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CHINESE JOURNAL OF CHEMICAL PHYSICS · 2020 ·Vol. 33 ·期 6 ·749-756 · IF 1.067

Magnetic solid-phase extraction of phthalate esters from environmental water samples using fibrous phenyl-functionalized Fe3O4@SiO2@KCC-1

Zhou Xue-zheng,Yan Xiang-yang,Zhu Ling,Ma Ming,Dai Ya,Wang Chang-guo,Zhu Li-jun,Yu Ke-jie,Liu Shao-min

A new kind of phenyl-functionalized magnetic fibrous mesoporous silica (Fe 3 O 4 @SiO 2 @KCC-1-phenyl) was prepared by copolymerization as an efficient adsorbent for the magnetic extraction of phthalate esters from environmental water samples. The obtained Fe 3 O 4 @SiO 2 @KCC-1-phenyl showed monodisperse fibrous spherical morphology, fairly strong magnetic response (29 emu/g), and an abundant π -electron system, which allowed rapid isolation of the Fe 3 O 4 @SiO 2 @KCC-1-phenyl from solutions upon applying an appropriate magnetic field. Several variables that affect the extraction efficiency of the analytes, including the type of the elution solvent, amount of adsorbent, extraction time and reusability, were investigated and optimized. Under optimum conditions, the Fe 3 O 4 @SiO 2 @KCC-1-phenyl was used for the extraction of four phthalate esters from environmental water samples followed by high-performance liquid chromatographic analysis. Validation experiments indicated that the developed method presented good linearity (0.1–20 ng/mL), low limit of detection (7.5–29 µg/L, S / N =3). The proposed method was applied to the determination of phthalate esters in different real water samples, with relative recoveries of 93%−103.4% and relative standard deviation of 0.8%–8.3%.

研究领域: 环境科学 · 分析化学
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Polymer Chemistry · 2020 ·Vol. 11 ·期 35 ·5693-5700 · IF 5.342

Direct fluorination as a one-step ATRP initiator immobilization for convenient surface grafting of phenyl ring-containing substrates

Taijun He,Zhenyu Xing,Yixing Wang,Difeng Wu,Yang Liu,Xiangyang Liu

Generally, surface initiated-atom transfer radical polymerization (SI-ATRP) often suffers from the immobilization of the initiator on the surface-inert substrate. Developing an effective and versatile one-step method to anchor the priming sites while retaining the bulk properties of the substrate still faces challenges. In this work, direct fluorination is proposed to treat the benzene ring-containing substrate and the C–F introduced on the benzene ring can be used as an initiation site to achieve SI-ATRP. Computer and molecular simulation experiments have shown that the C–F added on the phenyl ring is more suitable for initiating ATRP than the C–F on the alkane chain. Thereafter, polyethylene terephthalate (PET) fabric was successfully grafted with fluorinated methacrylate polymer via direct fluorination-initiated ATRP, resulting in durable superhydrophobic properties, which demonstrated the practicability of the method. Furthermore, fluorination-initiated ATRP presents universality with other phenyl ring-containing polymeric substrates, such as aramid fiber, polyimide fiber and poly-p-phenylene benzobisoxazole fiber. Among them, the fluorinated aramid fiber can be grafted with hydroxyethyl methacrylate to obtain increased interfacial shear strength.

研究领域: 材料科学 · 高分子化学
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LIQUID CRYSTALS · 2019 · IF 3.078

Synthesis and mesomorphic properties of the nematic mesophase benzoxazole derivatives with big twist angle of difluoro-biphenyl unit

Qiang Weng,Longyan Duan,Pei Chen,Aiai Gao,Xinbing Chen,Zhongwei An

Modifying the position and numbers of lateral fluorine substituent is a common method to design and adjust the mesophase of liquid crystal compounds. Here, a series of 2-(2,2ʹ-difluoro-4ʹ-alkoxy-1,1ʹ-biphenyl-4-yl)-5-substituted benzoxazole with both non-polar (H, CH3) and polar (NO2) groups (coded as nPF(2)PF(2)Bx) is synthesised and characterised. All of the compounds show a conspicuous inter-ring twist angle of 38° compared with corresponding reference compounds I and II which are calculated by density functional theory method, and it is interesting to note that the final compounds nPF(2)PF(2)Bx show only nematic mesophase during heating or cooling. Meanwhile, the UV-vis absorption bands and photoluminescence emission peaks both display remarkable blue-shifted. The aforementioned results reveal that lateral difluoro substituents play a key role to stable the nematic mesophase by increasing the dihedral angle of biphenyl.

