ANALYTICAL CHEMISTRY
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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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高影响因子
WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 7
·1-13
·
IF 2.9
Zhou Danli,Zhang Dong,Zhang Ming,Lü Ting,Huang Jingang,Zhao Hongting,Lin Jun
To clarify the sorption mechanism and removal efficiency of PAHs by waste biomass-based magnetic sorbents, the sorption performance of magnetic Myriophyllum aquaticum biomass (MMaB) for PAHs was studied. The structural characteristics and magnetic properties of MMaB were measured by FTIR, SEM–EDS, XRD and VSM. Batch experiments were carried out to evaluate the effects of contact time, initial concentration and properties of PAHs, pH, ionic strength and temperature on PAH sorption. The results showed that the sorption of seven PAHs achieved equilibrium at approximately 4–6 h, which fit well to the pseudo-second-order kinetic model. The isotherms followed the Freundlich model and linear model well, indicating that the sorption process was controlled by chemisorption. The distribution parameter ( K d ) values were 91.3, 563.7, 1010.5, 2917.8, 2706.6, 9046.8 and 15969.0 L·kg −1 for naphthalene, acenaphthene, fluorene, phenanthrene, anthracene, pyrene, and fluoranthene on MMaB, respectively, following the order of their hydrophobicity (e.g., K ow ). A positive correlation was obtained: log K d = 0.8091log K ow + 1.7034. Water chemical properties such as pH and ionic strength had no obvious effect on PAH removal. The spontaneity, feasibility and exothermic properties of PAH removal by MMaB were explained from thermodynamic point of view. The as-prepared MMaB sorbent underwent four consecutive sorption cycles and had good cycling performance. These studies indicate that MMaB has great potential as an easily-prepared, easy-to-operate and efficient biosorbent to remove PAHs from wastewater.
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TALANTA
·
2023
·
IF 6.1
Haoyu Long,Yanhao Jiang,Yanjuan Liu,Yuefei Zhang,Wei Chen,Sheng Tang
In this work, 2,4,6-tris(4-aminophenyl)-1,3,5-triazine (TAPT) and 1,3,5-tris(4-formylphenyl)benzene (TFPB) were used as monomers to construct a triazine-containing imine-linked covalent organic framework (COF), which was then bonded onto the surface of aldehydized silica (SiO 2 –CHO), and finally a COF@silica composite material (TAPT-TFPB COF@SiO 2 ) was successfully prepared. The chromatographic separation performance of SiO 2 –CHO, TAPT-TFPB COF@SiO 2 and TAPT-TFPB COF@SiO 2 /SiO 2 –CHO (80/20, mass ratio) was evaluated and compared. It was found that separation efficiency was obviously enhanced by adding an appropriate amount of SiO 2 –CHO into TAPT-TFPB COF@SiO 2 . The obtained TAPT-TFPB COF@SiO 2 /SiO 2 –CHO showed more favorable separation ability than SiO 2 –CHO and TAPT-TFPB COF@SiO 2 . Various aromatic compounds including alkylbenzenes , polycyclic aromatic hydrocarbons , environmental endocrine disruptors , foodborne stimulants and phenyl ketones were effectively separated on the TAPT-TFPB COF@SiO 2 /SiO 2 –CHO column in reversed phase chromatography mode. The silica microspheres surface-modified with triazine-containing imine-linked COFs proved to be a new type of promising chromatographic packing materials.
