JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Kunlin Li,Jiayu Feng,Xingguang Hao,Xin Song,Changbin Zhang,Ping Ning,Kai Li
In this study, CuO@SiO 2 core-shell catalysts were successfully synthesized and applied to efficiently remove hazardous gaseous pollutant arsine (AsH 3 ) by catalytic oxidation under low-temperature and low-oxygen conditions for the first time. In typical experiments, the CuO@SiO 2 catalysts showed excellent AsH 3 removal activity and stability under low-temperature and low-oxygen conditions. The duration of the AsH 3 conversion rate above 90 % for the CuO@SiO 2 catalysts was 39 h, which was markedly higher than that of other catalysts previously reported in the literature. The considerable catalytic activity and stability were attributed to the protection and confinement effects of the SiO 2 shell, which resulted in highly dispersed CuO nanoparticles . Meanwhile, the strong interaction between the CuO core and SiO 2 shell further facilitated the formation of active species such as coordinatively unsaturated Cu 2+ and chemisorbed oxygen. The accumulation of oxidation products (As 2 O 3 and As 2 O 5 ) on the interface between the CuO core and SiO 2 shell and the pore channels of the SiO 2 shell is the main cause of catalysts deactivation . Furthermore, through combined density functional theory (DFT) calculations and characterization methods, a reaction pathway including gradual dehydrogenation (AsH 3 *→AsH 2 *→AsH*→As*) and gradual oxidation (2As*→As*+AsO*→2AsO*→As 2 O 3 ) for the catalytic oxidation of AsH 3 on CuO (111) surface was constructed to clarify the detailed reaction mechanism. The CuO@SiO 2 core-shell catalysts applied in this study could provide a powerful method for developing AsH 3 catalysts from multiple know AsH 3 removal systems.
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Asian Journal of Organic Chemistry
·
2022
·Vol. 11
·期 8
·e202200234
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IF 3.116
Yifei Ye,Yanglin Chen,Junzhe Huang,Jianmin Sun
Graphical A series of functionalized ionic liquids (ILs) immobilized on B-doped mesoporous SiO 2 catalysts were fabricated for effectively converting CO 2 into cyclic carbonates under metal-absent and cocatalyst-free conditions A series of functionalized ionic liquids (ILs) immobilized on B-doped mesoporous SiO 2 catalysts were fabricated for effectively converting CO 2 into cyclic carbonates under metal-absent and cocatalyst-free conditions. Functionalized imidazolium ILs were in-situ synthesized by Debus-Rdziszewski imidazole reaction. Among the prepared catalysts, 5B−SiO 2 −NH 2 −3−I catalyst owing to the synergistic effects of nucleophile, Lewis acid-base and hydroxyl hydrogen bond donors in the catalyst, presented the better catalytic activity for propylene epoxide to the product of propylene carbonate with 99% yield and selectivity at 110 °C and 2 MPa CO 2 . The catalyst also displayed moderate yield for various mono-substituent epoxides. Besides, the gradual decline in the product yield during consecutive runs could be easily refreshed by aqueous acidic solution washing.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Zitian Liu,Rongrong Qiang,Ligang Lin,Xuesong Deng,Xu Yang,Kongyin Zhao,Jing Yang,Xinyang Li,Wensong Ma,Meina Xu
Selective filtration of dyes and inorganic salts is a challenge for the treatment of textile wastewater containing high salt contents. In this study, selective separation performance of PI/SiO 2 nanofiltration (NF) membrane for dye/inorganic salt mixtures was substantially improved through directional modulation of its thermal treatment parameters after phase inversion. After thermal modification, the pore size, porosity and roughness were reduced, and the mechanical strength was improved. The PI/SiO 2 membrane under optimized thermally-modified conditions (M6, heat treatment conditions: 50 °C for 8 min) possessed high porosity of 79.95%. Besides, the thermally-modified PI/SiO 2 membrane revealed high water permeance of 152.87 L m −2 h −1 ·bar −1 with efficient rejection performance for a variety of typical dyes. In single dye filtration tests, the thermally-modified PI/SiO 2 membrane displayed high rejection (>90%) for Coomassie Brilliant Blue (CBB), Congo Red (CR), Trypan Blue (TB) and Direct Black 38 (DB 38), and exhibited excellent permeance (84.21–133.76 L m −2 h −1 ·bar −1 ). In addition, the thermally-modified PI/SiO 2 membrane could selectively separate dyes and inorganic salts. The membrane exhibited high dye rejection (>90%) and low inorganic salt rejection (<10%) for the filtration tests of CR + NaCl/Na 2 SO 4 and CBB + NaCl/Na 2 SO 4 mixed solutions (2 g L −1 ). In particular, the permeances of the thermally-modified PI/SiO 2 membrane (89.45–130.21 L m −2 h −1 ·bar −1 ) were higher than those of many contemporary NF membranes used for the same type of dye/inorganic salt separation. In conclusion, the present study presents a simple, inexpensive and effective thermal modification means, which shows great promise in the selective filtration of industrial dye wastewater.