研究领域: 材料科学 · 化学 · 液晶
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Desalination and Water Treatment · 2024 · IF 1

Study on the fabrication and properties of polyphenylene sulfide (PPS) membrane and its application in VMD

Tingting Fan,Zhenhuan Li,Bowen Cheng

Polyphenylene sulfide (PPS) membranes were fabricated via a thermally induced phase separation method using mixed diluent of epsilon-caprolactam (CPL) and diphenyl sulfone (DPS). The effect of changing the CPL/DPS weight ratio on the structure and properties of prepared PPS membranes were investigated. The morphologies and performances of obtained PPS membranes were characterized by scanning electron microscopy, static water contact angles, mechanical strength, porosity, permeability and salt rejection rate. The characterized results showed that the morphologies of PPS membrane changed from cellular, bi-continuous to spherulitic structure with the increase of CPL/DPS mass ratio. PPS membranes exhibited the excellent stability and high salt rejection ratio in VMD experiments. The largest permeate flux stabilized at 10.63 L/(m 2 ·h 1 ) and the highest salt rejection remained above 98.9% after operating for 10 h.

研究领域: 材料科学 · 化学工程 · 膜技术
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Nature Communications · 2021 ·Vol. 12 ·期 1 ·1-8 · IF 14.919

Photo-fluorination of nanodiamonds catalyzing oxidative dehydrogenation reaction of ethylbenzene

Luo Zhishan,Wan Qiang,Yu Zhiyang,Lin Sen,Xie Zailai,Wang Xinchen

Styrene is one of the most important industrial monomers and is traditionally synthesized via the dehydrogenation of ethylbenzene. Here, we report a photo-induced fluorination technique to generate an oxidative dehydrogenation catalyst through the controlled grafting of fluorine atoms on nanodiamonds. The obtained catalyst has a fabulous performance with ethylbenzene conversion reaching 70% as well as styrene yields of 63% and selectivity over 90% on a stream of 400 °C, which outperforms other equivalent benchmarks as well as the industrial K−Fe catalysts (with a styrene yield of 50% even at a much higher temperature of ca. 600 °C). Moreover, the yield of styrene remains above 50% after a 500 h test. Experimental characterizations and density functional theory calculations reveal that the fluorine functionalization not only promotes the conversion of sp 3 to sp 2 carbon to generate graphitic layers but also stimulates and increases the active sites (ketonic C=O). This photo-induced surface fluorination strategy facilitates innovative breakthroughs on the carbocatalysis for the oxidative dehydrogenation of other arenes.

研究领域: 化学工程 · 材料科学 · 催化 · 有机化学
✓ 已验证 DOI PubMed 高影响因子
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2021 · IF 4.098

Efficient deep blue emission by 4-styrylbenzonitrile derivatives in solid state: Synthesis, aggregation induced emission characteristics and crystal structures

Ying Fang,Yuanyuan Meng,Chunming Yuan,Chunhui Du,Kun-Peng Wang,Shaojin Chen,Zhi-Qiang Hu

Organic fluorescent molecules with π-conjugated system have shown great importance in numerous applications including bioimaging and optoelectronics. Planar aggregation-induced emissive (AIE) organic compounds with efficient solid-state luminescence are rarely developed and urgently needed in various applications. In this work, highly planar 4-styrylbenzonitrile derivatives have been synthesized. Most of these compounds show strong AIE properties with hundred-fold fluorescent enhancement. Moreover, these molecules are deep blue emissive in solid state, exhibiting good to excellent fluorescence quantum efficiency. The single crystal analysis shows that adjacent molecules could form special J-type aggregation. The intramolecular rotations are efficiently restricted by various noncovalent interactions. These molecular arrangements could be essential for the observed strong emission in aggregated and solid state. This work has paved a new path to efficient AIE-active organic emitters with highly planar conformations from 4-styrylbenzonitrile structure.

