MICROPOROUS AND MESOPOROUS MATERIALS
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2020
·
IF 4.551
Yan Gao,Zhe Liu,Ruimin Gao,Guangfa Hu,Jianshe Zhao
In this work, a series of organic-inorganic hybrids based on N-alkyl-4-vinylpyridinium bromide ([C n VP]Br) with different carbon chain lengths and Dawson type heteropolyacid (HMoV) were designed and synthesized. And then the hybrids were loaded on mesoporous carbon aerogel (CA) with a high surface area of 1448.26 m 2 /g to form supported catalyst ([C n VP]MoV/CA), which used for extraction-oxidation desulfurization (EODS). Some techniques such as FT-IR, XRD , SEM, EDX , TEM, BET and XPS were used for characterization of the prepared materials. The test results show that the [C 6 VP]MoV/CA possesses the highest efficiency of 99.63% under the optimum conditions. Moreover, the catalysts can be efficiently reused with an efficiency of 85.39% after repeated use for 10 times, which confirms the industrial potential of the prepared [C 6 VP]MoV/CA.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Xue Shi,Yue Yu,Qiqi Yang,Xinlin Hong
Graphene oxide (GO) or reduced graphene oxide (RGO) is an excellent promoter to improve the photodegradation activity of a hybridized photocatalyst in advanced oxidation processes (AOPs). However, the identification of active sites remains a challenge due to the complexity of GO surface with different oxygen functionalities and defects coexisted. In this work, we synthesized different GO/polythiophene (GO/PTh) composites via in-situ polymerization of thiophene monomers on different GO supports with controlled content of oxygen functionalities such as carboxyl, hydroxyl and epoxide bonds. GO-COOH/PTh shows the highest performance in the degradation of methylene blue (MB) and phenol under visible light among all GO/PTh catalysts. We find the degradation rate is determined by the amount of hydroxyl free radicals ( OH) via the reaction of photoelectrons with H 2 O 2 . Different oxygen groups on GO surface results in different photoelectron conversion efficiency (η, the ratio of degradation rate to photocurrent). More importantly, we find that η correlates linearly with the amount of COOH in the catalysts, indicating COOH groups act as active sites for OH generation during photodegradation. This study provides a deep understanding of active sites for H 2 O 2 decomposition in photo-assisted Fenton-like systems over GO containing photocatalysts.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Xiao-Lu Sun,Zan Liu,Zhi-Lin Cheng
The Cu-intercalated layered h-BN/N-doped carbon-nanofiber composite films (PAN-Cu/ABN-CNFs) were successfully prepared by the combination of the electrospinning technique and the one-pot carbonization process, using the mixed solution of polyacrylonitrile (PAN) and Cu-intercalated activated boron nitride (Cu/ABN) as carbon precursor. A series of characterizations proved that the PAN-Cu/ABN-CNFs possessed the distinguished merits in the structure and composition, such as the pore feature of the micropore (0.076 cm 3 /g)-mesoporous (0.3582 cm 3 /g) structure, the structure of the exfoliated h-BN nanosheets , the low-coordination high-content N (11.65 at%) and the existence of self-reducing Cu nanoparticles (0.5 at%). For adapting the actual application, the mechanical properties of the PAN-Cu/ABN-CNFs were comprehensively evaluated, showing that the PAN-Cu/ABN-CNFs films had the robust tensile strength and bending properties as well as the desirable wear resistance. Furthermore, the selective adsorption desulphurization of the PAN-Cu/ABN-CNFs were examined by the selective adsorption removal of thiophene (TH) from the simulated oil, indicating that the optimum adsorption capacity of the fresh films was up to 78.38 mg/g in 800 mg/L initial concentration and the adsorption capacity after the four-time regeneration recycling still approached 74.894 mg/g. Finally, the adsorption kinetics , isotherm and thermodynamic studies suggested that the adsorption behavior of TH over the PAN-Cu/ABN-CNFs should be better described by the correlation coefficients of Avrami fractional-order kinetics and Liu isotherm, while the thermodynamic studies showed a favorable exothermic and spontaneous adsorption mechanism.
