JOURNAL OF MATERIALS SCIENCE
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2024
·Vol. 59
·期 45
·21027-21039
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IF 3.5
Zhang Peng,Guo Mengya,Wang Fujiang,Tang Qiong,Ge Hui,Guo Shuke,Zhou Ligong,Li Xuekuan,Dong Jinxiang,Tang Mingxing,Liu Lei
Selective hydrogenation is an effective approach to utilize coal tar and slurry oil to produce high value-added fine chemicals. However, how to efficiently improve the selectivity of the target product and the stability of the catalyst is difficult. Herein, the PdZn alloy catalyst was synthesized by the assistance of strong interaction between active metal (Pd) and support (ZnO) for hydrogenation of anthracene to symmetrical octahydro anthracene (sym-OHA). The PdZn alloy catalyst reduced at 400 °C was found to exhibit a 100% conversion of the anthracen with 84.77% selectivity to sym-OHA under the optimized conditions (200 °C, 1 MPa). The characterization analysis indicated that the PdZn alloy with electron-rich Pd active sites is more efficient in the selective hydrogenation than the pure Pd metal. The study of the deep hydrogenation of sym-OHA (Hydrogenation of sym-OHA to perhydroanhtracene) showed that PdZn alloy catalysts were inactive to further hydrogenation of sym-OHA. Additionally, due to the strong interaction between Pd and ZnO, the Pd/ZnO(400) catalyst shows high stability for five cycles. These findings are of practical significance for the selective hydrogenation of polycyclic aromatic hydrocarbons (PAHs) to produce high value-added products.
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ANALYTICA CHIMICA ACTA
·
2024
·
IF 5.7
Min Sun,Jiaqing Feng,Yang Feng,Xubo Xin,Yali Ding,Juanjuan Feng
Background Because of the advantages of good selectivity , high sensitivity, and fast analysis, high performance liquid chromatography (HPLC) has become one of the modern analytical techniques in wide application range, such as biological analysis, environmental detection, pharmaceutical and food inspection, agriculture and other fields. The stationary phase greatly decides the chromatographic separation performance, so the development of novel stationary phase is most important for HPLC. Results Pyridyl conjugated microporous polymers (P-CMP) with one to four layers were modified on the surface of amino silica to obtain a novel core-shell material (SiO2@P-CMP) by the layer-by-layer assembly strategy and Chichibabin reaction . The relationship between the structure of SiO2@P-CMP and chromatographic performance was carefully investigated, and the retention mechanism was revealed. The interactions including π-π stacking, hydrophobic effect and hydrogen bond gradually enhanced with the increase of P-CMP layers on the silica surface. Compared with C18 column, SiO2@P-CMP columns displayed better separation selectivity for polycyclic aromatic hydrocarbons (PAHs). According to the relative retention values ( α ), the separation performance of SiO2@P-CMP columns ( α = 1.144–1.884) for PAH isomers and other analytes was obviously better than that of C18 column ( α = 0.998–1.487). Furthermore, the SiO2@P-CMP column with four layers was selected to separate different types of analytes (eight PAHs, four bisphenols , four estrogens and nine phthalates), and the peak order of analytes was different from that on the C18 column due to the influence of hydrogen-bonding and π-π interactions. The relative standard deviations (n = 10) of retention time and peak area on SiO2@P-CMP column were between 0.28 % and 1.98 %. Significance and novelty Pyridyl conjugated microporous polymer was introduced as the stationary phase for the first time in HPLC. The proposed column displayed better separation characteristics compared to Zorbax SB-C 18 column. It provided a new idea for the separation of small molecules and the development of chromatographic packing or extraction material.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Shuhui Huo,Xiaohui Deng,Nan Yang,Mengya Qin,Xiaonan Zhang,Xiaoqiang Yao,Cuixiang An,Pengxin Zhou,Xiaoquan Lu
