased with decreasing temperature. The changes in relaxation time (T 1 , T 2 ), molecular correlation time (τ c ) and the molecular self-diffusion coefficients (D) supported the existence of interactions between CAR and TBAC/EG, presumably dominated by hydrogen bonding between the N H and the chloride ion. This study introduces an efficient method for screening solvents to separating CAR and AN, and it can also be applied to other fields of separating complex mixtures.
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