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POLYMER COMPOSITES
·
2022
·Vol. 43
·期 8
·5087-5094
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IF 3.531
Hongbo Hou,Zejun Pu,Xu Wang,Rongli Zhu,Xianyong Li,Jiachun Zhong
In this study, WPU@SiO 2 nanoparticles were obtained by grafting waterborne polyurethane (WPU) on the surface of silicon dioxide (SiO 2 ). Then, WPU@SiO 2 nanoparticles were introduced into the matrix of polybutylene succinate (PBS) to prepare a series of PBS/WPU@SiO 2 composites. The dispersibility and interfacial compatibility of filler and matrix can be improved obviously by grafting a layer of WPU onto the surface of SiO 2 nanoparticles. The FTIR and TGA results showed that WPU was successfully grafted onto the surface of SiO 2 . According to polarizing microscope images, it is clear that the size of the pure PBS crystals is much larger than that of the PBS/WPU@SiO 2 , and a large number of crystals are evenly distributed in the PBS/WPU@SiO 2 composite. In addition, DSC and TGA results indicated that PBS/WPU@SiO 2 composite films show excellent thermal properties. Meanwhile, the initial thermal decomposition temperature of PBS/WPU@SiO 2 composite films is about 366–374°C. For the 10 wt% WPU@SiO 2 reinforced PBS-based composite films, the tensile strength reached the ultimate value (38.49 MPa), which is 32.04% higher than that of pure PBS. Based on its excellent mechanical and thermal properties, the PBS/WPU@SiO 2 composites have a broad application prospect in the field of biodegradable materials.
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Coatings
·
2022
·Vol. 12
·期 8
·1085
·
IF 3.236
Huan Luo,Hui Yang,Min Zhang,Taihong Chen
Traditional textile dyeing and finishing industries are two of the most important sources of high pollution, high energy consumption, and high emissions. Structural color, as a clean ecological staining method that does not require any dye or pigment, has received extreme attention from researchers. In this study, core-shell structures of SiO2@PDA microspheres were prepared by coating polydopamine (PDA) formed by rapid polymerization of dopamine (DA) on the surface of SiO2microspheres. Moreover, the structural colors of full chromatography were successfully prepared by vertical self-assembly on silk. The morphology and chemical structure of the prepared SiO2@PDA microspheres were studied by SEM and FT-IR, and the morphology and optical properties of the structured colored fabrics were characterized by SEM and material microscope. The different structural colors of the entire visible region were obtained by controlling the particle size of SiO2@PDA microspheres and the viewing angle of the SiO2@PDA photonic crystal, which are consistent with Bragg’s diffraction law. Since the SiO2@PDA photonic crystal has thermal stability, the prepared structural color fabric could remain highly saturated in color at temperatures up to 200 °C. This has a previously unreported high thermal stability on structural colors of silk. Therefore, the research work will demonstrate a structural color fabric that can prepare full chromatography with high thermal stability.Keywords:photonic crystal;structural color;polydopamine;self-assembly;full chromatography;high thermal stability
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POLYMER COMPOSITES
·
2022
·Vol. 43
·期 8
·5375-5389
·
IF 3.531
Tingting Wang,Li Yuan,Guozheng Liang,Aijuan Gu
A hybrid architecture system was developed via in situ formation of SiO 2 nanoparticles in the cavities of COOH-terminated hyperbranched aromatic polyester (CHBPE). Results show that SiO 2 nanoparticles can be successfully anchored in the cavities of CHBPE owing to the hyperbranched structure of CHBPE. The resulting CHBPE-SiO 2 system is applied to epoxy (EP) resins using 4,4′-diaminodiphenyl sulfone (DDS) as curing agent. Because –COOH groups in CHBPE-SiO 2 system can react with epoxy groups, the conversion of epoxy groups in EP/CHBPE-SiO 2 systems can be improved, and the strong interface interaction between EP matrix and CHBPE-SiO 2 can be realized. The resulting EP/CHBPE-SiO 2 composites have excellent mechanical property. When the contents of CHBPE-SiO 2 are 8%–20%, the impact strengths, the flexural strengths and the tensile strengths of EP/CHBPE-SiO 2 composites can reach 24–46 kJ/m 2 , 121–165 MPa and 57–71 MPa, respectively, which are 16.1–31.9-fold, 4.0–5.9-fold and 8.9–11.3-fold higher than those of pure EP, respectively. EP/16%CHBPE-SiO 2 composites have the optimal comprehensive mechanical property. The initial thermal decomposition temperature at 5 wt% weight loss ( T di ) and glass-transition temperature ( T g ) of EP composites can increase by 70–84°C and 30–43°C, respectively, after introducing 8%–20% CHBPE-SiO 2 . Moreover, the dielectric constants of EP composites with 8%–20% CHBPE-SiO 2 decrease by 3%–11% as compared to pure EP. The high dispersion of SiO 2 in EP/CHBPE-SiO 2 composite and the strong interface interaction between EP matrix and CHBPE-SiO 2 can contribute to the outstanding comprehensive property of EP/CHBPE-SiO 2 composite.