In this study, a durable hydrophobicity hydrazone covalent organic framework (BTCH-PTA-COF) has been developed as fiber coating, which was applied to solid-phase microextraction (SPME) of polycyclic aromatic hydrocarbons (PAHs). The hydrophobic and π-π packing interactions between BTCH-PTA-COF and PAHs were confirmed by contact angle experiments and Van der Waals surface electrostatic potential analysis. Further, large specific surface area, good chemical and thermal stability have positive promoting effect on extraction. The method of wide linearity (0.25–300 µ g·L −1 ), low detection limits (0.03–0.05 µ g·L −1 ) and high enrichment factors (767–1411) for the detection of PAHs is explored, coupling BTCH-PTA-COF based SPME with gas chromatography with hydrogen flame detector (GC-FID). The relative standard deviations (RSDs) for inter-day and intra-day extractions of PAHs are ranging from 4.1 % to 9.6 % and 2.9 % to 6.4 %, respectively. The method successfully detected and quantified trace PAHs in tea beverages and river water samples with recoveries from 88.5 % to 104.8 %. The BTCH-PTA-COF coated fiber is ultra-stable in recycled extraction and reused at least 120 times, which could surpass published and commercial SPME fiber.
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JOURNAL OF CHROMATOGRAPHY A
·
2024
·
IF 3.8
Yali Yang,Jia Chen,Xiaojing Liang,Bei Liu,Kaijun Quan,Xiuhui Liu,Hongdeng Qiu
In this paper, three imidazole- and C18- bifunctional silica stationary phases (Sil-Im-C18) were prepared by adjusting introduction interval of octadecyltrichlorosilane (ODS) and 3-imidazol-1-ylpropyl(trimethoxy)silane (TMPImS), which can be used for reversed-phase liquid chromatography (RPLC) and ion exchange chromatography (IEC) with adjustable performance. The successful preparation of Sil-Im-C18 were confirmed by the characterizations of elemental analysis, infrared spectroscopy (FTIR) and contact angle (CA). Chromatographic performance of Sil-Im-C18 were evaluated by the separation of Tanaka test mixture, alkylbenzenes, linear PAHs and a set of analytes with different properties (uracil, phenol, 1,2-dinitrobenzene and naphthalene), and compared with commonly used C18 column. It was found that the chromatographic performance of Sil-Im-C18 changed significantly with the difference in bonding amount of imidazole and C18. Sil-Im-C18 demonstrated the excellent separation performance towards polycyclic aromatic hydrocarbons (PAHs), phenylesters, phenylamines , phenols and inorganic anions, and notably, nucleobases and nucleosides can be separated using pure water as mobile phases . The van Deemter plot showed that the column efficiency of Sil-Im-C18-3 was 64,933 plate· m − 1 for naphthalene, indicated that Sil-Im-C18 was reasonably chromatographic columns. The RSD values of retention time were 0.22 %-0.61 % for 10 needles alkylbenzenes injected continuously at 50 °C to investigate thermal stability and repeatability, all the fluctuations of k of naphthalene were less than 2.3 % for Sil-Im-C18-1 during flushing 24 h with the mobile phase at different pH values (pH = 3 and 8), the retention time of alkylbenzenes were almost same for Sil-Im-C18-1 at different time, the RSD values of retention time of alkylbenzenes were 0.45 %-2.28 % for two batches Sil-Im-C18-1, revealing the excellent repeatability, thermal stability, durability and reproducibility of Sil-Im-C18, and implying a commercial prospect.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Yuqian Li,Haomin Chen,Wei Li,Beidou Xi,Caihong Huang
The remediation of sites co-contaminated with polycyclic aromatic hydrocarbons (PAHs) and heavy metals (HMs) poses challenges for efficient and ecofriendly restoration methods. In this study, three strains ( Pseudomonas sp. PDC-1, Rhodococcus sp. RDC-1, and Enterobacter sp. EDC-1) were isolated from sites contaminated with PAHs and HMs. The constructed bacteria consortium was then immobilized using biochar, bentonite, and peat. The immobilized bacteria consortium (IBC) demonstrated efficient removal ability of phenanthrene (58.1 %-73.4 %) and benzo[ a ]pyrene (69.6 %-83.5 %) during 60 days. Additionally, the IBC decreased soil bacterial richness and diversity, but increased the relative abundance of Proteobacteria phylum and Ochrobactrum genus, which were capable of degrading PAHs. Soil microbial co-occurrence network with IBC was classified into three main modules, and 14 genera were identified as keystone taxa linked to PAHs degradation and HMs resistance. The IBC enhanced the dioxygenase metabolic pathways for PAHs degradation, including phthalic acid and salicylic acid pathways, which became the main driving factor affecting PAHs removal efficiency based on the structural equation modeling analysis. This study confirmed the potential application of the constructed IBC in the bioremediation of soil co-contaminated with PAHs-HMs, and provides insights into key removal mechanism and main driving factor of the enhanced elimination of PAHs.
