MICROPOROUS AND MESOPOROUS MATERIALS
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2020
·
IF 4.551
Fangbin Fan,Xiaobin Nie,Chao Fan,Xiaojing Liang,Xiaofeng Lu,Yong Guo
In this paper, L (+)-Cysteine (L-Cys) and 5-norbornene-2-carboxylic acid (5-N-2-CA) were modified on the silica spheres by cross-linking polymerization and thiol-ene click reaction. The Cys-Si-NCA was characterized by scanning electron microscopy, nitrogen sorption porosimetry , thermogravimetric analysis and other characterization methods. The results indicated that the colume had a regular spherical shape with porous surfaces and particle sizes mainly ranging from 4.5 to 5.5 μm. The surface area of the Cys-Si-NCA microspheres was 328.68 m 2 g −1 , and their respective average pore size was 9.27 nm. Furthermore, the colume exhibited excellent stabilities and reproducibility. Experimental results demonstrate that this new stationary phase can facilitate the separation of sulfonamides, nucleosides and nucleobases compounds in hydrophilic chromatographic (HILIC) conditions. In addition to being able to attenuate the peak tailing of separation, it can also be used for quantitative analysis of creatinine in urine. We also give the temperature and pH ranges of separation on Cys-Si-NCA column. The successful synthesis of the Cys-Si-NCA stationary phase provides foundation for the application of this kind of materials in liquid chromatography (LC).
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GREEN CHEMISTRY
·
2020
·Vol. 22
·期 5
·1630-1638
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IF 9.48
Bin Zhang,Mark Douthwaite,Qiang Liu,Chao Zhang,Qifan Wu,Ruhui Shi,Peixuan Wu,Ke Liu,Zhuangqing Wang,Weiwei Lin,Haiyang Cheng,Ding Ma,Fengyu Zhao,Graham J. Hutchings
A novel method for the synthesis of MFI zeolites has been developed, which does not require any crystal seeds or solvent. The adaptability of this method was also evidenced; a series of ZSM-5 zeolites with differing Si/Al ratios (18∼∞) were synthesized, which to date, has been a challenge in the field of solvent-free synthesis. The materials were probed by in situ DRIFTS and 2D 27Al–19F HETCOR NMR spectroscopy, the results from which indicated that fluorine-containing species play a crucial role in the crystallization of ZSM-5. During the crystallization process F− anions coordinate with Al3+ cations, resulting in the formation of 6-coordinated “F–Al–O–Si” species. It is these intermediate species which drive the formation of tetrahedral [AlO4]− units in the zeolitic framework. The effectiveness of these materials as catalyst supports was subsequently assessed in the hydrogenation of levulinic acid and glucose, which exhibited a comparable performance to commercial ZSM-5. The simple, efficient and low-cost method presented herein provides an alternative approach for the green scaled-up synthesis of zeolites.
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Materials Science & Engineering C-Materials for Biological Applications
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2020
·
IF 5.88
Zhong-Hui Wang,Yun-Fei Zhang,Xiao-Wen Sun,Ying-Jie Li,You-Ming Zhang,Tai-Bao Wei,Hong Yao,Qi Lin
Paraquat, one of non-selective herbicides, is widely used in agricultural production. However, it can cause death of people or animals quickly owing to its fatal toxicity. In the present work, for efficient separation and removal of the paraquat, a concept “employ collaboration effect to enhance the Host-Guest interactions” was rationally introduced into the design of paraquat adsorbent material. According to this concept, a novel linear tri-pillar[5]arene-based acceptor molecule was synthesized. Interestingly, the acceptor shows outstanding adsorption properties for paraquat through the collaboration effect of the adjacent pillar[5]arene moieties in the linear tri-pillar[5]arene acceptor. Compared with other adsorbents such as activated carbon and single-pillar[5]arene-based adsorbent materials, the linear tri-pillar[5]arene acceptor shows higher adsorption rate for paraquat. Additionally, the linear tri-pillar[5]arene acceptor was applied to adsorb the commercial pesticide paraquat sample in water with adsorption rate of 98%. Therefore, the linear tri-pillar[5]arene acceptor could serve as a paraquat adsorbent material and convey greatly potential application in the field of removal of paraquat. The concept “employ collaboration effect to enhance the Host-Guest interactions” is a useful way for the development of adsorption materials.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Tengjiao He,Yonghou Xiao,Qidong Zhao,Mengxue Zhou,Gaohong He
Separation of carbon dioxide (CO2) from a CO2/ethylene (C2H4) mixture represents an important and challenging field in industrial applications. Selective adsorption has become an attractive option as an energy-saving and environmentally friendly CO2 capture technology. In this work, an ultramicroporous metal–organic framework (MOF) Qc-5-Cu was prepared by solution method and applied for the highly selective separation of CO2 from an C2H4 stream. The performance of Qc-5-Cu was evaluated by static and dynamic adsorption experiments. It was found that the single-component adsorption capacities of CO2 and C2H4 on Qc-5-Cu at 298 K and 1 bar were 2.48 and 0.74 mmol/g, respectively. The measured breakthrough curves further illustrate that Qc-5-Cu could effectively separate CO2 from the C2H4 stream for more than 10 cycles. The pore size of the obtained Qc-5-Cu was ∼3.3 Å, as characterized by nitrogen adsorption. The ultramicroporous structure of Qc-5-Cu benefits the separation of CO2, as evidenced by the selectivity values of the CO2/C2H4 binary mixture (1:99, v/v) based on the ideal adsorbed solution theory (SIAST ≈ 39.95 avg.), which are larger than some MOFs with open metal sites, owing to the weak interaction between organic ligands with high aromaticity and C2H4, as well as the porous screening effect of Qc-5-Cu on ethylene. The observed high selectivity, excellent stability, and regeneration performance demonstrate that Qc-5-Cu is a promising adsorbent for the separation of the CO2/C2H4 mixture.
