JOURNAL OF CHROMATOGRAPHY A
·
2022
·
IF 4.601
Ruijuan Duan,Meiling Qi
This work presents the investigation of two new pentiptycene (PP)-functionalized triblock copolymers (PEPE1, PEPE2) for gas chromatographic (GC) analyses with an aim to address the separation problems toward analytes of high resemblance in properties and a wide variety of components in complex samples. Up to date, these two materials are not reported in any fields. The PEPE1 and PEPE2 columns showed close column efficiency (above 4000 plates/m) but differed in polarity, morphology and separation performance. As testified by the challenging Grob test mixture, the PEPE1 column exhibited comprehensively higher separation capability than the PEPE2 column and the commercial reference columns. Also, the PEPE1 column achieved high-resolution performance for both apolar and polar isomers of high resemblance, such as xylenes, phenols and anilines. Moreover, it displayed high inertness towards carboxylic acids and excellent separation repeatability and reproducibility tested by the aniline isomers with the RSD values in the range of 0.01–0.04% for run-to-run, 0.09–0.13% for day-to-day and 1.2–2.0% for column-to-column, respectively. Its application to GC–MS analysis of the essential oil from tea flowers demonstrated its advantageous separation performance towards a wide range of components and proved its feasibility for practical analyses of complex samples.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Yuanji Gao,Hongru Feng,Bing Xia,Lei He,Congling Yang,Lijuan Zhao,Yuanjiang Pan
Ultratrace organic pollutants in the environment pose severe threats to human health; hence, their accurate detection is essential. In this study, we develop a secondary solvent-free enrichment strategy based on bubbling extraction (BE). Especially, we used BE solid-phase microextraction and BE carbon nanotube paper absorption to capture aerosols from a liquid water surface, desorb analytes, and analyze the analytes using mass spectrometry. The application of a solvent-free enrichment strategy helps overcome technical challenges in implementing BE technology, including reproducibility, quantification, and sensitivity. This approach objectively demonstrates the enrichment efficiency of BE, resulting in improved mass spectrometry response and quantification. It effectively tackles the difficulties in detecting and quantifying ultratrace environmental pollutants in mass spectrometric analysis. The present study successfully conducted a quantitative analysis of 16 polycyclic aromatic hydrocarbons and 7 antibiotics in 48 environmental water samples. This strategy proved effective in detecting the presence and distribution of polar and nonpolar environmental pollutants in rivers and lakes. Moreover, this strategy has several advantages, such as ultrahigh sensitivity at the femtograms per liter level, good greenness, multiplexed quantitation, low sample consumption, and ease of operation. Overall, the utilization of the ultrasensitive and environmentally friendly BE approach presents a reliable and adaptable method for the identification of ultratrace environmental pollutants in water specimens, thereby enabling early monitoring of pollutant levels.
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CHEMOSPHERE
·
2023
·
IF 8.8
Wei Zhang,Wenjie Wu,Jianfei Wu,Xiaobin Liu,Jian Tian,Heng Li,Qingbiao Li,Yanmei Zheng
Although advanced oxidation processes (AOPs) based on persulfate (PS) is an attractive approach for repairing polycyclic aromatic hydrocarbons (PAHs) contaminated soils, limited oxidizability of PAHs and efficient in-situ activation of PS hinder its practical applications. In this study, we comprehensively examined the contributions of five representative surfactants on the oxidative remediation of PAHs-contaminated soil in terms of degradation kinetics of the pollutants, and further proposed an innovative coupling strategy of surfactant-enhanced thermally activated PS remediating PAHs-contaminated soil. The results showed that the degradation process of PAHs in soil was significantly facilitated only via adding sodium dodecyl benzenesulfonate (SDBS) and fitted the pseudo-first-order kinetic pattern. The removal of phenanthrene (PHE) reached 98.56% at 50 mM PS, 50 °C, 5 g L −1 SDBS and 48 h reaction time, accompanying an increase of 25% in reaction rate constant from 0.0572 h −1 (without SDBS) to 0.0715 h −1 . More importantly, SDBS-enhanced thermally activated PS degrading PAHs with higher benzene rings were more effective as the reaction rate constants of pyrene (PYR) and benzo(a)anthracene (BaA) were significantly increased by 49.40% and 56.86%. Additionally, only appropriate dosages (5–10 g L −1 ) of SDBS facilitated the oxidative degradation of PHE, as well as the aging time of contaminant-soil contact slowed down the enhancement of oxidative degradation of PHE by SDBS. Scavenger experiments demonstrated that SO 4 ·- and 1 O 2 were the dominant reactive oxygen species . Finally, a possible oxidative degradation pathway of PHE was proposed, and the toxicity of derived intermediates got alleviation by the assessment using the Toxicity Estimation Software Tool . This investigation was promising for in situ scale-up remediation of PAHs-contaminated soil.
