Catalysis Science & Technology
·
2023
·Vol. 13
·期 10
·3060-3068
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IF 5
Guanghua Liang,Jianyi Chen,Tao Dou,Zhijie Wu,Xiaofeng Li,Yuanshuai Liu
EU-1 zeolite is employed as an active component of a catalyst for isomerization or hydroisomerization of C8 aromatics (i.e., xylenes, ethylbenzene) in petrochemical processes to increase the para-xylene yield. However, conventional manufacturing of EU-1-based catalysts involves the production of mother liquors for zeolite synthesis which usually contain plentiful unreacted raw materials, or the negative impact of incorporated binders in mass transfer during reactions over shaped catalysts. Herein, we developed a novel route to prepare the monolithic EU-1 zeolite, and used it as an active component of a catalyst for hydroisomerization of ethylbenzene with meta-xylene. Recrystallization of the shaped zeolite precursors composed of incompletely crystallized zeolites with amorphous silica and alumina powders as binders in recycled mother liquor led to formation of the monolithic EU-1 zeolite. Transformation of binder species to a full-zeolitic phase was corroborated comprehensively by characterization methods. Compared with the conventionally fabricated counterpart, the monolithic EU-1 zeolite possessed similar mechanical strength, high crystallinity, and high acidity and, in particular, enhanced mesoporosity, which led to improved catalytic performances in hydroisomerization reactions. Our developed synthetic strategy provides an effective way to produce the monolithic EU-1 zeolite, but is also a reference for the sustainable production of other types of zeolitic materials for energy-related applications.
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CHEMISTRY OF MATERIALS
·
2023
·
IF 8.6
Meijun Wan,Yunchao Zheng,Xuemei Dai,Honglin Yang,Jingqiu Zhou,Jing Ou,Yaxin Yang,Meifang Liao,Zhining Xia,Lujun Wang
Covalent organic framework (COF) as a kind of crystalline porous material possesses intriguing advantages, including low density, large surface area, permanent porosity, and excellent chemical stability. This novel material has shown great potential in the development of chromatographic stationary-phase materials. In this work, a room-temperature solvothermal method was utilized to yield a uniformly spherical COF-modified silica named Sil-COF. Then, the thiol-ene click chemistry was further used to modify thiolated β-cyclodextrin on the spherical Sil-COF composite for chiral separation called Sil-COF-CD. A series of characterization methods were performed to identify the successful construction of COF-modified stationary-phase materials. Then, three types of nonpolar substances realized baseline separation on the Sil-COF column. In addition, 2-phenylpropionic acid and 1-phenyl-1-propanol were selected as model enantiomers to identify the chiral recognition capability of the Sil-COF-CD column. Sil-COF and commercial β-CD columns were compared to further confirm the superiority of the prepared chiral column. In addition, both COF-modified columns possessed good repeatability. The results open a new avenue to apply spherical chiral COF for the preparation of the HPLC stationary phase.
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CHEMOSPHERE
·
2023
·
IF 8.8
Yue Sun,Yanbo Liu,Gangsen Yue,Jinhui Cao,Chong Li,Jie Ma
Traditional natural attenuation studies focus on aqueous process in the saturated zone while vapor-phase biodegradation and natural attenuation in the unsaturated zone received much less attention. This study used microcosm experiments to explore the vapor-phase biodegradation and natural attenuation of 23 petroleum VOCs in the unsaturated zone including 7 monoaromatic hydrocarbons, 6 n-alkanes, 4 cycloalkanes , 3 alkylcycloalkanes and 3 fuel ethers. We found that monoaromatic hydrocarbon vapors were easily attenuated with significantly high first-order attenuation rates (9.48 d −1 -43.20 d −1 ) in live yellow earth, of which toluene and benzene had the highest rates (43.20 d −1 and 28.32 d −1 , respectively). The 13 aliphatic hydrocarbons and 3 fuel ethers all