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Journal of Materials Research and Technology-JMR&T
·
2022
·
IF 6.267
Tian Hao,Yao Wang,Miaorong Zhang,Zhipeng Liu,Jixian Liu,Linjun Huang,Jie Li,Yao Peng,Jianguo Tang
The graphene oxide-silica, GO-SiO 2 (GS) nanoparticles synthesized by in-situ hydrolysis were grafted with block polymers polyethylene glycol (PEG) and low-molecular polyethylene terephthalate (LPET) using 3-isocyanatopropyltrimethicone (IPTES) as a bridge to prepare the additive GS-IPTES plus PEG-LPET (GSIP). This grafting process was confirmed by Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. The GSIP of various contents was used as reinforcing fillers to prepare PET/GSIP composite by melt blending. The crystallization and mechanical properties of the PET/GSIP composite were dramatically enhanced with the addition of small amounts of GSIP. Compared with pure PET, the crystallization temperature of PET/GSIP was increased by 41 °C at 1 wt.% addition of GSIP. Moreover, the highest tensile strength was 91.2 MPa and the highest modulus was 14.7 GPa at 0.8 wt.% addition. The crystalline and mechanical properties improvements were attributed to the synergistic effects of GS and block polymer chains.
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Chemosensors
·
2022
·Vol. 10
·期 5
·170
·
IF 4.229
Henggan Li,Feiming Li,Yipeng Huang,Linchun Zhang,Min Ye,Jingwen Jin,Xi Chen
In this study, CsPbBr3@SiO2perovskite nanocrystal composites (CsPbBr3@SiO2PNCCs) were synthesized by a benzyl bromide nucleophilic substitution strategy. Homogeneous halide exchange between CsPbBr3@SiO2PNCCs and Cl−solution (aqueous phase) was applied to the determination of Cl−in sea sand samples. Fast halide exchange with Cl−in the aqueous phase without any magnetic stirring or pH regulation resulted in the blue shift of the photoluminescence (PL) wavelength and vivid PL color changes from green to blue. The results show that the PL sensing of Cl−in aqueous samples could be implemented by using the halide exchange of CsPbBr3@SiO2PNCCs. A linear relationship between the PL wavelength shift and the Cl−concentration in the range of 0 to 3.0% was found, which was applied to the determination of Cl−concentration in sea sand samples. This method greatly simplifies the detection process and provides a new idea for further broadening PL sensing using the CsPbBr3PNC halide.Keywords:CsPbBr3perovskite nanocrystal composites;colorimetric sensing;photoluminescence wavelength shift;sea sand;Cl−
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Qian Zhang,Zhiwei Guo,Yujie Yang,Yanxiang Li,Chuanfang Yang,Wangliang Li
Surfactants in ultra-low sulfur diesel (ULSD) can improve the stability of the emulsified water droplet by forming a thin film at the water-fuel interface. Emulsified water droplets block the oil spray nozzle and break down the engine, which need to be removed. For colliding emulsified water droplets, surfactant film with high viscoelastic modulus provides an obstacle to their coalescence. Micro/nanosized-SiO 2 particles were added into ULSD to interrupt the arrangement of the surfactant film. After adding with 20 nm SiO 2 , the interfacial tension of water-monoolein-ULSD increased from 16.0 mN/m to 21.4 mN/m, and its viscoelastic modulus decreased from 17.1 mN/m to 10.9 mN/m, a decrease of 36.3%. It proved that the addition of nanosized SiO 2 into water-monoolein-ULSD system increased the interfacial tension and reduced the viscoelastic modulus of the monoolein film. However, after adding nanosized SiO 2 , the viscoelastic modulus of the water-PETO-B-ULSD layer had no significant changes. Therefore, we concluded that 20 nm SiO 2 disturbed the dense packing of monoolein as its adsorption to surfactants and the electrostatic repulsion force between them and the hydrophobic group, resulting in a decrease in elastic modulus . However, PETO-B had a complex branched structure leading to a loose packing, which had unoccupied adsorption sites and barely affected by the intrusion of 20 nm SiO 2 . Therefore, this research provided a strategy to add nanosized-SiO 2 into W/O emulsions containing monoolein-like surfactant to reduce its stability.
