SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Peng Ding,Ping Wu,Qihao Cao,Hongbo Liu,Chongjun Chen,Min-Hua Cui,He Liu
The use of co -metabolic substrates is effective for polycyclic aromatic hydrocarbons (PAHs) removal, but the potential of the high phenol concentrations in coal chemical wastewater (CCW) as a co-metabolic substrate in microbial electrolysis cell (MEC) has been neglected. In this study, the efficacy of varying phenol concentrations in comparison to simple substrates for degrading naphthalene in MEC under comparable COD has been explored. Results showed that phenol as a co-metabolic substrate outperformed sodium acetate and glucose in facilitating naphthalene degradation efficiency at 50 mg-COD/L. The naphthalene removal efficiency from R P , R A , and R G was found to be 84.11 ± 0.44 %, 73.80 ± 0.27 % and 72.43 ± 0.34 %, respectively. Similarly, phenol not only enhanced microbial biomass more effectively, but also exhibited optimal COD metabolism capacity. The addition of phenol resulted in a stepwise reduction in the molecular weight of naphthalene, whereas sodium acetate and glucose led to more diverse degradation pathways. Some bacteria with the potential ability to degrade PAHs were detected in phenol-added MEC, including Alicycliphilus , Azospira , Stenotrophomonas , Pseudomonas , and Sedimentibacter . Besides, phenol enhanced the expression of ncrA and nmsA genes, leading to more efficient degradation of naphthalene, with ncrA responsible for mediating the reduction of the benzene ring in naphthalene and nmsA closely associated with the decarboxylation of naphthalene. This study provides guidance for the effective co-degradation of PAHs in CCW with MEC, demonstrating the effectiveness of using phenol as a co-substrate relative to simple substrates in the removal of naphthalene.
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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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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Yi Li,Xinze Wu,Hui Lyu,Huaixia Chen,Xueping Dang
A novel polyaniline (PANI) coating doped with Zn 5 (H 2 L n ) 6 (NO 3 ) 4 (Zn 5 , H 3 L n =(1,2-bis(benzimidazole-2-yl)-ethenol) cluster on a stainless-steel wire was prepared by the electrodeposition method for the headspace solid-phase microextraction (HS-SPME) of nine volatile phenols. Scanning electron microscopy, Fourier transform infrared spectrometry, energy dispersive spectrometry and thermogravimetry were employed to characterize the morphology, composition, structure and thermal stability of the Zn 5 /PANI composite coating. The extraction efficiency of the Zn 5 /PANI composite coating for nine phenols was nearly 2 times higher than that of pure PANI coating. After the extraction conditions were optimized, an HS-SPME-gas chromatography-flame ionization detector (GC-FID) method was developed for the determination of nine phenols in water samples. The HS-SPME-GC-FID method had superior analytical performance with good linearities (0.05–50.0 μg/L) and low limits of detection (0.01–0.08 μg/L). Then, the proposed method was successfully applied for the determination of nine phenols in water samples with satisfactory recoveries (79.4–110.0%).
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Nannan Zhang,Xiao Chen,Shiyao Liu,Jipeng Meng,Marc Armbrüster,Changhai Liang
High-entropy alloys (HEAs), as new heterogeneous catalytic materials, possess remarkable catalytic performance in numerous reactions. However, rational and controllable synthesis of these complex structures remains a challenge. In this work, bulk and carbon nanotube (CNT)-supported ultrasmall PtFeCoNiCu HEA nanoparticles with an average particle size of 1.58 nm are prepared by lithium naphthalenide-driven reduction under mild conditions. The supported PtFeCoNiCu/CNT catalyst exhibits high catalytic activity in the aqueous-phase hydrogenation of maleic anhydride to succinic acid with a selectivity of 98% at full conversion of maleic acid (the hydrolysis product of maleic anhydride), a low apparent activation energy (Ea = 49 kJ mol–1), and excellent stability. Moreover, a much higher mass-specific activity of Pt in the catalyst is displayed over PtFeCoNiCu/CNT (1515.4 mmolmaleic acid gPt–1 h–1) than that of 5 wt % Pt/CNT (388.0 mmolmaleic acid gPt–1 h–1). This work provides a strong support for HEAs as advanced heterogeneous catalysts and will be of great significance for promoting the research and application of HEAs in the field of selective hydrogenation.
