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APPLIED CATALYSIS B-ENVIRONMENTAL · 2016 · IF 8.328

Construction of heterostructured MIL-125/Ag/g-C3N4 nanocomposite as an efficient bifunctional visible light photocatalyst for the organic oxidation and reduction reactions

Zhiwang Yang,Xueqing Xu,Xixi Liang,Cheng Lei,Yuhan Cui,Wenhua Wu,Yaoxia Yang,Zhe Zhang,Ziqiang Lei

Photocatalytic synthesis using visible light is a desirable chemical process because of its potential to utilize sunlight. A heterostructured MIL-125/Ag/g-C 3 N 4 nanocomposite was implemented as an efficient bifunctional visible-light response catalyst for the photoreduction of nitrocompounds and the oxidation of alcohols. The photocatalyst was prepared via an accessible method and characterized by XRD, SEM, TEM, XPS, FT-IR, N 2 adsorption–desorption isotherm, UV–vis DRS, PL and EIS. The reactive efficiency of the photocatalyst depends on two primary factors, one is the light adsorption of catalysts, Ag nanoparticles (NPs) were photodeposited on the surface of g-C 3 N 4 and MIL-125 to increase visible-light absorption via the surface plasmon resonance. And the other is the separation efficiency of the photogenerated charge carrier. As an electron-conduction bridge in the interface between MIL-125 and g-C 3 N 4 , Ag NPs could facilitate the direct migration of photoinduced electrons from g-C 3 N 4 to MIL-125 and retard the recombination of electron-holes. Therefore, the MIL-125/Ag/g-C 3 N 4 sample shows highest photocatalytic activity compared with MIL-125, g-C 3 N 4 , MIL-125/Ag and MIL-125/g-C 3 N 4 . A corresponding photocatalytic mechanism of these reactions was discussed in detail. Moreover, the photoreduction of nitrocompounds and oxidation of the alcohols with superior conversions and selectivities were obtained, and the catalyst can be recycled four times. It is concluded that MIL-125/Ag/g-C 3 N 4 would be a promising visible light photocatalyst in the field of selective organic transformations.

研究领域: 材料科学 · 化学工程 · 环境科学
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ADVANCED FUNCTIONAL MATERIALS · 2019 ·Vol. 29 ·期 19 ·1901101 · IF 15.621

Electrocontrolled Liquid Marbles for Rapid Miniaturized Organic Reactions

Zhou Liu,Tiyun Yang,Yuxing Huang,Yang Liu,Liucheng Chen,Libo Deng,Ho Cheung Shum,Tiantian Kong

Miniaturized droplet reactors hold great promise for the development of green and sustainable chemistry. However, handling liquids with small volumes, especially viscous ones, in a convenient and loss-free manner remains a challenge. Here, by electrically controlling the coalescence and mixing of particle-coated droplets, also known as liquid marbles, an effective microreactor is demonstrated for miniaturized chemical reactions involving viscous reagents. By applying an electric voltage to marbles, the induced electromixing of marble microreactors promotes the reaction rate and the product yield. The advantages of electromixed marble reactors are manifested by a series of chemical reactions between aldehydes and 2-methylindole in viscous glycerol solution. The electrically-controlled coalescence and mixing establish liquid marbles as microreactors for rapid, efficient, and miniaturized chemical reactions.

研究领域: 化学工程 · 绿色化学 · 材料科学
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JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY · 2024 · IF 3.1

Ortho C–H Bond Activations in an Atmospheric Microwave Plasma Ion Source

Guanru Chen,Fengjian Chu,Shuheng Zhang,Wangyu Li,Shiwen Zhou,Wei Wei,Weiwei Chen,Xiaozhi Wang,Lei Yue,Hongru Feng,Yanli Cui,Yuanjiang Pan

C–H bond ortho-substitution reaction has always been a significant and challenging topic in organic chemistry. We proposed a synthesis method based on microwave plasma torches. High-resolution mass spectrometry was used to monitor rapid reaction products. 2-Alkylbenzimidazole can be formed through the reaction of phenylnitrenium ion and nitriles on a millisecond scale. This reaction can achieve the one-step formation of benzimidazoles from benzene ring single-substituted compounds without the addition of external oxidants or catalysts. A similar C–H bond activation reaction can be accomplished with ketones. Meanwhile, the microwave plasma reactor was modified, and the resulting 2-methylbenzimidazole was successfully collected, indicating the device has good application potential in organic reactions such as C–H bond activation reaction.