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JOURNAL OF CHEMICAL EDUCATION
·
2023
·
IF 3
Xiang Wan,Dian Wang,Yuqing He,Jiafei Wang,Qin Xu,Donglin Zhao,Fazhi Xie,Qishu Qu
High-performance liquid chromatography (HPLC) experiments are an important part of the undergraduate analytical instrumentation laboratory courses and usually use commercial C18 silica-packed reversed-phase columns. In this experiment, a simple method of preparing SiO2 core–shell packed columns was developed to enable students to master the whole process of HPLC experiment from stationary phase preparation and column packing to separation experiments, just as they do for gas chromatography. Nonporous SiO2 particles with a particle size of approximately 2.2 μm were prepared by a three-step dilution reaction using the sol–gel method. The product yield was 92.1%. Monodisperse and spherical SiO2 core–shell particles (SiO2@dSiO2) with a particle size of about 2.4 μm were prepared by a one-step hydrothermal method using the prepared SiO2 spheres as the core. The product yield was 83.3%. The prepared SiO2@dSiO2 particles were derivatized with n-octadecyldimethylchlorosilane and then packed into a stainless steel chromatography column. A high column efficiency of 83,188 theoretical plates per meter was obtained for fluorene in reversed-phase mode for the separation of a mixture of polycyclic aromatic hydrocarbons. The column efficiency obtained with this method is the same as that of a commercial column packed with fully porous particles of the same particle size. The SiO2 core–shell stationary phase preparation method developed in this experiment has the advantages of simple process, high yield, and good repeatability. The experiment can be designed to be completed over a period of 1–3 weeks. Inorganic material synthesis is another important aspect of this experiment.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2023
·
IF 7.8
Wei Zhang,Heng Li,Siqiang Xiao,Jianfei Wu,Chuanhu Wang,Xiaobin Liu,Qingbiao Li,Yanmei Zheng
Controllable delivery of persulfate (PS) and the enhancement of oxidative availability of pollutants in in-situ oxidative remediation of low-permeability polycyclic aromatic hydrocarbons (PAHs) contaminated soil are crucial. To tackle the above challenges, the coupling of Tween 80 solubilization enhanced oxidation of phenanthrene (PHE) in low-permeability soil under electrokinetic remediation (EKR) was proposed. Firstly, batch degradation experiments showed that the addition of Tween 80 significantly inhibited the degradation of PHE in soil under thermally activated PS, as the dosage of Tween 80 increased from 0 % to 1 % with the corresponding removal rate declining from 99.19 % to 40.90 %. Accordingly, in-situ electrokinetic delivery of Tween 80 and PS was regulated in further EKR, intending to reduce unproductive consumption. PS was more uniformly delivered to the whole remediation regions from the cathode chamber by electromigration , while Tween 80 was transported into the soil from the anode chamber by electroosmosis , which made Tween 80 solubilization and PS oxidation achieve synergistic effect . And the total removal rate of PHE reached 64.90 % under this strategy, which had increased by 415.90 % and 8.76 %− 130.14 % compared with only EKR or EKR coupling single enhanced technology , respectively. After further thermal activation of transported PS at 50 ℃ by electrical resistance heating, the total removal rate of PHE increased to 71.58 %. EPR spectrum indicated that SO 4 . - and OH . were responsible for the degradation of PHE.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yaling Wang,Maolin Wang,Qing Xie,Xiyun Cai
We report new activated persulfate systems with cyclodextrin (CD)-coated Fe 3 O 4 @Fe 0 nanoparticles (Fe 3 O 4 @Fe 0 -CD) that are characterized by both highly activating persulfates and rapidly accessing hydrophobic PAHs. Fe 3 O 4 @Fe 0 -β-CD displays chain-like structure of core–shell Fe 3 O 4 @Fe 0 nanoparticles coated with a CD layer (about 5.9 nm). CD coating stabilizes the polycrystalline structure of Fe 3 O 4 @Fe 0 nanoparticles and accelerates mass transfer of PAHs in water, thereby making Fe 3 O 4 @Fe 0 -β-CD intrinsically stable and reactive. Fe 3 O 4 @Fe 0 -β-CD/PS, featured by high yields of highly reactive Fe(IV), had about 30-fold rate constants of naphthalene (Nap) in water as much as Fe 3 O 4 @Fe 0 /PS. Fe 3 O 4 @Fe 0 -β-CD/PS completely removed Nap in water during 13 of total 18 supplementations of Nap and/or PS, whereas Fe 3 O 4 @Fe 0 /PS completely removed Nap only at the first supplementation of Nap. Likewise, Fe 3 O 4 @Fe 0 -β-CD/PS completely removed Nap in simulated groundwater, and degraded four PAHs in soils by >63%. This study may provide a technical basis for the developments of new PS activators to remove recalcitrant hydrophobic contaminants in water and soils.
