TURKISH JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 4
·597-619
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IF 1.3
YUAN HANG,CAO GUI-PING,LV HUI
The reaction solvent and catalyst play an essential role in the Prins reaction for the synthesis of 3-methyl-3-buten-1-ol (MBO) from formaldehyde and isobutene. The reactivity of the solid base catalyzed Prins condensation reaction by formaldehyde and isobutene in supercritical CO2 was investigated using CsH2PO4 modified HZSM-5. We finds that the alkaline sites of the alkali-loaded catalyst can extract the α-H on isobutene to generate olefin carbon negative ions, while the supercritical CO2 with weak Lewis acidity can activate formaldehyde to carbon positive ions, which can combine more easily with the carbon negative isobutene to react, thus improving the reactivity of the reaction system.
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ANALYTICA CHIMICA ACTA
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2026
·
IF 6.1
Xiaolong Shen,Ruizhi Tang,Shujuan Ma,Yangyang Bian,Zichao Tang,Junjie Ou
Background As a class of star macrocyclic molecules, cucurbit [n]urils (CB[n]) have gained extensive applications across multiple fields, including perovskite batteries, adsorption separation, room-temperature phosphorescence and biomolecular science and so on. The acquisition of high-purity CB[n] presents a significant challenge, especially for researchers without a dedicated background in organic synthesis and purification. The separation of individual CB[n] homologues is notoriously difficult, especially in the case of CB[7] and CB[5] due to their similar solubility and chemical properties. Therefore, development of specific and selective chromatographic methods is necessary for efficient separation of CB[n] homologues. Results In this work, three types of bipyridine-containing hybrid monolithic materials were designed and fabricated through “one-pot” approach, and then employed as an adsorption platform for the separation of CB[5] and CB[7] via supramolecular affinity chromatography strategy. This novel method offers efficient separation based on the differential molecular recognition mechanism of CB[5] and CB[7] toward the guest bipyridine moiety. Compared with the guests within the polymer chains, exposing the guests at the terminal ends of the adsorbent surface would benefit the specific adsorption capability of CB[7]. After optimizing the chromatographic conditions, the separation of CB[5] and CB[7] was successfully achieved on hybrid monolithic materials modified with 4,4′-bipyridine (Monolith-Ⅱ-Bp), enabling the isolation of 12 mg CB[5] and 10 mg CB[7] with high-purity from 40 mg of the crude product, corresponding to yields of 30.0% and 25.0%, respectively. Significance This work is the first to introduce hybrid monolithic materials and a separation strategy based on specific and reversible host-guest interactions, enabling simplified purification of CB[5] and CB[7] and accurate determination of their purity by MALDI-TOF MS. This approach is expected to serve as a reliable laboratory-scale method for the preparation of high-purity CB[n] homologues.
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ACS Omega
·
2026
·
IF 5.2
Yulin Sun,Yiwei Zhang,Yong He,Wubin Weng,Yanqun Zhu,Peixi Liu,Zhihua Wang
Mn-based catalysts usually exhibit considerable potential for enhancing the catalytic ozonation of volatile organic compounds (VOCs) at a lower temperature. In this study, bimetallic oxides M-Mn (M = Cr, Cu, Co) were supported on HZSM-5 zeolites to degrade dimethyl carbonate (DMC, chemical formula C3H6O3), a typical VOC emitted during the productive process of lithium batteries, with Mn/ZSM-5 for comparison. The Cr-doped catalyst CrMn/ZSM-5 could achieve 92% DMC conversion with 91% CO2 selectivity (O3/DMC = 6, T = 120 °C), showing an excellent catalytic performance among the prepared catalysts. The exceptionally low-temperature activity of CrMn/ZSM-5 was attributed to the synergistic effect of its large surface area, sufficient oxygen vacancies, and suitable acidity and reducibility, which collectively enhanced the level of O3 activation and accelerated DMC degradation. Furthermore, the catalyst demonstrated desirable stability and resistance to varying concentrations of water vapor. To elucidate the reaction pathway, in situ DRIFTS was employed to track the evolution of intermediate species during the adsorption and catalytic ozonation of DMC. With a further study of DFT calculation, the reaction mechanism of DMC catalytic ozonation on CrMn/ZSM-5 catalysts was put forward.