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PEDOSPHERE
·
2024
·
IF 5.2
Xiaonuo ZHANG,Yaxi DENG,Goujian CHI,Hong LÜ,Hongxia ZHAO
ABSTRACT Rhizoremediation has emerged as a burgeoning approach for the removal of petroleum hydrocarbons (PHCs) from soil, with a primary emphasis on terrestrial plant systems. However, the mechanism on how soil microbiomes influence the dissipation of PHCs within a hygrophyte planting system has yet to be fully elucidated. This work concentrated on investigating the potential evolution of soil microbiomes and their effect on the PHCs dissipation within the Suaeda salsa (L.) Pall. planting system using the pot experiment. Two representative compounds, namely polycyclic aromatic hydrocarbons (PAHs) and n-alkanes, were used as target PHCs. The findings revealed a significant efficiency in the dissipation of petroleum hydrocarbons (PHCs) in soil, particularly with respect to n-alkanes. The high dissipation efficiency of PHCs was the synergistic result of both the root accumulation and the microbial biodegradation. The key microbes involved in PHCs dissipation were revealed, with the dominant phylum of Protobacteria and genus of Salinimicrobium . The alterations in microbial diversity and abundance were closely associated with the root exudation and PHCs exposure. Significant differences in enzyme activity, which serves as an indicator of soil health and fertility, were observed between the rhizospheric and non-rhizospheric soil, attributed to root exudation. This study offers novel insights into the phytoremediation potential for Suaeda in PHC-contaminated soil and serves as a valuable scientific reference for the phytoremediation of such soils.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xudong Zhang,Yang Deng,Yanhua Liu,Fan Yang,Yugao Wang,Jun Shen
Carbazole is a highly value-added compound derived from crude anthracene. Deep eutectic solvents (DESs) have been extensively used as promising green solvents for the separation of target compounds from mixture. In this work, 135 acidic DESs, formed by combining 9 quaternary ammonium salts with 15 common acids, were screened based on the conductor-like screening model for real solvents (COSMO-RS) model. The four top-ranked DESs, including tetraethylammonium chloride (TEAC)/2 acetic acid (AA), TEAC/2 propionic acid (PA), tetrapropylammonium chloride (TPAC)/2AA, and TPAC/2PA were identified as suitable extractants for carbazole separation based on their performance index (PI). Among them, TEAC/2AA had the best separation performance for carbazole due to its highest PI value (1448.19). Liquid–liquid extraction experiments were performed, and the results were in good accordance with those predicted by COSMO-RS calculations. Therefore, TEAC/2AA was determined as the most promising DES for the carbazole separation. The extraction conditions of TEAC/2AA were optimized. The extraction efficiency (EE) and selectivity (SE) of carbazole were 97.67 % and 66.64 %, respectively, under the optimal extraction conditions (25 ℃, 5 min of extraction time, DES-oil mass ratio of 1:5, initial carbazole concentration of 5000 ppm). Additionally, the deionized water was employed to regenerate the DES and recovery of carbazole. The recycling performance of promising DES was also investigated. Finally, quantum chemical calculations and Fourier Transform Infrared spectroscopy (FT-IR) analysis were conducted to explore the separation mechanism. The results indicated that the separation of carbazole by DESs were predominantly dominated by hydrogen bonds and van der Waals interaction. This work provided a valuable reference for the selection and design of DES extractants to separate other high value-added components from mixture.