研究领域: 有机化学 · 材料科学 · 光电子学
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CRYSTAL GROWTH & DESIGN · 2012 · IF 4.72

Phenazopyridine Cocrystal and Salts That Exhibit Enhanced Solubility and Stability

Qian Tao,Jia-Mei Chen,Lei Ma,Tong-Bu Lu

One phenazopyridine monohydrate (1·H2O), one cocrystal of phenazopyridine with phthalimide (2), and three salts of phenazopyridine with benzoic acid (3), 4-hydroxyphenylacetic acid (4), and scaaharin (5) were synthesized, and their structures were determined by single crystal X-ray diffraction. The results of dissolution experiments indicate that the solubility of phenazopyridine can be enhanced after the formations of cocrystal and salts, in which the apparent solubility value of 5is approximately 9 times as large as that of phenazopyridine in water, and the apparent solubility value of 4 is approximately 10 times as large as that of phenazopyridine hydrochloride (1·HCl) in 0.1 M HCl aqueous solution. The results of the stability study demonstrate that 2–5 are less hygroscopic than 1·H2O and 1·HCl at both 85% and 98% RH.

研究领域: 药学 · 化学
✓ 已验证 DOI 高影响因子
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Catalysis Science & Technology · 2019 ·Vol. 9 ·期 12 ·3270-3278 · IF 5.726

One-step green conversion of benzyl bromide to aldehydes on NaOH-modified g-C3N4 with dioxygen under LED visible light

Dan Liu,Chengwei Qiu,Minbo Li,Yanyu Xie,Lu Chen,Huaxiang Lin,Jinlin Long,Zizhong Zhang,Xuxu Wang

Kornblum oxidation (benzyl bromide to benzaldehyde) can be realized efficiently by NaOH-modified graphitic carbon nitride (g-C3N4). Different from the oxidation reaction carried out at high temperature using DMSO as an oxidant, our reaction is eco-friendly because it is carried out at room temperature under LED light irradiation using molecular oxygen as an oxidant, which avoids the problems of toxicity, pollution and purification. Alkali treatment leads to the surface deprotonation of g-C3N4 to form NaOH-modified g-C3N4 (Na/g-C3N4). The modifications of the electronic structure and surface chemical environment of g-C3N4 facilitate light absorption and formation of ˙O2− and therefore make the conversion of benzyl bromide reach up to 99%. This work demonstrates a green and sustainable route for benzaldehyde production and the superiority of g-C3N4 for organic syntheses.

研究领域: 有机化学 · 环境科学
✓ 已验证 DOI 高影响因子
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CHEMOSPHERE · 2022 · IF 8.943

Photochemical transformation of hexachlorobenzene (HCB) in solid-water system: Kinetics, mechanism and toxicity evaluation

Zhengnan Tu,Yumeng Qi,Ruijuan Qu,Xiaosheng Tang,Zunyao Wang,Zongli Huo

As one of the first batch of persistent organic pollutants (POPs) included in Stockholm Convention , hexachlorobenzene (HCB) has attracted great attention because of its wide occurrence and great environmental risks. Considering the easy adsorption of HCB on solids and the complexity of natural particles, we systematically investigated the photodegradation of HCB on the surface of silica gel (SG) in aqueous solution in this work to reveal its fate in natural waters. Under mercury lamp irradiation, more than 90% of HCB loaded on SG could be removed after 240 min. Moreover, the effects of solution pH and water constituents were examined, and results showed that the presence of NO 2 − , NO 3 − , Fe 3+ and humic acid (HA) significantly inhibited the reaction due to the scavenging of ROS and/or competitive absorption of light. According to radical quenching experiments and electron paramagnetic resonance (EPR) spectra, hydroxyl radicals and singlet oxygen generated on the surface of SG could participate in the transformation of HCB, but •OH played a dominant role. Based on products identified by high performance liquid chromatography-mass spectrometry (HPLC-MS) and gas chromatography-mass spectrometry (GC-MS), two main pathways were proposed for the removal of HCB, including dechlorination and hydroxylation which represent direct and indirect photodegradation, respectively, and the occurrence of these two reactions was further supported by density functional theory (DFT) calculations. From the quantitative analysis of penta-chlorobenzene, it was estimated that dechlorination and hydroxylation contributed to approximately 44.4% and 55.6% of initial HCB degradation, respectively. Furthermore, toxicity predictions by the ecological structure–activity relationship model (ECOSAR) suggested that the toxicity of HCB was decreased in the photodegradation process. This study would provide important information for understanding the photochemical transformation mechanism of HCB at the solid/water interface.