have relatively low attenuation rates (<0.54 d −1 ) in live soil and negligible biodegradation contribution. We explored the effects of soil types (black soil, yellow earth, lateritic red earth and quartz sand), soil moisture (2, 5, 10, and 17 wt%) contents and temperatures (4, 15, 25, 35 and 45 °C) on the vapor attenuation. Results showed that increasing soil organic matter (SOM) content, silt content, porosity and soil microorganism numbers enhanced contaminant attenuation and remediation efficiency. Increasing moisture content reduced the apparent first-order biodegradation rates of monoaromatic hydrocarbon vapors. The vapor-phase biodegradation had optimal temperature (∼25 °C in yellow earth) and increasing or decreasing temperature slowed down biodegradation rate. Overall, this study enhanced our understanding of vapor-phase biodegradation and natural attenuation of petroleum VOCs in the unsaturated zone, which is critical for the long-term management and remediation of petroleum contaminated site.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Tian-Tian Ma,Cheng Yang,Hai-Long Qian,Piming Ma,Tianxi Liu,Xiu-Ping Yan
Development of novel functional materials for effective isomer separation is of great significance in environmental science, chemical industry, and life science due to the different functions of isomers. However, the similar physicochemical properties of isomers make their separation greatly challenging. Here, we report the fabrication of trifluoromethyl-functionalized 2D covalent organic framework (COF) TpTFMB with 2,2′-bis(trifluoromethyl)benzidine (TFMB) and 1,3,5-triformylphloroglucinol (Tp) for the separation of isomers. TpTFMB was in situ-grown on the inner surface of a capillary for the high-resolution separation of isomers. The introduction of hydroxyl and trifluoromethyl functional groups with uniform distribution in 2D COFs is a powerful tactic to endow TpTFMB with various functions such as hydrogen bonding, dipole interaction, and steric effect. The prepared TpTFMB capillary column enabled the baseline separation of positional isomers such as ethylbenzene and xylene, chlorotoluene, carbon chain isomers such as butylbenzene and ethyl butanoate, and cis–trans isomers 1,3-dichloropropene. The hydrogen-bonding, dipole, and π–π interactions as well as the structure of COF significantly contribute to the isomer separation. This work provides a new strategy for designing functional 2D COFs for the efficient separation of isomers.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2023
·
IF 2.6
Jiajun Wei,Lingxiao Yi,Wang Yuxin,Erkang Li,Zhen Yujie,Fangyu Zhang,Xinlei Niu,Jinshan Wang,Deming Zhao,Yingmin Yu
Liquid–liquid equilibrium (LLE) measurements were conducted at a temperature of 298.2 K and a pressure of 101.3 kPa for the ternary system consisting of 1,3-propanediol, 2-propyl-1-heptanol, and various extractants (n-hexane, vinyl acetate, ethyl benzene, and water). By calculating the distribution constant (D) and selectivity (S) in each system, the ability of four extractants to separate the mixture of 1,3-propanediol and 2-propyl-1-heptanol was compared. Furthermore, the LLE data underwent regression using thermodynamic models NRTL and UNIQUAC. The degree of deviation between the experimental data and regression data was assessed using the root mean square deviation (RMSD) and the average absolute deviation (AAD). The RMSD values for the NRTL and UNIQUAC models were below 0.74 and 0.76%, respectively, with corresponding AAD values below 0.39 and 0.60%. These results indicate a robust concurrence between the experimental data and the outcomes of the regression analysis. Finally, the GUI-MATLAB tool was employed to validate the coherence of the experimental data with the regression parameters. σ-Profiles are used to discuss the interactions of substances in this work. The results showed that the D and S of all four systems were greater than 1, indicating that all four extractants were effective in separating 1,3-propanediol and 2-propyl-1-heptanol. The order of their extraction capacity was water ≥ hexane ≥ ethyl benzene ≥ vinyl acetate.