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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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Food Analytical Methods
·
2023
·Vol. 16
·期 6
·1131-1144
·
IF 2.9
Yu Chen,Luo Xiaogang,Wu Fengshou,Zhang Juan
A covalent organic framework/reduced graphene oxide composite (COF/rGO) was fabricated by facile ultrasonic self-assembly strategy and further coated onto stainless-steel wire by physically adhesion for headspace solid-phase microextraction (HS-SPME) of polycyclic aromatic hydrocarbons (PAHs) prior to their determination by gas chromatography-flame ionization detection (GC-FID). Compared with the individual porphyrin-based COF and GO, the as-prepared COF/rGO composite effectively prevented the stacking of GO nanosheets and exhibited enhanced extraction efficiency due to the synergistic effect, with the enrichment factor up to 8816 for phenanthrene. The morphology, structure, and stability of COF/rGO composite was characterized by Fourier transform infrared spectroscopy, X-ray diffraction, scanning electron microscopy, thermogravimetric analysis, and N 2 adsorption–desorption. Effective adsorption and desorption parameters including extraction temperature, extraction time, desorption temperature, desorption time, agitation speed, and ionic strength were optimized. The established HS-SPME/GC-FID method based on COF/rGO composite fiber was evaluated in terms of linear ranges from 0.5 to 250.0 ng mL −1 with R 2 ≥ 0.9985, limits of detection in the range of 0.09–0.59 ng mL −1 , and limits of quantitation in the range of 0.31–1.97 ng mL −1 . The intra-day, inter-day, and fiber-to-fiber relative standard deviations (RSDs) were in the range of 1.86–4.37%, 2.48–5.40%, and 3.51–7.81%, respectively. The established method was employed to determine trace level of PAHs in honey with good recoveries (62.99–128.8%) and reliable reproducibility (0.51–7.63%).
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Food Analytical Methods
·
2023
·Vol. 16
·期 6
·1110-1119
·
IF 2.9
Zhong Ming,Huang Lijun,Zhou Binbin,Liu Yuliang,Fang Mian,Wang Ying
A new type of magnetic zinc metal–organic framework molecularly imprinted polymer (MZMMIP) was created by a crystal growth method, combined with molecular imprinting technology. The material was designed to solve the problems associated with metal–organic frameworks, which have the disadvantages of small pore size and low selectivity in the detection field. MZMMIPs were characterized by SEM, XRD, FTIR, TGA, BET, etc. The results showed that MZMMIPs achieved good crystalline form, excellent magnetic separation ability, rich pore structure, and large specific surface area (602.4 m 2 /g). Furthermore, the results of the adsorption experiment show that the crystal growth method with molecular imprint technology not only improved the MZMMIP adsorption capacity (64 mg/g) and microporous aperture, but also accelerated its adsorption (3 min) and elution rate (10 min) on the target product. With the introduction of molecular imprinting technology, MZMMIPs show a suitable adsorption selective performance (selection factor is 1.6) in the adsorption performance test of structural and nonstructural analogs of pyrene. MZMMIPs display good stability and reusability (the adsorption capacity of MZMMIPs decreased by only 21.8% after 10 elution times). The detection method in the study was successfully implemented for the determination of pyrene in vegetable oil, and achieved an excellent detection effect. The detection limit of MZMMIPs to pyrene is 0.11 µg/kg. The recovery ranged from 93.34 to 95.92%.