研究领域: 有机化学 · 合成化学 · 分析化学
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Molecular Catalysis · 2021 · IF 5.062

Alkene-modified Fe3O4 nanoparticle-mediated construction of functionalized mesoporous poly(ionic liquid)s: Synergistic catalysis of mesoporous confinement effect and hydrogen proton for organic transformations

Zhong-Qiu Liu,Sheng-Nan Li,Qing-Shuai Zeng,Yu-Jing Liu,Jin-Mao You,An-Guo Ying

The preparation of mesoporous poly(ionic liquid)s (MPILs) is critically fundamental for the design of heterogeneous catalysts, whereas traditional methods are difficult to obtain these materials with both well-defined mesoporous structure and unique functionality. Here, HClO 4 -functionalized MPILs with well-defined mesoporous structure were successfully fabricated, in which the alkene-modified Fe 3 O 4 nanoparticles as structural reinforcer play a vital role for mesoporous structure formation. The MPILs were characterized by N 2 adsorption/desorption, scanning electron microscope (SEM), transmission Electron Microscope (TEM), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), and vibration sample magnetometry (VSM), and the results confirm that MPILs possess moderate surface area, well-defined mesoporosity, abundant active ionic centers, as well as efficient magnetic recovery. The resulting MPILs show excellent catalytic activity for condensation reaction and Knoevenagel condensation. The kinetic study reveals that the excellent catalytic activity of MPILs is attributed to the synergistic catalysis of mesoporous confinement effect and hydrogen proton from MPILs, albeit with mass transfer resistance produced by mesoporous channels. Further, the catalyst can be recovered using an external magnetic field and reused at least 10 times without a considerable decrease in its catalytic activity. Finally, alkene-modified Fe 3 O 4 nanoparticle-mediated mesoporous construction promotes a textural engineering approach to the development of novel mesoporous materials for other applications.

研究领域: 材料科学 · 催化化学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2020 · IF 3.99

Synthesis of penta-fold twinned Pd-Au-Pd segmental nanorods for in situ monitoring catalytic reaction

Guangliang Niu,Fangyan Liu,Yun Yang,Yunzhi Fu,Wei Wang

Multimetallic nanomaterials have many applications. The controlled synthesis of multimetallic nanomaterials is highly desired. We report a study on using penta-fold twinned (PFT) Au nanorods (NRs) as seeds to synthesize PFT Pd-Au-Pd segmental NRs. The results show that the different crystal structures of seeds, I − and cetyltrimethylammonium bromide (CTAB) significantly affect the deposition of Pd on seeds surface. The PFT Pd-Au-Pd segmental NRs showed excellent surface-enhanced Raman scattering (SERS) performance and improved catalytic activity. Our research is of great significance for the synthesis of similar nanostructures, and we also shown that PFT Pd-Au-Pd segmental NRs might have potential applications in studying the process of organic reaction.

研究领域: 材料科学 · 化学
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JOURNAL OF SUPERCRITICAL FLUIDS · 2023 · IF 3.9

On-line SFC-UV/Vis-MS using flow selection interfaces to monitor continuous flow single and sequential stage organic reactions in supercritical carbon dioxide

Wei Guo,Ben Li,Haijun Chi,Zhongliang Jiang,Liu Qing Wei,Edward D. Ramsey

Two flow selection interfaces have been developed for connecting single or linked reactors with on-line SFC equipped with UV/Vis diode-array (DAD) and mass spectrometer detectors coupled in series (SFC-DAD-MS). This process analytical technology system, enabled the study of reactions performed in supercritical fluid carbon dioxide (SF-CO 2 ). Each interface is designed to obtain on-line samples at different reaction progress points. Three single stage electrophilic annulation reactions performed in SF-CO 2 using aniline, indole and pyrrole as amine reactants to synthesize N-heterocyclic products within a stirred continuous flow reaction vessel containing montmorillonite K-10 catalyst were monitored. Also, both stages of a two step synthetic procedure conducted within two connected continuous flow reaction coil systems were monitored using on-line SFC-DAD-MS. The first step involved a Knoevenagel reaction in SF-CO 2 that provided a continuous feed to perform a second stage acetylation reaction. Use of on-line SFC-DAD-MS enabled early detection and characterization of unexpected by-products.