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JOURNAL OF CHROMATOGRAPHY A
·
2023
·
IF 4.1
Yuanyuan Fu,Zhentao Li,Changjun Hu,Qiaoyan Li,Zilin Chen
A new kind of covalent organic framework (COF) was first utilized as an stationary phase for open-tubular electrochromatography (OT-CEC) by in situ synthesis immobilized method at room temperature. On the basis of our previous work, 4,4′,4″-(1,3,5-Triazine-2,4,6-triyl)trianiline (TZ) and 2,5-bis(2-propyn-1-yloxy)-1,4-benzenedicarboxaldehyde (BPTA) were employed as building blocks for the synthesis of COF TZ-BPTA. The coated capillary and COF TZ-BPTA were characterized by scanning electron microscopy (SEM). Then, Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD) were also applied to characterize COF TZ-BPTA and the modified column. In SEM, it can be seen that COF TZ-BPTA was the spherical shape and the modified capillary was covered with globular particles equably. The COF TZ-BPTA coated column exhibited good separation resolution and efficiency towards two antiepileptic drugs and other kinds of small organic molecules involving alkylbenzene, sulfonamides, polycyclic aromatic hydrocarbon (PAH), parabens, amino acids and herbicides. The maximum column efficiency was over 2.8 × 10 5 plates·m −1 . In addition, the precisions (RSDs) of the retention times for the alkylbenzenes of intra-day runs (n = 3), inter-day runs (n = 3) and column-to-column runs (n = 3) were all less than 1.70% and separation performance was without obvious change within 100 times run. In addition, the real sample was tested on COF TZ-BPTA coated column. Hence, COF TZ-BPTA showed great potential in the separation domain.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Yue Liu,Dianlong Ge,Jijuan Zhou,Yajing Chu,Xiangxue Zheng,Li Ke,Pan Li,Yan Lu,Xue Zou,Lei Xia,Yawei Liu,Chaoqun Huang,Chengyin Shen,Yannan Chu
The investigation of volatile organic compounds (VOCs) in human metabolites has been a topic of interest as it holds the potential for the development of non-invasive technologies to screen for organ lesions in vivo. However, it remains unclear whether VOCs differ among healthy organs. Consequently, a study was conducted to analyze VOCs in ex vivo organ tissues obtained from 16 Wistar rats, comprising 12 different organs. The VOCs released from each organ tissue were detected by the headspace-solid phase microextraction-gas chromatography-mass spectrometry technique. In the untargeted analysis of 147 chromatographic peaks, the differential volatiles of rat organs were explored based on the Mann–Whitney U test and fold change (FC > 2.0) compared with other organs. It was found that there were differential VOCs in seven organs. A discussion on the possible metabolic pathways and related biomarkers of organ differential VOCs was conducted. Based on the orthogonal partial least squares discriminant analysis and receiver operating characteristic curve, we found that differential VOCs in the liver, cecum, spleen, and kidney can be used as the unique identification of the corresponding organ. In this study, differential VOCs of organs in rats were systematically reported for the first time. Profiles of VOCs produced by healthy organs can serve as a reference or baseline that may indicate the presence of disease or abnormalities in the organ’s function. Differential VOCs can be used as the fingerprint of organs, and future integration with metabolic research may contribute to the development of healthcare.
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ANALYTICAL LETTERS
·
2022
·
IF 2.267
Yu Huang,Yi Wu,Wenhui Li,Xiaohui Yan,Dapeng Wu
Highly spherical porous silica particles (PSPs) with a controlled pore size were prepared by ultrasonic spray drying and were used as a packing material for high-performance liquid chromatography (HPLC). By using organic additives added to the silica sol as porogens instead of low-melting salts, choosing the size of the colloidal SiO2 particles, and varying the type and the ratio of additives, the pore size of the PSPs was finely tuned from 2.9 to 34.4 nm. Subsequently, PSPs having pore sizes of 7.4, 13.5, and 29.0 nm were modified by chlorodimethyloctadecylsilane (PSPs-C18), and HPLC columns packed with the different PSPs-C18 were evaluated systematically using aromatic compounds and alkylbenzene derivatives as probes. A plate number of 81,000/m and the relative standard deviation of less than 1% in the retention time were obtained for pentylbenzene over 100 injection and HPLC separation cycles for the 7.4-PSPs-C18 column. Five proteins were also separated within 25 min using the 29.0-PSPs-C18 column.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Zhihui Liu,Siyuan Sun,Fan Yang,Hongchen Liu,Yang Sun,Na Ta,Ge Zhang,Sai Che,Yongfeng Li