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Inorganic and Nano-Metal Chemistry
·
2026
·
IF 1.7
Heng-Feng Du,Jia-Tian Shang,Hong-Biao Tang,Shi-jie Wang,Xing Li
Functionalized Au nanomaterials have significant potential in colorimetric detection of fatal toxic metals. In this work, a simply colorimetric sensor was designed and prepared for visual detection of Hg(II) ions based on gold nanoparticles (AuNPs) modified by 5-(m-aminophenyl)tetrazole (APT) and characterized by transmission electron microscopy (TEM), dynamic light scattering (DLS) and UV − vis absorption spectroscopy. The colorimetric sensor exhibited the fine anti-interference and selectivity in an environment with the presence of other interfering ions. The limit of detection (LOD) is 0.6 µmol/L by the naked eye, and 0.21 µmol/L by UV-vis spectroscopy, indicating that the sensor of AuNPs modified with APT (APT@ AuNPs) could be used for the quantitative determination of Hg2+. Based on the above peculiarity, the sensor could be used to detect Hg2+ in real samples.
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CARBOHYDRATE RESEARCH
·
2026
·
IF 3.4
Dongqi Liu,Jun Qian,Xing Chen,Qiaoling Liu,Xiaolei Liu,Xiaoqian Wang,Siyu Zhou,Ying Guan,Liang Zhou,Siquan Xu
A SnCl 4 ·5H 2 O/LVA-DMSO binary system was developed for glucose conversion. • The optimized system achieved 84% HMF yield at 150 °C within 10 min. • DMSO enhanced HMF formation by improving solvation and suppressing side reactions. • Balanced Lewis-Brønsted acidity was crucial for glucose to HMF. A deep eutectic solvent (DES) composed of SnCl 4 ·5H 2 O and levulinic acid (LVA) was developed and combined with dimethyl sulfoxide (DMSO) to construct an efficient reaction medium for the conversion of glucose into 5-hydroxymethylfurfural (HMF). Under the optimized conditions, the Sn/LVA-16-DMSO binary solvent, coupled with AlCl 3 ·6H 2 O as the catalyst, afforded an HMF yield of 84% at 150 °C within 10 min. The effects of key parameters, including solvent composition, DES molar ratio, catalyst dosage, glucose dosage, reaction temperature, and reaction time, were systematically investigated. Response surface methodology (RSM) revealed that reaction temperature and glucose dosage were the most significant linear factors affecting HMF yield within the studied range. The system also showed acceptable recyclability, as HMF could be extracted from the reaction mixture with a recovery efficiency of 86%, and an HMF yield of 52% was retained after five consecutive cycles. FTIR, DSC, TG, and DTG analyses indicated that the Sn/LVA DES formed a strong hydrogen-bonding network and modified the coordination environment of Sn species, while the combination of DMSO and AlCl 3 ·6H 2 O further provided favorable solvation and Lewis-Brønsted acid synergy for glucose conversion. Compared with previously reported DES-based systems, the present homogeneous DES-DMSO strategy combines a high HMF yield of 84% with a short reaction time of only 10 min, demonstrating an efficient approach for the rapid conversion of glucose to HMF. Download: Download high-res image (416KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wei Zhou,Wanglong Mao,Pingyang Huang,Xiong Huang,Haoyuan Xu,Bo Wu,Xiaofang Jiang,Xiangtao Chen,Hanyu Liu,Guofu Zhou,Jinyou Xu
This study introduces a facile method for the controlled growth of addressable planar arrays of highly luminescent, catalyst-free 1,4-bis(5-phenyloxazol-2-yl)benzene (POPOP) nanowires. By employing a hollow mask over a faceted sapphire substrate, simultaneous control over the position and orientation of the nanowires is achieved through a mask-confined graphoepitaxial growth, offering substantial advantages over traditional post-growth assembly techniques. High-temperature annealing creates parallel nanogrooves on the sapphire surface, inducing a graphoepitaxial effect that aligns the nanowires with a consistent [102] crystallographic axis. The hollow mask further aids in precisely localizing nanowire growth through its shadowing effect. Optoelectronic investigations reveal that these nanowires emit intense and stable blue photoluminescence at room temperature, with a broad spectrum spanning from 400 to 600 nm. This luminescence is achieved through excitation by continuous-wave ultraviolet light or two-photon absorption using femtosecond infrared light. Notably, the emission quantum efficiency of POPOP nanowires reaches 59 %, a remarkable improvement over the 12 % observed in powder counterparts when excited with 405 nm light. Transit absorption spectra indicate that ground state bleaching and excited state absorption display consistent kinetics within a 100 ps time window, suggesting the same origin from singlet excitons. The precise alignment and positioning of these nanowires make them viable for in-situ integration into photodetectors with rapid ultraviolet light responses. This study advances the controlled growth of catalyst-free nanowire arrays and enhances the understanding of the optoelectronic properties of POPOP nanowires.