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Journal of Cleaner Production
·
2023
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IF 11.1
Chun Wang,Qianqian Wang,Jintao Yu,Xinmeng Wang,Lijuan Wang,Bin Zhao,Lin Hao,Weihua Liu,Zhi Wang,Hao Chen,Qiuhua Wu
White pollution caused by the massive discharges of waste expanded polystyrene (WEPS) has become a critical global issue, so the effective conversion of WEPS is of great significance to reduce white pollution. Herein, adopting WEPS as raw material, three high-value-added hyper-crosslinked polymers (WEPS-HCPs) with high surface areas and abundant micro/mesoporous structures were synthesized via Friedel-Crafts alkylation reaction using dimethoxymethane, dichloroxylene and 4,4′-bis(chloromethyl)-1,1′-biphenyl (BCB) as cross-linker, respectively. The WEPS-HCPs were used as sorbent to extract aflatoxins (AFs) and all the HCPs exhibited high adsorption capacity . For the fast separation and recovery of the sorbent, WEPS-BCB was chosen as a model HCP to be magnetically functionalized to obtain a magnetic HCP (mWEPS-BCB) for the first time. Based on magnetic solid phase extraction with the mWEPS-BCB as sorbent, a fast and sensitive method was developed to determine trace level of AFs in grain food . Under the optimal conditions, the proposed method presented wide linear range (0.008–10.0 ng g −1 ), low detection limit (0.002–0.015 ng g −1 ) and satisfactory precision (relative standard deviation < 7%). Converting WEPS into a high-value-added sorbent not only provided a facile strategy for effective recycling of WEPS, but also developed a sensitive method for accurate determination of AFs in grain food, achieving significant economic and environmental benefits.
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Analytical Methods
·
2021
·Vol. 14
·期 3
·306-311
·
IF 2.896
Song Zhao,Hongbo Jiang,Chengbin Gong,Wenjing Qi,Lianzhe Hu,Yan Zhang
A novel fluorescent sensor based on an asymmetric anthracene derivative (SSAPA) was designed and synthesized. Using this molecule, a rapid and sensitive assay for detecting Tb3+ and ATP in aqueous solutions was established. The SSAPA molecule had excellent aggregation-induced emission (AIE) performance and good aqueous dispersion ability. This molecule could coordinate with Tb3+ and the fluorescence quenched linearly with the increase in the concentration of Tb3+ from 0.005 to 1.2 μM. Since both Tb3+ and adenosine triphosphate (ATP) have strong binding ability, ATP can compete with Tb3+ from the SSAPA/Tb3+ complex leading to fluorescence recovery. In this way, a brand-new fluorescent “turn-on” assay for ATP in the range from 0.01 to 0.4 μM was developed using the Tb3+-based complex probe. The detection limits for Tb3+ and ATP both reached single-digit nanomole per millilitre (2.8 nM and 4.5 nM, respectively), which demonstrated that this method has high sensitivity. Besides, Tb3+ and ATP also could be well detected in other complex environments such as real water samples or serum samples. This study provides a feasible assay for detecting trace amounts of Tb3+ and ATP in aqueous solutions.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
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IF 7.963
Jiaolong Huang,Peng Duan,Ling Tong,Weicheng Zhang
In this study, the influences of polystyrene microplastics (PS MPs) on the volatilization, photodegradation and photoinduced toxicities of anthracene and pyrene were determined in freshwater and artificial seawater. The PS MPs reduced the volatilization of anthracene and pyrene, and the volatilization reduction was highly dependent on the PS MPs sizes and concentrations. The PS MPs increased the photodegradation kinetics ( k p ) of anthracene by promoting 1 O 2 generation and altered the photodegradation pathways through OH attack of the photodegradation byproducts. However, the k p of pyrene was decreased by PS MPs suppressing the transfer of electrons from excited pyrene to oxygen. The PS MPs modified the pathways of pyrene photodegradation via OH attack of the photodegradation byproducts. Due to light shielding by DOM and/or PS MPs aggregates in seawater, the modification of the photodegradation pathways of anthracene and pyrene by PS MPs was hardly happened in seawater compared with in freshwater. By changing the concentrations of anthracene or pyrene and their photodegradation byproducts, the PS MPs greatly affected the photoinduced toxicities of anthracene and pyrene to Selenastrum capricornutum and Phaeodactylum tricornutum . The influences of PS MPs on the volatilization, photodegradation and photoinduced toxicity of anthracene and pyrene are important and should be carefully considered during environmental risk assessments of anthracene and pyrene.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Mingxia Sun,Juanjuan Feng,Jiaqing Feng,Haili Sun,Yang Feng,Xiangping Ji,Chunying Li,Sen Han,Min Sun