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FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Yu Chen,Zemin Zhao,Ze Li,Jieying Jing,Wenying Li
Hydrogenation saturation of phenanthrene was an effective method to acquire high energy density fuels. It is essential to design highly active and stable hydrogenation saturated catalyst to realize the above reaction. Herein, series of Ni-Co/NiAlOx catalysts were synthesized by reducing at different temperatures. Activity evaluation showed that the catalysts reduced at 560 °C (Cat-560) possessed a phenanthrene conversion amount of 8.0 mmol·g -1 active component·h −1 and 98% perhydrophenanthrene selectivity after running 6 h under 300 °C, 5 MPa. Furthermore, it was found that Cat-560 presented superior specific activity (4.3 mmol·kg −1 ·s −1 ) and TOF (41.1 × 10 −3 s −1 ) for symmetric octahydrophenanthrene hydrogenation (the rate determining reaction), and its specific activity was 3 times as high as that of the catalysts reduced at 520 °C The excellent hydrogenation performance of Cat-560 could be attributed to its special geometric and electronic structure. Characterization indicated that the Ni 2+ in Ni-Co/NiAlO X catalyst was mainly located in the nickel aluminum spinel octahedral sites, which was beneficial to the reduction of Ni and the formation of smaller Ni particles. Moreover, it was explored that the Ni d charge density of Cat-560 catalyst was −0.12 e, which was suitable for the adsorption and activation of phenanthrene and symmetric octahydrophenanthrene.
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TALANTA
·
2023
·
IF 6.1
Li Xu,Wei Hu,Fengshou Wu,Juan Zhang
In this work, a novel spherical metal organic framework (MOF) was first in situ grown on the surface of iron wire (IW), in which IW served as the substrate and metal source for MOF (type NH 2 -MIL88) growth without adding additional metal salts in the process, while spherical NH 2 -MIL88 provided more active sites for further construction of multifunctional composites. Subsequently, a covalent organic framework (COF) was covalently bonded to the surface of the NH 2 -MIL88 to obtain the IW@NH 2 -MIL88@COF fibers, which were used for headspace solid-phase microextraction (HS-SPME) of polycyclic aromatic hydrocarbons (PAHs) in milk samples prior to determination by gas chromatography-flame ionization detection (GC-FID). Compared with the fiber prepared by physical coating, the IW@NH 2 -MIL88@COF fiber prepared by in situ growth and covalent bonding exhibits better stability and possesses more uniform layer. The extraction mechanism of the IW@NH 2 -MIL88@COF fiber for PAHs was discussed, which mainly owed to π-π interactions and hydrophobic interactions. After optimization of the primary extraction conditions, the SPME-GC-FID method was established for five PAHs with a wide linear range (1–200 ng mL −1 ), good linearity coefficient (0.9935–0.9987) and low detection limits (0.017–0.028 ng mL −1 ). The relative recoveries for PAHs detection in milk samples ranged from 64.69 to 113.97%. This work not only provides new ideas for the in situ growth of other types of MOF, but also provides new methods for the construction of multifunctional composites.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiahao Dong,Yan Kang,Shaoping Kuang,Haoqin Ma,Mei Li,Jingqian Xiao,Yafei Wang,Zizhang Guo,Haiming Wu
Microplastics, as emerging pollutants, can adsorb polycyclic aromatic hydrocarbons (PAHs) in aqueous environments. However, the coeffects of PAHs and microplastics on aquatic organisms are vague. In this study, nanoscale and micron-scale microplastics (30 mg/kg) and phenanthrene (10 mg/kg) were added to aquatic sediment to explore the effects of different particle sizes of microplastics and typical PAHs on invertebrates ( Tubifex tubifex ) and microbes after 28 days operation. The fluorescence signal of fluorescently labelled micron-scale and nanoscale microplastics were detected in T. tubife x, especially nanoscale microplastics. The reduced activities of CAT, GST, SOD and MDA in T. tubifex suggested that the micron-sized microplastics and PAHs exacerbated the oxidative damage to T. tubif ex. Microbial analysis confirmed that microplastics and PAHs decreased the abundance of Proteobacteria , Fusobacteriota and Bacteroidetes in the gut of T. tubifex and thereby affected the degradation of phenanthrene. Microplastics also reduced the abundance of Bacteroidetes , Acidobacteria and Proteobacteria in sediment. The abundance of salicylate hydroxylase enzyme that related to PAHs metabolism was increased with the addition of phenanthrene. The results in this study would be useful for further risk assessment of PAHs and microplastics in aquatic environments.
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