研究领域:
材料科学
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纳米科技
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光电子学
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凝聚态物理
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表面科学
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有机半导体
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APPLIED CATALYSIS A-GENERAL
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2012
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IF 3.903
Hui-hui Wu,Gang Li
In situ growth of ZSM-5 crystals on the surface of Ni-based alloy supports by hydrothermal synthesis and their mechanical, structural stability were investigated. ZSM-5 crystals grown on the wall of a long (750 mm) tubular reactor with a small inner diameter (1 mm) was evaluated as a structured catalyst for cracking of n -heptane as a model endothermic fuel. The results have shown that the adhesion strength between ZSM-5 crystals and the support was strong enough to resist a heating/fast-cooling cycle (the sample was immersed into water immediately after being heated to be 750 °C). The crystalline structure of ZSM-5 crystals was also stable against the heating/fast-cooling cycle. The structured catalyst was shown to be catalytically active for cracking of n -heptane (LHSV = 200 h −1 ) at 700 °C. The formation rates of gaseous cracking products were 9.8 ml min −1 and 29.3 ml min −1 for the bare tubular reactor and the tubular reactor with ZSM-5 crystals grown on the wall, respectively. These structured catalysts show high promise for cracking of endothermic fuels at high temperatures.
研究领域:
催化化学
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材料科学
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化学工程
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能量转换
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Shaoqing Wang,Yan Jiao,Zhihe Li,Zhen Wan,Yu Han,Weiming Yi
In this paper, a surface encapsulation method has been developed to synthesize the HZSM-5 @Al-KIT-6 hierarchical zeolites, due to the poor mono-aromatic hydrocarbons (MAHs) selectivity and rapid coke deactivation during the catalytic upgrading lignin pyrolysis vapors. Results showed that the acidity and accessibility of HZSM-5 @Al-KIT-6 hierarchical zeolite can be modulated by changing the TEOS/HZSM-5 mass ratio during catalyst synthesis. The three-dimensional (3-D) cubic mesoporous shell can capture the bulky phenolic oligomers and pre-crack for further reforming. The highest MAH content (44.03%) and lower polycyclic aromatic hydrocarbons (PAHs) (23.79%) were produced when the TEOS/HZSM-5 mass ratio was 1.0. The hierarchical zeolites improved the yield of xylenes due to the enhanced alkylation reaction. In addition, the micro-mesoporous highway reduced the formation of coke deposition. The catalytic mechanism of hierarchical zeolites was then proposed based on the obtained results. This study provides a reference for pilot-scale experiments for the catalytic upgrading lignin pyrolysis vapors.
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BIODEGRADATION
·
2023
·Vol. 34
·期 4
·371-381
·
IF 3.6
Yue Caixu,Jia Nan,Lv Xueru,Wang Shenghui
3, 5, 6-Trichloro-2-pyridinol (TCP) is a metabolite of the insecticide chlorpyrifos and the herbicide triclopyr, and it is higher toxic than the parent compounds. Microbially-mediated mineralization appears to be the primary degradative pathway and the important biological process of detoxification. However, little information is available on TCP complete metabolic pathways and mechanisms. In this study, the degradation of TCP was studied with a novel strain Micrococcus luteus ML isolated from a stable TCP degrading microbiota. Strain ML was capable of degrading 61.6% of TCP (50 mg/L) and 35.4% of chlorpyrifos (50 mg/L) at 24 h and 48 h under the optimal conditions (temperature: 35 °C; pH: 7.0), respectively. It could also degrade 3, 5-dichloro-2-pyridone, 6-chloropyridin-2-ol, 2-hydroxypyridine and phoxim when provided as sole carbon and energy sources. Seven TCP intermediate metabolites were detected in strain ML and two possible degradation pathways of TCP were proposed on the basis of LC–MS analysis. Both the hydrolytic-oxidative dechlorination pathway and the denitrification pathway might be involved in TCP biodegradation by strain ML. To the best of our knowledge, this is the first report on two different pathways responsible for TCP degradation in one strain, and this finding also provides novel information for studying the metabolic mechanism of TCP in pure culture.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Chao Miao,Shumei Chen,Lixing Liang,Kaixuan Shang,Jing Ouyang
In this paper, we used kaolinite tailings as raw materials to design and prepare ZSM-5 zeolite with “flower ball” morphology. Through the functional design of the material, Cr–Ce/ZSM-5 catalysts were prepared for CO 2 -assisted ethane oxidative dehydrogenation reaction (CO 2 -ODH). The folds and grooves on the surface of the “flower ball” ZSM-5 carrier act as a good anchor site for the loading of the active components, thus better anchoring Cr and Ce metal oxides , and leading to a strong interaction between the active component and the carrier. The 5%Cr–10%Ce/ZSM-5 catalyst exhibited the best catalytic performance, the conversion rate of C 2 H 6 and the selectivity of C 2 H 4 can always maintain the initial 64% and 80% within 30 h stability test at 800 °C. The existence of abundant Cr 6+ species in catalyst strengthens the binding ability of the catalyst and active oxygen species and promotes the formation-gasification process of carbon deposits on surface of the catalyst.