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Energy Storage Materials
·
2023
·
IF 20.4
Chen Wu,Jieming Hu,Hanxian Chen,Chengyi Zhang,Mingli Xu,Lin Zhuang,Xinping Ai,Jiangfeng Qian
Prussian blue analogues (PBAs) have been attracting intense attention owing to its two-electron storage capability and considerable cost advantage, especially in Na-ion and K-ion batteries. However, things are quite different when it comes to Li-ion batteries, because lithium-containing Li 4 Fe(CN) 6 precursor is not commercially available and thus the traditionally prepared Li-deficient FeFe(CN) 6 products fail to couple with commercial graphite anode for full cells. Herein, we put forward a potential matching principle to guide the chemical pre-lithiation of FeFe(CN) 6 into a Li-rich Li x FeFe(CN) 6 ( x varies from 0 to 2) cathode. The potential matching principle was convincingly confirmed by theoretical analysis and over-lithiation experiments. Perylene-Li reagent was elaborately screened to serve as both Li + and electron donor for controllable chemical lithiation reaction while preserving the host framework stable. Our work provided a general guiding principle and effective methodology for controllable synthesis of Prussian blue analogues in gradient lithiation depth, which could be served as a platform for in-depth, systematic and comprehensive research on the properties of PBAs materials.
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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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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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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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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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JOURNAL OF MOLECULAR STRUCTURE
·
2023
·
IF 3.8
Yuxiu Fu,Xiaoli Song,Yaming Pang,Yinan Zheng,Liguo Gao
In this paper, a green solvent [BMIM] [PF 6 ] ionic liquid was selected for the extraction and separation of quinoline from simulated wash oil. The effects of extraction temperature, extraction time, and solvent oil ratio on the extraction of quinoline from wash oil were studied. The optimal process parameters were obtained by changing single factor conditions and optimizing the experiment using response surface methodology. When the temperature is 71 ℃, the time is 60 min, and the solvent oil ratio is 3:5, the extraction efficiency can reach 67%. The ionic liquids were recovered and their properties were investigated by infrared spectroscopy. The mechanism of quinoline extraction by ionic liquids was analyzed using infrared spectroscopy and GROMACS kinetic simulation calculations.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Rui Shi,Yipeng Huang,Yanqun Yang,Zhuqiang Wu,Zhengyi Chen,Guihua Ruan
In this work, spherical amine-functionalized mesoporous silica (Sp- Amino-Si ) molecular sieve was fabricated by an acid hydrothermal method using 3-aminopropyltriethoxysilane as a modifier and toluene as the solvent. The results of scanning electron microscopy, Barrett-Joyner-Halenda pore size distribution, Fourier transform-infrared spectroscopy, and low-angle X-ray diffraction patterns revealed that the Sp- Amino-Si was monodispersed microspheres with uniform and controllable pore sizes sharing two-dimensional hexagonal P6mm symmetry and a large number of amino groups. The Sp- Amino-Si molecular sieve was verified to be suitable for the selective separation of aromatic hydrocarbons (AMHs) containing two fused benzene rings among other compounds from environmental water matrix. Under the optimized conditions, the Sp- Amino-Si exhibited much higher adsorption efficiency for AMHs (above 88.19%), comparing to the original SBA-15 (below 44.52%). The maximum adsorption capacities for naphthalene, methyl naphthalene, 2-methyl naphthalene, and acenaphthene were 477.1, 1006.5, 893.3, and 1253.2 µg·g −1 , respectively. The high selectivity of Sp- Amino-Si for the four AMHs attributed to the size sieving and p-π interactions between the lone pair electrons of amine groups and the π-electrons in AMHs molecules. The Sp- Amino-Si based solid-phase extraction coupled with high performance liquid chromatography detection method was constructed for the analysis of the four AMHs, and the recoveries of spiked AMHs ranged from 89.67% to 112.74% with a relative standard deviation lower than 5.75%. This study provides some inspiration and a reliable method for AMHs separation, removal, and analysis.
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