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高影响因子
Advanced Composites and Hybrid Materials
·
2021
·Vol. 4
·期 3
·459-468
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IF 5.693
Gu Hongbo,Gao Chong,Zhou Xiaomin,Du Ai,Naik Nithesh,Guo Zhanhu
In this work, in order to ameliorate the hydrophobic property and adsorption capacity of nanocellulose (NC) aerogel, the nanochitosan (NCS) and reduced graphene oxide (rGO) have been introduced into the NC aerogel to construct the NC/NCS/rGO nanocomposite aerogel by a hydrothermal method combined with freeze-drying method. The optimal conditions including the effect of NC and NCS weight percentages for preparation of NC/NCS/rGO nanocomposite aerogel with good porous microstructures and excellent adsorption capacities have been evaluated. The results demonstrate that the NC/NCS/rGO nanocomposite aerogel produced under the fabrication condition of 0.1 wt% NCS and 0.05 wt% NC exhibits a very low density of 9.3 mg cm −3 , a high hydrophobicity with a large water contact angle (115.26°) and the high adsorption capacities of 171.85 ± 3.02, 159.64 ± 1.83, 153.22 ± 2.92, 149.60 ± 6.26, 139.93 ± 3.69, 132.47 ± 3.45, 176.82 ± 4.66, 128.70 ± 0.69, and 120.34 ± 5.57 g g −1 to mineral oil, sesame oil, acetone, ethyl acetate, thiophene, pump oil, waste pump oil, kerosene, and ethyl alcohol, respectively. In addition, this aerogel adsorbent could efficiently and continuously remove/collect the oil from wastewater confirmed by a designed oil/water pump apparatus. As a consequence, this NC/NCS/rGO nanocomposite aerogel has a potential application in the oil and organic solvent adsorption. Graphical abstract
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Jiacheng Xu,Bo Zhang,Yongkang Lu,Leigang Wang,Wanyi Tao,Xiao Teng,Wensheng Ning,Zekai Zhang
Preparation of PdO/SiO 2 @graphene oxide (GO) hybrid aerogels were carried out sol-gel method combined with atmospheric drying technology to study their adsorption performance for thiophenics and compared with PdO/SiO 2 . Scanning electron microscope (SEM), N 2 adsorption-desorption isotherms, X-ray diffraction (XRD) analysis, X-ray photoelectron spectroscopy (XPS), and fourier transformation infrared spectroscopy (FT-IR) for samples were performed. The adsorption performance of PdO/SiO 2 @GO for thiophene were better than that of PdO/SiO 2 , attributed to that incorporation of GO increased the specific surface area and the Pd incorporation rate, where Pd 2+ ions acted as the π-complexation and sulfur-metal (S M) bond adsorption active centers, as well as GO adsorbed thiophene by the π-π stacking effect. The adsorption capacities of PdO/SiO 2 @GO-1.0 for thiophene (TH), benzothiophene (BT) and dibenzothiophene (DBT) were 8.89, 9.3 and 12.6 mg-S/g ads , respectively. The addition of GO in aerogels could improve the inhibition effect of toluene, cyclohexene and pyridine while decreased the inhibition effect of MTBE and H 2 O for the adsorption of thiophene, due to the π-π stacking effect and the hydrophobicity of GO, respectively. The adsorption process was spontaneous and exothermic, be well fitted by the apparent second-order kinetic model and dominated by chemical interaction. Pd/SiO 2 @GO-1.0 had a good solvent elution regeneration performance.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Luxia Yin,Jiacheng Xu,Bo Zhang,Leigang Wang,Wanyi Tao,Xiao Teng,Wensheng Ning,Zekai Zhang
A simple, low energy consumption and environment-friendly strategy was used to prepare highly dispersed CeO 2 /SiO 2 aerogel composites with different molar ratio of Si/Ce via sol-gel method and subsequently drying under the ambient pressure, in which the oxidation of Ce 3+ species into Ce 4+ species could be achieved by adding H 2 O 2 . The structural and surface properties of adsorbents were analyzed by XPS, XRD, FT-IR, Py-IR, SEM, XRF and N 2 adsorption-desorption isotherm. The adsorption desulfurization performances of CeO 2 /SiO 2 for thiophenic compounds from simulated gasoline and model aromatic products were investigated and compared by the breakthrough and batch adsorption experiments. As a result, the weak Lewis acid centers appeared on the surface of CeO 2 /SiO 2 . Among them, CeO 2 /SiO 2 with a Si/Ce of 25 performed best, the adsd by Duanpacity for TP from simulated gasoline (n-heptane) was 10.9 mg-S/g ads , followed by model aromatic products (benzene, 10.6 mg-S/g ads ; p-xylene, 10.1 mg-S/g ads ), however, the difference between them was slight, attributed to the formation of S-Ce bonding instead of C-Ce bonding. The very weak competitive adsorption of benzene and p-xylene with thiophene originated from the weak Lewis acid-base interaction. After the fourth solvent washing regeneration, the breakthrough adsorption capacity of regenerated CeO 2 /SiO 2 -25 still remained 60% of the fresh one. The equilibrium adsorption data of CeO 2 /SiO 2 -25 for thiophene were well fitted by Langmuir and Freundlich model, and the adsorption for TP was more favorable at the higher temperature. The adsorption process of CeO 2 /SiO 2 -25 was well fitted by pseudo-second-order kinetic model, which was spontaneous, endothermic and the freedom degree increased. The solvent (n-heptane, benzene, p-xylene) hardly influence the adsorption behavior of TP on CeO 2 /SiO 2 .