To improve the extraction efficiency of carbon fibers (CFs) toward organic pollutants, TiO 2 nanorod arrays (NARs) were grown in situ on CFs. Subsequently, biochar nanospheres and covalent organic framework nanospheres were separately introduced to functionalize the NARs. A sequence of materials was produced by regulating the reactant concentrations and characterized using a scanning electron microscope, an X-ray photoelectron spectrometer, an X-ray diffractometer, a Raman spectrometer, and a specific surface area analyzer. The materials were then deposited into separate poly(etheretherketone) tubes for in-tube solid-phase microextraction (IT-SPME). These tubes were evaluated with different types of organic pollutants (polycyclic aromatic hydrocarbons (PAHs), estrogens, bisphenols, and phthalate esters) using a combination of high-performance liquid chromatography and IT-SPME, and they exhibited diverse extraction performance. The extraction mechanism of each material is carefully discussed, and the structure–performance relationship is also summarized based on the chemical structures and extraction properties of the materials. The most efficient extraction materials for different analytes were discovered and used to develop analytical methods. Three online methods were used to sensitively detect PAHs, estrogens, and bisphenols in real water samples, respectively. Satisfactory results were obtained, including enrichment factors up to 6784, detection limits as low as 0.001 μg L −1 , linear ranges of 0.003–15.0 μg L −1 , and relative standard deviations ranging from 0.2% to 15.2%. The results indicate that these methods have some advantages over previous material-based methods.
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Arabian Journal of Chemistry
·
2021
·
IF 5.165
Qiong Jiang,Juanjuan Feng,Min Sun
Carbon fibers (CFs) were modified with carbon nanoparticles (CNPs) by a facile and fast flame preparation method. CNPs-CFs were observed by scanning electron microscope, and the nano-scaled granular structure on the surface was found. This material was also characterized by Raman microscope and X-ray photoelectron spectroscope. It was placed into a polyetheretherketone tube to get an extraction tube, which was connected with high performance liquid chromatography for online analysis. The tube displayed the effective extraction to several polycyclic aromatic hydrocarbons (PAHs), based on the possible hydrophobic and π stacking mechanism. Under the optimized conditions (60 mL of sample volume, 2.00 mL min −1 of sample rate, 0.5% of methanol in sample, 2.0 min of desorption time), an analytical method towards these PAH targets was established. The low limits of detection (0.001–0.005 μg L −1 ), satisfactory linear ranges (0.003–5.0 μg L −1 , 0.003–10.0 μg L −1 ) and efficient enrichment factors (1012–3164) were presented. The method was applied to detect trace targets in several water samples and satisfactory results were obtained. The method provided some superiorities over other analytical methods, like online test, shorter time and better sensitivity.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Linfeng Chen,Xike Tian,Yong Li,Chao Yang,Yunjie Huang,Yulun Nie
Simple and rapid sensing of polycyclic aromatic hydrocarbons (PAHs) remains a great technical challenge due to their chemical stability and structural similarity. Here, a simple, sensitive and cost-effective sensing strategy is proposed to detect multiple PAHs by utilizing the inner filter effect (IFE) and a reusable fluorescent sensor array consisting of four polyvinyl alcohol (PVA) composite carbon quantum dots (CDs) film sensors. The CDs/PVA films have a wide and tunable excitation range, which provide sufficient spectral overlap with PAHs and ensure the efficient occurrence of IFE. Under different excitations, the diverse UV absorption capacities of PAHs resulted in diverse spectral responses , enabling a unique chemical fingerprint for each PAH. Upon multivariate pattern recognition analysis, the array rendered high-throughput discrimination and sensitive quantification of 16 priority PAHs with 100% classification accuracy and detection limit as low as 57 nM. Moreover, the rapid and accurate screening of multiple environmental samples were also realized with the results consistent with high-performance liquid chromatography . This IFE-based reusable array is readily prepared, green and feasible, which exhibits great potential in environmental analysis and brings an advanced strategy to high-throughput sensing of more pollutants with similar structures and lack of recognition sites.