研究领域: 化学工程 · 分析化学
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Thermally enhanced biodegradation of benzo[a]pyrene and benzene co-contaminated soil: Bioavailability and generation of ROS

Mukhtiar Ali,Xin Song,Qing Wang,Zhuanxia Zhang,Meng Zhang,Xing Chen,Zhiwen Tang,Xin Liu

In this study, a set of comprehensive experiments were conducted to explore the effects of temperature on the biodegradation, bioavailability , and generation of reactive oxygen species (ROS) by thermally enhanced biodegradation (TEB) under benzene and BaP co-contaminated conditions. The biodegradation rates of benzene increased from 57.4% to 88.7% and 84.9%, and the biodegradation efficiency of BaP was enhanced from 15.8% to 34.6% and 28.6%, when the temperature was raised from the ambient temperature of 15 °C to 45 °C and 30 °C, respectively. In addition, the bioavailability analysis results demonstrated that the water- and butanol-extractable BaP increased with elevated temperatures. High enzymatic activities and PAH-RHD α gene in gram-positive bacteria favored the long-term elevated temperatures (30 and 45 °C) compared to gram-negative bacteria. Moreover, ROS species (O 2 •− and •OH) generation was detected which were scavenged by the increased superoxide dismutase and catalase activities at elevated temperatures. Soil properties (pH, TOC , moisture, total iron, Fe 3+ , and Fe 2+ ) were affected by the temperature treatments, revealing that metal-organic-associated reactions occurred during the TEB of benzene–BaP co-contamination. The results concluded that biodegradation of benzene–BaP co-contamination was greatly improved at 45 °C and that microbial activities enhanced the biodegradation under TEB via the increased bioavailability and generation and degradation of ROS.

研究领域: 环境科学 · 生物修复 · 微生物学 · 土壤化学
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JOURNAL OF MOLECULAR STRUCTURE · 2025 · IF 4.7

Three new molybdovanadates modified with different organic cations: Syntheses, Structure, efficient catalysis in the hydroxylation of benzene and oxidation of benzothiophene

Jie Wu,Xiaoyu Bai,Jianbo Yang,Siman Li,Hua Mei,Yan Xu

Phenol, as an important industrial raw material, the traditional three-step method for preparing phenol has drawbacks such as numerous by-products and difficulties in oxidation. In this regard, we use nitrogen-containing cations that can make conjugated π electrons more active to assemble with Keggin-type polyoxometalates with excellent redox properties, which can not only enable Keggin-type polyoxometalates to obtain the catalytic performance of activated benzene rings, but also increase their stability in organic solvents. Therefore, we synthesized three zero-dimensional compounds ((C 10 H 10 N 2 ) 2 [HPMo VI 9 V V 3 O 40 (FeH 2 O) 0.5 ].1.5H 2 O ( 1 ), (C 7 H 10 N 4 ) 2 [H 3 PMo VI 8 V V 4 O 40 ] ( 2 ), (C 9 H 8 N) 3 [PMo VI 8 Mo V 4 V IV 2 O 42 ] ( 3 )) through simple hydrothermal and solvothermal methods using different nitrogen-containing cations and molybdovanadate. Structural analysis indicates that these three compounds are structurally similar, each consisting of its own molybdovanadate anion and protonated organic counter cations. The experiment demonstrated that compound 3 had a yield of 11.2 % and a selectivity of 93 % for phenol at 60°C. To further explore the oxidation performance of the compound, we selected different sulfides for oxidation experiments and found that it could completely oxidize sulfur-containing substances (such as BT) at 90°C. This indicates that the idea of combining molybdovanadate and nitrogen-containing organic cations has a promising application prospect in the benzene hydroxylation and Sulfur oxidation.

研究领域: 无机化学 · 催化化学 · 有机反应 · 材料化学 · 环境化学
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