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WATER RESEARCH
·
2021
·
IF 11.236
Yao Pan,Dan Shan,Li-li Ding,Xu-dong Yang,Ke Xu,Hui Huang,Jin-feng Wang,Hong-qiang Ren
Our screening data revealed the threat macrolide antibiotics, especially azithromycin (AZN), posed to human health with its increasing occurrence in water environment. The electrochemical sensor based on molecularly imprinted polymer (MIP) is a promising platform that caters for the next generation of intelligent wastewater treatment plants (WWTPs) by virtue of its wide tolerance to water from all sources and in-situ monitoring. However, low initiation potentials of cross-linking monomers contributed by the electron-rich circumstance allowed them to usurp sites designed for functional monomers when electrically stimulated, leading to an unsatisfactory binding capacity. Another uncertainty is that multiple reaction sites of cross-linking monomers granted them complex polymerization routes and made it difficult to ensure the consistency of preparation. Serval monomers had been investigated with electrochemical tools and the performance of sensors constructed with these monomers were compared in this study. Based on the results, we proposed a protocol in which a novel functional monomer possessing a stronger electron-donating group, phenyl, was adopted to compete for the dominance in electropolymerization. Beyond that, the cross-linking monomer was modified with electron-withdrawing groups to raise its initiation potential. A monothiophene with a moderate initiation potential was also recruited as the linker to address the steric hindrance. In this way, polymerization proceeded in a specific order. It is worth mentioning that the Marangoni flow is an ideal tool to deal with the Coffee-ring deposition while drop-casting. The resulting sensor showed good performance with a limitation of detection (LOD) of 0.120 μM for AZN and a satisfactory selectivity, and the design can be applied to constructing sensors for a variety of macrolide antibiotics.
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PubMed
高影响因子
ENERGY & FUELS
·
2019
·
IF 3.021
Songjie Hua,Yuqi Hu,Liang Zhao,Liyuan Cao,Xiaoqin Wang,Jinsen Gao,Chunming Xu
For the effective removal of thiophene, a novel surface molecularly imprinted polymer (SMIP/MA@PCNS) was fabricated using porous carbon nanospheres (PCNS-5) as the support matrix and maleic acid (MA) as the functional monomer. Benefiting from the special amphiphilic properties of β-cyclodextrin as the carbon source, PCNS-5 exhibited good dispersion, uniform nanoscale sphere, and high specific surface area, which favored the rapid adsorption rate. Based on the intermolecular hydrogen bonds existing between carboxylic acid functional groups and thiophene, adsorption performances of different unsaturated polycarboxylic acids were investigated systematically. The results revealed that the optimal functional monomer was MA instead of the conventional methacrylic acid. Accordingly, SMIP/MA@PCNS was successfully applied to the direct removal of thiophene in the oil, reaching remarkable sulfur adsorption capacity (22.6 mg S g–1) within 120 min. Moreover, SMIP/MA@PCNS could selectively remove thiophene (16.2 mg S g–1) in the presence of structural analogues (3-methylthiophene, benzene, and cyclopentane) and exhibited an excellent regenerability with nice structural ability. These results indicated that SMIP/MA@PCNS possessed great promise in the desulfurization field.