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CHEMOSPHERE
·
2021
·
IF 7.086
Xintong Li,Hongxia Zhao,Baocheng Qu,Yu Tian
Environmentally persistent free radicals (EPFRs) generated under irradiation have been widely detected in soil particles, atmospheric particles and microplastic particles, but the formation of EPFRs in water is not well understood. This study investigated the formation of EPFRs on particulate organic matter (POM) in water contaminated by anthracene (Ant) under irradiation. The photoformation and decay progress of EPFRs was represented with the help of electron paramagnetic resonance (EPR) technique on both actual POM and Fe(III)-montmorillonite simulated samples. EPR signals at the range of 10 16 to 10 17 spin/g were detected and the half-life time of EPFRs stored in water was at around 16.62 h and 60.80 h, much shorter than those in the air. The g factors were all larger than 2.0040, which indicated the generation of oxygen centered EPFRs. The primary intermediates were identified by gas chromatography-mass spectrometer (GC-MS) and a possible EPFR formation pathway during Ant degradation was proposed. The interaction between Ant and POM, and the hydroxylation and carbonylation of the intermediates made contributions to the generation of EPFRs. Meanwhile, the indirect photodegradation of bisphenol A (BPA) has been demonstrated by analyzing the reactive oxygen species (ROS) and photogenerated electrons in the solution with POM containing EPFRs. It is found that hydroxyl radicals (•OH) and singlet oxygen ( 1 O 2 ) were induced and might promote the photodegration. Overall, our present study provided useful information to understand the photoformation of EPFRs on POM and their fate in aqueous environments.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xiao Chen,Xing-Bao Wang,Shuhua Han,Dong Wang,Chuang Li,Weixiang Guan,Wen-Ying Li,Changhai Liang
Interactions between metals and oxide supports are crucial in determining catalytic activity, selectivity, and stability. For reducible oxide supported noble metals, a strong metal–support interaction (SMSI) has been widely recognized. Herein we report the intermediate selectivity and stability over an irreducible SiO2 supported Pt catalyst in the hydrogenation of anthracene that are significantly boosted due to the SMSI-induced formation of intermetallic Pt silicide and Pt–SiO2 interface. The limitation in the strong interaction between Pt nanoparticles and irreducible SiO2 has been breached by combining the strong electrostatic adsorption method and following the high temperature reduction strategy. Due to the isolated Pt active sites by Si atoms, the activated H species produced over the Pt2Si/SiO2 catalyst with an initial catalytic activity of 2.49 μmol/(m2/g)/h as well as TOF of 0.95 s–1 preferentially transfer to the outer ring of anthracene to 87% yield of symmetric octahydroanthracene (sym-OHA) by subsequent hydrogenation. In addition, the Pt2Si/SiO2 catalyst presents an excellent stability after five cycles, which can be attributed to the fact that intermetallic Pt2Si nanoparticles are anchored firmly onto the surface of the SiO2 support. The discovery contributes to broaden the horizons on the SMSI effect in the irreducible oxide supported metal particle catalysts and provides guidance to design the metal–SiO2 interface and tune the surface chemical properties in diverse application conditions.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 29
·期 17
·24612-24622
·
IF 4.223
Li Zhansheng,Zhao Hongxia,Li Xintong,Bekele Tadiyose Girma
Environmentally persistent free radicals (EPFRs) are an emerging class of environmental hazardous contaminants that extensively, stably exist in airborne particulate matter and pose harmful effects on human health. However, there was little research about the sources of EPFRs in actual atmospheric conditions. This study reported the occurrence, characteristics, and sources of EPFRs and polycyclic aromatic hydrocarbons (PAHs) in PM 2.5 collected in Dalian, China. The concentrations of PM 2.5 -bound EPFRs ranged from 1.13 × 10 13 to 8.97 × 10 15 spins/m 3 (mean value: 1.14 × 10 15 spins/m 3 ). Carbon-centered radicals and carbon-centered radicals with adjacent oxygen atoms were detected. The concentration of ∑PAHs ranged from 1.09 to 76.24 ng/m 3 , and PAHs with high molecular weight (HMW) were predominant species in PM 2.5 . Correlation of EPFRs with SO 2 , NO 2 , O 3 , and 12 kinds of PAHs indicated that both fuel (coal and biomass) combustion and photoreaction in atmosphere influenced the concentrations of EPFR. The positive matrix factorization (PMF) model results have shown that the primary sources contributed most of the EPFRs and those of secondary sources had a little proportion. Coal combustion (52.4%) was the primary contributor of EPFRs, followed by traffic emission (22.6%), industrial sources (9.6%), and secondary sources (9.2%) during the heating period, whereas industrial emission (39.2%) was the primary contributor, followed by coal combustion (38.1%), vehicular exhaust (23.5%), and secondary sources (9.6%) during the non-heating period. The finding of the present study provides an important evidence for further study on the formation mechanism of EPFRs in actual atmospheric to control the air pollution.
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