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Catalysts
·
2024
·Vol. 14
·期 5
·311
·
IF 3.8
Changzhao Chen,Zhe Yuan,Shenshen Sun,Jiacai Xie,Kunfeng Zhang,Yuanzheng Zhai,Rui Zuo,Erping Bi,Yufang Tao,Quanwei Song
Soil contamination by polycyclic aromatic hydrocarbons (PAHs) has been an environmental issue worldwide, which aggravates the ecological risks faced by animals, plants, and humans. In this work, the composites of nanoscale zero-valent iron supported on carbonylated activated carbon (nZVI-CAC) were prepared and applied to activate persulfate (PS) for the degradation of PAHs in contaminated soil. The prepared nZVI-CAC catalyst was characterized by scanning electron microscopy (SEM), X-ray diffractometer (XRD), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). It was found that the PS/nZVI-CAC system was superior for phenanthrene (PHE) oxidation than other processes using different oxidants (PS/nZVI-CAC > PMS/nZVI-CAC > H2O2/nZVI-CAC) and it was also efficient for the degradation of other six PAHs with different structures and molar weights. Under optimal conditions, the lowest and highest degradation efficiencies for the selected PAHs were 60.8% and 90.7%, respectively. Active SO4−•and HO•were found to be generated on the surface of the catalysts, and SO4−•was dominant for PHE oxidation through quenching experiments. The results demonstrated that the heterogeneous process using activated PS with nZVI-CAC was effective for PAH degradation, which could provide a theoretical basis for the remediation of PAH-polluted soil.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
·
IF 11.3
Na Zhang,Lei-qiang Liu,Yao Zhang,Jun Shen,Yu-gao Wang,Gang Liu,Yan-xia Niu
Coal tar pitch (CTP) is a carbon material with abundant yield in China, but the toxic polycyclic aromatic hydrocarbons (PAHs) contained in it have restricted its broader applications. In order to reduce the PAHs content, an alkylation method was developed in this study to modify CTP (MCTP) by using 1-dodecene as the alkylating reagent, and the optimal reaction conditions (temperature 170 °C, time 4 h, solvent dosage 60 times that of CTP, and alkylating reagent dosage 4 times that of CTP) for synthesizing the MCTP were determined by alkylation modification with model compounds. Compared with CTP, the content of PAHs in MCTP was reduced by 97.35 %. The mechanism of the reaction was explained by analyzing the types of alkylation products and combining structural analyses of CTP and MCTP. PAHs emissions from fumes and the toxic equivalent quantity (TEQ) among different environmental standards were greatly reduced, while MCTP demonstrated low cytotoxicity and ecotoxicity. The method can also be applied to the toxicity assessment of road materials such as alkylation by-products.
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TALANTA
·
2014
·
IF 3.511
Man Wang,Shihai Cui,Xiaodi Yang,Wentao Bi
An easy preparation of g-C 3 N 4 /Fe 3 O 4 nanocomposites by chemical co-precipitation has been demonstrated. The as-prepared materials were characterized by X-ray diffraction, transmission electron microscopy , Fourier transform infrared spectroscopy and thermogravimetric analysis . The high affinity of g-C 3 N 4 toward polycyclic aromatic hydrocarbons and the magnetic behavior of Fe 3 O 4 were combined to provide an efficient and simple magnetic solid phase extraction (MSPE). The adsorption and desorption of polycyclic aromatic hydrocarbons on g-C 3 N 4 /Fe 3 O 4 were examined. Different factors affecting the magnetic solid phase extraction of polycyclic aromatic hydrocarbons were assessed in terms of adsorption, desorption, and recovery. Under the optimized conditions, the proposed method showed good limits of detection (LOD, S/N=3) in the range of 0.05–0.1 ng mL −1 and precision in the range of 1.8–5.3% (RSDs, n =3). This method was also successfully applied to the analysis of real water samples; good spiked recoveries over the range of 80.0–99.8% were obtained.