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Processes
·
2022
·Vol. 10
·期 12
·2480
·
IF 3.352
Linli Xu,Jianhui Fu,Cunbin Du,Qianqian Xu,Baojian Liu,Zongbi Bao
The solubility of 2,5-furandicarboxylic acid (FDCA) and its synthetic intermediates (e.g., 5-formylfuran-2-carboxylic acid, FFCA) provides fundamental information for the preparation and purification of the value-added biocompound FDCA. We measured the solubility of FDCA and FFCA in binary water + 1,4-dioxane mixtures with different mixing ratios at 303.15 K–342.15 K. The obtained solubility values were correlated with the Jouyban-Acree-van’t Hoff model, and the preferential solvation theory was used to study the microscopic dissolution mechanism. The solubility of FDCA/FFCA increases with increasing temperature, and pure 1,4-dioxane dissolves more solutes than pure water. FFCA shows higher solubility than FDCA. In the binary solvent mixtures, the phenomenon of co-solvency exists for both FDCA and FFCA, i.e., at a 1,4-dioxane mole fraction of about 0.60, FDCA and FFCA dissolve the most. Acceptable mean percentage deviations (MPD) (5.5% and 6.9%) are obtained for FDCA and FFCA (Jouyban-Acree-van’t Hoff model). The calculated preferential solvation parameters show different dissolution mechanisms at different solvent compositions. When the 1,4-dioxane mole fraction is 0.17~0.62/0.63, FDCA/FFCA are preferentially solvated by 1,4-dioxane. Otherwise, they are preferentially solvated by water. A trend similar to the “co-solvency phenomenon” is observed in the differences in solubility of FFCA and FDCA. This study gives important guidance for the use of binary water and 1,4-dioxane solvents in practical FDCA purification.Keywords:solubility;binary solvent mixtures;water + 1,4-dioxane;2,5-furandicarboxylic acid;5-formylfuran-2-carboxylic acid;co-solvency phenomenon
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Hongyu Qu,Xiangcheng Li,Xiao Han,Xinqiang Feng,Junjie Li,Zhendong Wang,Weimin Yang
The upgrading and utilization of 5-hydroxymethylfurfural (HMF) as a platform chemical for the manufacture of biofuels and biopolymers have drawn a lot of attention, especially for the selective hydrogenation of HMF to the biobased polymeric monomer tetrahydrofuran-2,5-dimethanol (THFDM). However, the catalytic hydrogenation of HMF with sustainability remains challenging. Herein, we report the synthesis of the Ni@U-Silicalite-1 catalyst, which shows a satisfying selectivity to THFDM (95.6%) under mild reaction conditions (1.5 MPa H2 and 130 °C). Characterization results show that the U-Silicalite-1 zeolite has a short b-axis, a flat reaction surface, and enlarged mesopores, which facilitate the accessibility to active sites of HMF. Meanwhile, the high distribution and small size of Ni nanoparticles contribute to the excellent catalytic efficiency and recyclability. Moreover, the strong interaction between Ni species and U-Silicalite-1 zeolite prevents the aggregation and leaching of Ni nanoparticles and endows the Ni@U-Silicalite-1 catalyst with good stability.
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