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OPTICS AND LASER TECHNOLOGY
·
2020
·
IF 3.233
Gulgina Mamtmin,Nuerguli Kari,Renagul Abdurahman,Patima Nizamidin,Abliz Yimit
Optical waveguide (OWG) sensors are widely used in gas detection, and sensitive materials are the key factors affecting sensor performance. Herein, we report on a 5,10,15,20-tetrakis-(4-methoxyphenyl) porphyrin (TMP) deposited optical wave guide (OWG) sensor. The porphyrin solutions with different acidity were deposited on a K + -ion exchanged glass OWG surface by spin coating, to fabricate porphyrin film-coated OWG gas sensing devices. The effects of pH values of the porphyrin solution used to prepare the sensitive film on the sensing properties of these devices were investigated. The gas sensitive performances of these devices in response to analytes were compared. Among them, the sensing devices fabricated using original and acidic solutions of porphyrin exhibited significant responses to sulfide gases and ethanediamine, respectively. The sensing device prepared using an acidic solution has a good response to ethanediamine gas (response and recovery times of the sensor for 1 ppm of EDA (ΔI = 48) are 13 and 38 s, respectively). The RSD of the output light intensity is ±2.84, the signal to noise ratio (S/N) is 5.6. The device prepared using the original solution has an excellent response to sulfide gases (H 2 S, SO 2 ), and can detect low concentration levels (ppm) of sulfide gases. These sensing devices thus have the potential to be used in food quality testing and environmental monitoring.
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Nanoscale
·
2020
·Vol. 12
·期 6
·3846-3854
·
IF 6.895
Xiao Xiao,Shuang Liang,Yajie Zhao,Dayu Huang,Bengang Xing,Ziyong Cheng,Jun Lin
High treatment efficiency and low drug toxicity are two key factors in tumor therapy. The development of multifunctional drug carrier systems is of great significance for the diagnosis and therapy of tumors. Herein, a novel biodegradable treatment system based on zeolitic imidazolate framework-90 (ZIF-90) was designed in this study. This 5-FU@ZIF-90@ZnO (FZZ) drug delivery system achieves synergistic treatment with antineoplastic 5-fluorouracil (5-FU) and zinc oxide, and also has good dispersibility in the acidic tumor microenvironment (TME), which enables the drug to achieve pH-controlled delivery in acidic organisms. Interestingly, zinc oxide nanoparticles can play a dual role here. They can prevent the premature leakage of drugs under physiological conditions. Moreover, Zn2+ produced after the decomposition of nanoparticles can act as a therapeutic agent, overcoming the tumor resistance to 5-FU and regulating a series of physiological reactions to inhibit tumor growth. It is worth noting that the porous ZIF-90 is an emerging drug carrier with a relatively high drug loading rate of 39% in this study. Synergistic 5-FU and ZnO nanoparticles have achieved tumor inhibition and have shown high therapeutic biosafety. Thus, the FZZ core–shell nanoparticles are a potential pH-controlled drug release system that can be applied to tumor treatment.