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JOURNAL OF THE ENERGY INSTITUTE
·
2025
·
IF 6.2
Hao-Dong An,Guang-Hui Liu,Yan-Jun Li,Ling-Zhi Tuo,Yu-Hong Kang,Zhi-Ping Wang,Yong Gao,Chen Shi,Yun-Yan Gao,Xian-Yong Wei
Hydrofining of low-grade lignite liquefied oils into high-density liquid fuels is a critical pathway for their value-added utilization. However, abundant condensed aromatic rings (ARs) and O atoms in such crude oils pose significant challenges for secondary upgrading, particularly in achieving concurrent AR hydrogenation and hydrodeoxygenation in one-pot to produce alkyl cyclanes. In view of this, Co-CoN x @C 650 was constructed by a cascade preparation strategy consisting of in-situ co-pyrolysis and NH 3 nitridation. It has highly dispersed Co-CoN x dual-sites and carbon substrate with abundant defects/vacancies, and exhibits good performance in AR hydrogenation and hydrodeoxygenation. In addition, this catalyst can effectively activate H 2 and promote the synergistic transfer of H ··· H, δ+ H ··· H δ− , and H · . Good accessibility, cyclic stability, and renewability make it suitable for the hydrogenation of medium/large-sized molecules such as naphth-2-ol and aryl ethers into cyclanes. The liquefied oil (SP TD ) from Dongming lignite thermal dissolution in n -hexane is rich in aromatics (76.1 %), while refined oil (CHSP TD ) from catalytic hydrofining over Co-CoN x @C 650 is rich in saturated hydrocarbons (91.7 %), especially alkyl cyclanes (69.8 %). The efficient conversion of aromatic-oxygenated moieties demonstrated by Co-CoN x @C 650 provides a new solution for converting low-grade lignite liquefied oils into value-added cyclanes-rich liquid fuels.
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EES Catalysis
·
2025
·
IF 8.1
Guangxun Sun,Peng Xue,Changle Yue,Yang Li,Hongfu Shi,Xin Zhang,Fengyu Tian,Junxi Li,Zekun Guan,Bin Liu,Zhi Liu,Yunqi Liu,Yuan Pan
The development of a synergistic coupling catalyst at the atomic scale for slurry-phase hydrogenation of vacuum residue (VR) is extremely challenging. Herein, we designed and constructed a robust coupling catalyst comprising Mo single atoms and MoS2 (Mo SAs–MoS2) using a reaction induction transformation strategy. The spontaneous generation of Mo SAs–MoS2 synergistically promoted H2 activation and enhanced local active hydrogen concentration in the hydrogenation of VR. Benefiting from the strong hydrogen concentration distribution in MoS2 and Mo SAs, the catalyst revealed remarkable hydrogenation performance toward VR with a TOFT of up to 0.39 s−1, liquid product yield of 92 wt%, and coke content of 0.6 wt%. Theoretical calculations revealed that the synergistic action of Mo SAs–MoS2 facilitated electron transfer between Mo species and reactants, reducing the desorption energy barriers for H2 and anthracene and thereby promoting the hydrogenation of VR. This work provides a novel idea for the design of efficient coupling catalysts for strengthening local active hydrogen concentration in the hydrogenation of VR, and this concept can be applied to other hydrogenation systems.
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