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JOURNAL OF NANOPARTICLE RESEARCH
·
2019
·Vol. 21
·期 10
·1-13
·
IF 2.009
Liu Yanan,Yin Han,Xu Chengcheng,Zhuge Xingchen,Wan Jun
The organic dye pollutants are of more concern due to their toxic effects on human health, animals, and plants, and researchers thus should pay more attention to their removal. The nanocomposite photocatalysts of polythiophene-tungsten selenide/nitride-doped graphene oxide (PTh-WSe 2 /NG) were synthesized by a facile hydrothermal method. The catalytic activity of the nanocomposite was detected by degradation methylene blue (MB) under visible light. The as-prepared nanocomposite was characterized by scanning electron microscope (SEM), transmission electron microscope (TEM), X-ray powder diffraction (XRD), and Fourier transform infrared spectroscopy (FT-IR). The results showed that the photocatalytic performance of the composites was better than those of WSe 2 and PTh. This was mainly due to the PTh-WSe 2 /NG which contains excellent conductivity and charge separation characteristics of PTh, WSe 2 , and NG. They effectively inhibit the recombination of electron-hole pairs of PTh-WSe 2 /NG. 12.5 wt% PTh-WSe 2 /NG (12.5 wt% of PTh) was the most efficient catalyst, with the removal rate reaching to 94.8% of 1.0 × 10 –4 mol/L MB within 60 min of visible light irradiation.
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RSC Advances
·
2020
·Vol. 10
·期 2
·1015-1020
·
IF 3.119
Xing Wei,Yu-Jia Wang,Tie-Qiang Ren,Hai-Yan Wang,Min Wei
Hydrothermal synthesis is a typical method for the preparation of TS-1. In the current study, agitation was introduced during the crystallisation stage, and nano-sized TS-1 with little anatase TiO2 was successfully synthesised in a short time (1–8 h). Furthermore, under rotational crystallisation conditions, a series of TS-1 samples was prepared with different crystallisation times, and the products obtained were investigated as catalysts for the oxidative desulfurisation of thiophene from a model fuel. All samples were characterised utilising X-ray diffraction (XRD), scanning electron microscopy (SEM), N2-adsorption, ultraviolet-visible (UV-Vis) spectroscopy and Fourier-transform infrared (FT-IR) spectroscopy techniques. It was found that under rotational crystallisation conditions, nano-sized TS-1 could be synthesised in a short time that had improved efficiency for the oxidative desulfurisation reaction of thiophene in comparison with TS-1 synthesised by static crystallisation for 24 h.
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高影响因子
Materials Science and Engineering B-Advanced Functional Solid-State Materials
·
2019
·
IF 3.507
Zhiyuan Feng,Yekun Zhu,Qin Zhou,Ying Wu,Tinghua Wu
In this work, a magnetic WO 3 /Fe 3 O 4 catalyst was synthesized by grinding-calcination method and applied in the deep oxidative desulfurization of dibenzothiophene (DBT). The results showed that the as-synthesized WO 3 /Fe 3 O 4 had high catalytic efficiency for sulfur-removal. The content of WO 3 , amount of the catalyst, TBHP/DBT molar ratio and reaction temperature had significant effects on the desulfurization efficiency. The highest DBT conversion of 92.3% was achieved on 35% WO 3 /Fe 3 O 4 catalyst with the O/S ratio of 12:1 at 100 °C for 4.5 h. The results of this study revealed that WO 3 /Fe 3 O 4 catalyst has excellent potential for desulfurization properties because of its high catalytic activity and easy separation ability under an external magnetic field.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 16
·9912-9923
·
IF 10.733
Meidi Wang,Fusheng Pan,Hao Yang,Yu Cao,Hongjian Wang,Yimeng Song,Zean Lu,Mingze Sun,Hong Wu,Zhongyi Jiang
Inspired by the efficient facilitated diffusion via carrier proteins in biological membranes, facilitated transport membranes with synthetic carriers have been fabricated to enhance the separation performance via carrier-penetrant reversible reactions. Constructing highly ordered channels for the facilitated transport process in such membranes is favorable for achieving high efficiency, but reports are quite rare. Herein, crystalline porous covalent organic framework nanosheets (CONs) with regular pore structures, were used to load transition metal ions (typical carriers for unsaturated molecules) on their pore wall to enable a facilitated transport process in ordered channels. The physicochemical properties of the channels were elucidated by the CON microenvironments including the physical microenvironment (pore size) and the chemical microenvironment (carrier amount and carrier type). The microenvironment–performance relationship of the membranes was explored. The optimized facilitated transport membranes exhibited promising separation performance for gasoline desulfurization with a permeation flux of 21.6 kg m−2 h−1 and an enrichment factor of 6.29. Long-term operational stability and enhanced anti-swelling properties manifested superior stability of the resulting membranes.
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