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ACS Omega
·
2020
·
IF 2.87
Xing Huang,Guangcai Zhang,Lu Zhang,Qinhui Zhang
This work presented the microfluidic preparation of zeolite film in a capillary microchannel with different length-to-diameter ratios. In the quartz capillary with an inner diameter of 0.53 and 0.32 mm, Zeolite Socony Mobil-5 (ZSM-5) film was prepared by a continuous flow hydrothermal method. Considering the chemically inert surface of quartz capillary and the difficulty of preparing uniform and continuous zeolite film by conventional static synthesis, the ZSM-5 seed layer was precoated as active sites to induce film growth. The parameters of length-to-diameter ratio, seed coating, feed flow rate, and synthesis time were investigated. It revealed that the crystallinity of the ZSM-5 film was significantly affected by the capillary length-to-diameter ratio and seed coating in this flow system. The film morphology and thickness could be precisely controlled by adjusting the feed flow rate and synthesis time. This hydrogen form of the ZSM-5 (HZSM-5) film capillary microreactor was applied in the ketalization reaction of glycerol with acetone to produce solketal. The single-pass yield of solketal could reach ∼30% under mild conditions. This work provided a convenient stratagem of preparing zeolite catalytic coating or other support coatings in closed microchannels with a high length-to-diameter ratio and the potential application in valuable transformation of biomass glycerol.
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RSC Advances
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2020
·Vol. 10
·期 51
·30848-30857
·
IF 3.119
Shiben Wang,Lin Qi,Hui Liu,Kang Lei,Xuekun Wang,Renmin Liu
In this study, two series of 1,3,4-oxadiazole derivatives were designed and synthesized using the forced swimming test (FST) model to test the antidepressant activity of the target compound in vivo. Five compounds with potential activity were selected from the FST model to test affinity with 5-HT1A receptor in vitro. The results of the FST experiment showed that compound N-(3-((5-((4-chlorobenzyl)thio)-1,3,4-oxadiazol-2-yl)methoxy)phenyl)acetamide (10g) showed the best antidepressant activity (DID = 58.93, percentage decrease in immobility duration in FST), similar to the activity of positive drug fluoxetine. Compound 10g also exhibited the most potent binding affinity to 5-HT1A receptors (Ki = 1.52 nM). The results of the in vivo 5-HT concentration estimation in mice showed that compound 10g may have an effect on the brain. The experimental results of exploratory activity in mice showed that compound 10g did not affect spontaneous activity in the open-field test model. Molecular docking was used to study the binding mode of compound 10g and the 5-HT1A receptor. Compound 10g showed significant interactions with residues at the active site on the 5-HT1A receptor. The physicochemical and pharmacokinetic properties of the target compounds were predicted using Discovery Studio 2019 and ChemBioDraw Ultra 14.
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高影响因子
Nanomaterials
·
2020
·Vol. 10
·期 9
·1624
·
IF 4.324
Haian Xia,Jiahuan An,Weizi Zhang
The metal–support interaction (MSI) has a remarkable effect on the catalytic properties, but how to precisely modulate its degree remains a huge challenge. Herein, polyvinylpyrrolidone (PVP) with three different molecular weights (MWs) (24, 58, and 130 kDa) was used as a capping agent to fabricate Ag nanoparticles (NPs) supported on ZrO2. The physiochemical properties of the catalysts were characterized by X-ray diffraction (XRD), Transmission Electron Microscope (TEM), X-ray Photoelectron Spectroscopy (XPS), and Fourier transform infrared (FT-IR) techniques. The impacts of MSI on the catalytic activity and reaction kinetics for aerobic oxidation of 5-hydroxymethylfurfural (HMF) were investigated. The results showed that the introduction of PVP with various MWs could efficiently tailor the interfacial interactions and charge transfers (CT) among PVP, the support, and Ag NPs, thereby affecting the oxidation activity of HMF. The turnover number (TON) for HMF oxidation decreases in the order of unsupported colloidal Ag clusters > Ag/ZrO2(58,000) > Ag/ZrO2(130,000) > Ag/ZrO2(24,000) > Ag/ZrO2. The reason for this large difference in the catalytic activity for HMF oxidation is that various MWs of PVP result in a change of MSI, thereby facilitating CT from PVP to Ag metal sites. This study offers a new strategy for modulating MSI by varying the MW of capping agents, thereby tuning the catalytic properties in the oxidation of HMF.Keywords:metal–support interaction;molecular weight;capping agent;PVP;HMF oxidation
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AQUATIC TOXICOLOGY
·
2020
·
IF 4.346
Lei Peng,Chang Wang,Pingdeng Li,Bo Cheng,Yeli Hu,Yang Cheng,Qi Zheng