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GREEN CHEMISTRY
·
2022
·Vol. 24
·期 5
·2240-2248
·
IF 11.034
Yanlong Qi,Ruilin Feng,Shijun Liu,Long Cui,Quanquan Dai,Chenxi Bai
Functionalized monomers are of utmost importance in producing new polymers and smart materials. Herein, a two-step approach involving heterogeneous catalysis was developed to produce a functionalized monomer (2-vinylfuran) from bio-based furfural, giving an overall yield of 89%. Economic analysis suggests that this facile approach incurs much lower costs, and its practicality improves the availability of 2-vinylfuran. This is due to the delicate structure of the optimized 4Na5Ce/SiO2, where Na species are present at the oxygen vacancies of the ceria that protect the catalyst structure from collapse, and the catalyst consequently displays excellent performance. Density functional theory (DFT) calculations revealed that the reaction occurs on the Na and Ce species. The adsorption of a furan group onto Na led to side reactions, which were suppressed in the presence of Ce, resulting in higher selectivity. Finally, a polymer based on 2-vinylfuran was prepared, which shows good surface properties and thermodynamic stability.
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Wei Xie,Yulong Ju,Jian Zhang,Yiwen Yang,Yanbo Zeng,Hailong Wang,Lei Li
A magnetic Fe 3 O 4 @SiO 2 @MIPIL fluorescent sensor for the determination of imidacloprid (IMD) with high sensitivity and specificity was prepared through surface molecular imprinting technology on the surface of Fe 3 O 4 @SiO 2 by using dialkenyl ionic liquid (C) as a fluorescent polymer monomer . The as-prepared sensor was characterized by thermogravimetric, FT-IR, SEM, TEM, and nitrogen adsorption-desorption analysis. Results showed that IMD rapidly quenched the fluorescence of the sensor within 1 min and had an excellent linear relationship to the fluorescent quenching intensity of the sensor within the range of 1–1000 nM (IMD). The LOD was 0.3 nM (S/N = 3). The sensor had a specific response to IMD and was used to detect IMD in actual spiked environmental water and food samples with satisfactory result.
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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
·
2022
·Vol. 61
·期 18
·e202117201
·
IF 16.823
Jiaqi Si,Guofeng Zhao,Weidong Sun,Jincun Liu,Cairu Guan,Yong Yang,Xue-Rong Shi,Yong Lu
Graphical For the oxidative coupling of methane (OCM) reaction, the MnO x -Na 2 WO 4 /SiO 2 catalyst enriched with Q 2 units in the SiO 2 carrier achieves 23 % CH 4 conversion and 72 % C 2–3 selectivity at 660 °C. A large number of Q 2 units in MnO x -Na 2 WO 4 /SiO 2 is a trigger for markedly lowering the light-off temperature of the Mn 3+ ↔Mn 2+ redox cycle because of the easy formation of MnSiO 3 . Oxidative coupling of methane (OCM) catalyzed by MnO x -Na 2 WO 4 /SiO 2 has great industrial promise to convert methane directly to C 2–3 products, but its high light-off temperature is the most challenging obstacle to commercialization and its working mechanism is still a mystery. We report the discovery of a low-temperature active and selective MnO x -Na 2 WO 4 /SiO 2 catalyst enriched with Q 2 units in the SiO 2 carrier, being capable of converting 23 % CH 4 with 72 % C 2–3 selectivity at 660 °C. From experiments and theoretical calculations, a large number of Q 2 units in the MnO x -Na 2 WO 4 /SiO 2 catalyst is a trigger for markedly lowering the light-off temperature of the Mn 3+ ↔Mn 2+ redox cycle involved in the OCM reaction because of the easy formation of MnSiO 3 . Notably, the MnSiO 3 formation proceeds merely through the SiO 2 -involved reaction in the presence of Na 2 WO 4 : Mn 7 SiO 12 +6 SiO 2 ↔7 MnSiO 3 +1.5 O 2 . The Na 2 WO 4 not only drives the light-off of this cycle but also gets it working with substantial selectivity toward C 2–3 products. Our findings shine a light on the rational design of more advanced MnO x -Na 2 WO 4 based OCM catalysts through establishing new Mn 3+ ↔Mn 2+ redox cycles with lowered light-off temperature.
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危险品化学品经营许可证（带存储）