研究领域: 环境科学 · 化学
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FOOD CHEMISTRY · 2022 · IF 9.231

Degradation, migration, and removal of trichlorfon on harvested apples during storage at room temperature

Changjian Li,Kexin Chi,Hang Yu,Yahui Guo,Weirong Ya,He Qian

Dissipation of an organophosphorus pesticide, trichlorfon, in natural and waxed apples during storage was studied. The results showed that the trichlorfon content in natural and waxed apples decreased by 85% and 64%, respectively, during storage. The morphology of the surface film was dense and regular, which resulted in a higher water vapor resistance and a lower respiration rate in the waxed apples. This indicates that waxing affected the dissipation of pesticide residues in the apple storage environment, increasing food safety risk. Ozone was used to remove the residual pesticides on the apple surface. The trichlorfon degradation rate reached 73%. The ozone treatment had no effect on the surface color of the apple, which means that the fruit can be pre-treated with ozone prior to waxing or storage.

研究领域: 食品安全 · 植物保护 · 环境科学
✓ 已验证 DOI PubMed 高影响因子
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DALTON TRANSACTIONS · 2021 ·Vol. 50 ·期 26 ·9076-9087 · IF 4.39

Construction of MOF-shell porous materials and performance studies in the selective adsorption and separation of benzene pollutants

Yu Qiao,Na Lv,Dong Li,Hongji Li,Xiangxin Xue,Wei Jiang,Zhanlin Xu,Guangbo Che

Metastable Cu2O is an attractive material for the architectural design of integrated nanomaterials. In this context, Cu2O was used as the sacrificial agent to form the core–shell structure of Cu2O@HKUST-1 by in situ growth technology. The MOFs with BOPs adsorption property were gathered together by a Cu2O etching method, and the hollow structure of the HKUST-1 shell material with fast BOP adsorption was successfully constructed. The adsorption experiments showed that the HKUST-1 shell has a good adsorption effect on nitrobenzene pollutants in wastewater. The investigation of various factors affecting the adsorption, thermodynamic and kinetic equations was carried out. The adsorption equilibrium was reached within 30 min, and the maximum adsorption capacity was 94.67 mg g−1 at 298 K. The adsorption capacity of nitrobenzene by the HKUST-1 shell is in good agreement with the Freundlich model and the second-order kinetic model. The possible mechanism of adsorption of nitrobenzene by the HKUST-1 shell was discussed. The experimental results suggested that Cu-BTC materials have potential applications for wastewater treatment involving benzene pollutants.

研究领域: 材料科学 · 环境科学
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ANALYTICA CHIMICA ACTA · 2022 · IF 6.911

Triphenylbenzene functionalized polyhedral oligomeric silsesquioxane fluorescence sensor for the selective analysis of trace nitrofurazone in aquatic product and cosmetics

Simin Huang,Peipei Zhou,Yufei Hu,Gongke Li,Ling Xia

Nitrofurazone (NFZ) is carcinogenic and mutagenic to human in long-term ingestion, and it is prohibited to be added in food. In this work, a novel triphenylbenzene (TPB) functionalized fluorescent hybrid porous polymers (POSS@TPB) was constructed by using polyhedral oligomeric silsesquioxane (POSS) as the rigid group and TPB as the core unit of high fluorescence. The morphology and physicochemical properties of POSS@TPB were characterized in detail. Moreover, the synergistic effect of inner filter effect and photoinduced electron transfer is verified by experimental and simulation results. After condition optimization, a NFZ analysis method based on POSS@TPB probe was established with a linear range of 0.4–16.5 mg/L and a detection limit of 0.13 mg/L. In addition, the fluorescent probe has good stability, anti-interference and considerable reusability. At the same time, the selective analysis of trace NFZ in aquatic product and cosmetics was carried out with satisfied recoveries of 87%–110.6% and relative standard deviation less than 4.1%. And the results were verified by high-performance liquid chromatography method. Overall, this fluorescence sensor has excellent performance in NFZ analysis, which provides a broad application prospect for the repeatable and selective residue NFZ analysis in aquatic product and cosmetics.

研究领域: 食品安全 · 分析化学 · 环境科学
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