Halogenated dipeptides, 3, 5-di-I-tyrosylalanine (DIYA), have been identified as novel disinfection byproducts (DBPs), following chloramination of authentic water. However, little is known about their toxicity. Zebrafish embryos were used to assess the toxicity of novel iodinated DBPs (I-DBPs). Although DIYA did not exhibit high acute toxicity to embryonic zebrafish (LC 50 > 2 mM), it significantly inhibited pigmentation of melanophores and xanthophores on head, trunk and tail at 500 μM as determined by photographic analysis. Whereas N-phenylthiourea (PTU) as a pigment inhibitor did not inhibit development of yellow pigments. Colorimetric detection of melanin further confirmed these results. Quantitative real time polymerase chain reaction (qRT-PCR) measurements indicated that genes ( dct , slc24a5 , tyr , tyrp1a , tyrp1b , silva ) associated with the melanogenesis pathway were dramatically down-regulated following exposure to 500 μM DIYA. In addition, enzymatic activity of tyrosinase (TYR) decreased, also demonstrating that the underlying mechanism of hypopigmentation was attributed to the disruption of melanogenesis pathway. Transcription levels of xanthophore genes ( gch2 , bnc2 , csf1a , csf1b , pax7a and pax7b ) were also monitored by qRT-PCR assay. DIYA exposure up-regulated expression of gch2 and bnc2 , but not csf1 and pax7 . Tested DIYA analogues, brominated tyrosine was unlikely to inhibit pigmentation, indicating that the iodine substitution and dipeptides structure are of important structural feature for the inhibition of pigmentation. In this study, we observed that DIYA inhibited melanogenesis related genes, which might contribute to pigmentation defects. Moreover, as an emerging I-DBPs, the developmental toxicity of aromatic dipeptides should be further studied.
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JOURNAL OF FOOD PROTECTION
·
2020
·
IF 1.581
Hongying Li,Qiujin Zhu,Rui Chang,Ke Hu,Xuling Zhu,Aqi Xu,Shitao Xu,Pengyu Tang
ABSTRACT In order to reduce the health risks associated with red meat as listed by the World Health Organization, the work presented in this article aimed to elucidate the interaction between 5′-CMP–supplemented feed and N -glycolylneuraminic acid (Neu5Gc) in experimental animals in vivo. 5′-CMP was added to the diet of 90-, 180-, and 270-day-old Xiang pigs, and after 30 days, the Neu5Gc contents, physicochemical parameters, and free amino acid contents of muscle and internal viscera were measured by high-performance liquid chromatography coupled with fluorescence detection. The mechanism by which 5′-CMP affects Neu5Gc contents was investigated using molecular docking. Results show that 5′-CMP significantly decreased the Neu5Gc content in 180-day-old Xiang pigs ( P < 0.05) but had no effect on the Neu5Gc contents in 90- and 270-day-old Xiang pigs. Umami amino acids were significantly increased in 180-day-old Xiang pigs. In the 90- and 270-day-old pigs, histidine increased by 10.38 and 17.87%, respectively. The other free amino acids were either reduced or not affected. Moreover, the 5′-CMP–supplemented diet did not affect the physicochemical parameters of the longissimus muscle in the Xiang pigs. 5′-CMP could occupy almost all the sialyltransferase active-site residues but not His302 and showed inhibition of the sialyltransferase activity. The results provided an experimental basis for the subsequent reduction of Neu5Gc in red meat before slaughter.
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ChemCatChem
·
2020
·Vol. 12
·期 15
·3880-3889
·
IF 4.853
Xingling Zhao,Jun Xu,Yueying Chu,Guodong Qi,Qiang Wang,Wei Gao,Shenhui Li,Ningdong Feng,Feng Deng
Graphical Methane activation : Different types of Ga-CH 3 species were observed in methane activation on Ga-modified ZSM-5 zeolite, evidencing different pathways for heterolytic cleavage of C−H bond of methane. Two-dimensional solid-state NMR experiments provided detailed information on the location and local environment of the Ga-CH 3 species. Methane activation on Ga-modified ZSM-5 zeolites (Ga/ZSM-5) was studied by solid-state NMR spectroscopy. Two types of Ga species, namely highly dispersed oxides and cationic Ga species, were determined by 71 Ga QCPMG NMR. The activation of methane on Ga/ZSM-5 was explored by using 13 C and 1 H MAS NMR. Four types of Ga-CH 3 species along with Ga-OH groups were observed on Ga/ZSM-5, evidencing different pathways for heterolytic cleavage of C−H bond of methane. Two-dimensional (2D) 1 H- 1 H correlation NMR experiments provide detailed information on the location and local environment of the Ga-CH 3 species by correlating the protons in Ga-CH 3 with those in Ga-OH and other hydroxyls on zeolite. The structures of different Ga-CH 3 species were further determined by 2D 1 H- 13 C heteronuclear correlation NMR experiments, which were supported by theoretical calculations. The activation routes of C−H bond in methane were proposed on Ga/ZSM-5 zeolite.
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