Transition metal-based (Fe, Co, Cu, etc.) single-atom catalysts (SAC) have been widely used in the direct oxidation of ethylbenzene and benzene. However, their catalytic performance is limited by the low metal loading. Compared with traditional SAC, dual site single-atom catalysts (DSAC) show the advantages of abundant active sites, high metal loading, and excellent catalytic performance. Herein, a novel Fe/Cu N C DSAC was prepared by facile one-pot pyrolysis of formaldehyde, dicyandiamide, and metal salts. Dicyandiamide acted as the carbon source with advantage of high nitrogen content, which promoted the formation of metal centers and increased the metal loading. Meanwhile, the synergistic effect between Fe and Cu active centers was revealed to adjust the coordination environment, thus improving the catalytic activity of oxygen activation. The synthesized Fe/Cu N C DSAC demonstrated superior catalytic performance in ethylbenzene oxidation reaction with O 2 as a green oxidant under mild reaction conditions, with a 99 % conversion of acetophenone and no significant degradation of activity after 10 circles. In addition, NaCl was added into the synthesis as a template to adjust the pore structure, and the modified Fe/Cu N C DSAC showed excellent performance in benzene oxidation reaction with high product conversion. In conclusion, this work paves the way for the construction of efficient, green, and cost-effective catalysts for the direct oxidation of ethylbenzene and benzene.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 9
·24470-24478
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IF 5.19
Ma Ge,Xiao Han,Wei Xinming,Xiao Anshan,Sun Xiaoying,Gao Xiang
Oil leakage from water coolers in refinery circulating water occurs from time to time, which affects the long-term and stable operation of refinery units. So far, workers in the refineries still adopt manual check methods, opening water coolers one by one and checking the water’s smell and color to find out the spilled water coolers. In this study, a more rapid method of source appointment of oil spill in the circulating water by combining chemical fingerprinting with model recognition was developed. Firstly, chemical fingerprints including benzene/naphthalene series, and light hydrocarbon (C 3 -C 5 ) in oil samples from all water coolers in the refinery fluid catalytic cracking (FCC) unit were analyzed by gas chromatography-mass spectrometry (GC/MS). Gasoline, diesel, and poor oil could be distinguished in terms of benzene and naphthalene distribution. The three similar types of gasolines could be distinguished by the volatile hydrocarbons especially C 3 -C 4 . The classification model for the spill of gasoline, diesel, and poor oil in circulating water was constructed by the partial least squares discriminant analysis algorithm with a 100% correct classification rate at the concentration more than 10 ppm. The gasoline spills in the circulating backwater of the refinery were successfully recognized by the classification model. This method enables the rapid prediction of oil spill type in refinery circulating water, and a similar method by installing online instrument and software potentially can be used for monitoring the circulating water in real time.
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Journal of Pharmaceutical Analysis
·
2022
·
IF 14.026
Yikun Liu,Ning He,Yingfang Lu,Weiqiang Li,Xin He,Zhentao Li,Zilin Chen
Here, a styrene-based polymer monolithic column poly(VBS- co -TAT- co -AHM) with reversed-phase/hydrophilic interaction liquid chromatography (RPLC/HILIC) bifunctional separation mode was successfully prepared for capillary electrochromatography by the in situ polymerization of sodium p-styrene sulfonate (VBS) with cross-linkers 3-(acryloyloxy)-2-hydroxypropyl methacrylate (AHM) and 1,3,5-triacryloylhexahydro-1,3,5-triazine (TAT). The preparation conditions of the monolith were optimized. The morphology and formation of the poly(VBS- co -TAT- co -AHM) monolith were confirmed by scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FT-IR). The separation performances of the monolith were evaluated systematically. It should be noted that the incorporation of VBS functional monomer can provide π−π interactions, hydrophilic interactions, and ion-exchange interactions. Hence, the prepared poly(VBS- co -TAT- co -AHM) monolith can achieve efficient separation of thiourea compounds, benzene series, phenol compounds, aniline compounds and sulfonamides in RPLC or HILIC separation mode. The largest theoretical plate number for N , N′ -dimethylthiourea reached 1.7 × 10 5 plates/m. In addition, the poly(VBS- co -TAT- co -AHM) monolithic column showed excellent reproducibility and stability. This novel monolithic column has great application value and potential in capillary electrochromatography (CEC).
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JOURNAL OF CHROMATOGRAPHY A
·
2022
·
IF 4.601
Changjun Hu,Zhentao Li,Zhuang Hu,Qiaoyan Li,Yuanyuan Fu,Zilin Chen
Crown ethers are macrocyclic polyether compounds containing multiple -oxo-methylene-structural units, which are often used for recognition of metal ions and ammonium ions. Inspired by the molecular design of rotaxanes, a novel covalent organic nanospheres material (CON ADBC-Tp) constructed by 4,4′-diaminodibenzo-18-crown-6 (ADBC) and 2,4,6-triformylphloroglucinol (Tp) was rationally designed as stationary phase for the separation of compounds containing imidazole structure. Scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FT-IR) were carried out to confirm the morphology and composition of ADBC-Tp and ADBC-Tp modified capillary column. Thanks to the introduction of crown ether building ligands, the prepared capillary column exhibited excellent separation selectivity towards protonated imidazole structure, with benzimidazole and its 2-substituted derivatives as modal analytes. Moreover, separation of fungicides, nucleobases, short peptides and sulfanilamides were achieved on ADBC-Tp@capillary. The multifunctional ADBC-Tp@capillary with satisfactory reproducibility and stability gives great promise for separation science.
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