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Catalysis Science & Technology · 2019 ·Vol. 9 ·期 24 ·7034-7044 · IF 5.726

Insight into the impact of Al distribution on the catalytic performance of 1-octene aromatization over ZSM-5 zeolite

Liwei Zhang,Huaike Zhang,Zhiqiang Chen,Qiang Ning,Suyao Liu,Jie Ren,Xiaodong Wen,Yong-Wang Li

To correlate the relationship between the Al distribution and the catalytic performance of long-chain olefin aromatization, several ZSM-5 zeolites with different Al locations and proximities were prepared via adjusting the hydrothermal synthesis conditions. Characterization by XRD, SEM and N2-adsorption indicated that all the as-prepared ZSM-5 zeolites exhibited high crystallinities, uniform morphologies and open channels. However, a great difference in the framework Al (AlF) positions was observed by 27Al MAS NMR and UV-vis-DRS of Co(II) ions, thus leading to the distinct acidity of various zeolites as determined by NH3-TPD and Py-IR. In 1-octene aromatization reaction, ZSM-5 catalysts exhibited significantly different catalytic performances and reaction pathways, which were closely related to the types and locations of the AlF atoms. The ZSM-5 zeolite catalyst with the most abundant single Al sites exhibited the lowest aromatics selectivity, while Al pairs in the framework were more favorable to the formation of aromatics. Moreover, the product distribution revealed that the Al pairs in the channel intersections of the ZSM-5 zeolite were responsible for the improved selectivity to heavy aromatics due to the fewer space restrictions; however, the Al pairs in the sinusoidal and straight channels with severe size restrictions suppressed the generation of bigger aromatics on the Al sites. This result provided a new potential method for precisely tailoring the catalytic selectivity in olefin conversion and upgrading the Fischer–Tropsch oil.

CAS / MDL: 71-43-2 111-66-0
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APPLIED SURFACE SCIENCE · 2019 · IF 5.155

Fabrication of the pod-like KCC-1/TiO2 superhydrophobic surface on AZ31 Mg alloy with stability and photocatalytic property

Meiling Zhang,Mingwu Zhao,Rongrong Chen,Jingyuan Liu,Qi Liu,Jing Yu,Rumin Li,Peili Liu,Jun Wang

It has been broadly studied to ensure the protection of magnesium alloy by superhydrophobic surface. In this work, the layered TiO 2 was prepared in response to the AZ31 Mg alloy by hydrothermal method and loaded wrinkled silicon dioxide (KCC-1) on the layer by electrostatic self-assembly to build a pod-like structure. After modification by stearic acid, the surface shows superhydrophobicity. The morphology, structure and composition of the surface were characterized by scanning electron microscope (SEM), the X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FT-IR), respectively. The anticorrosive effect of the superhydrophobic surface was investigated by detecting the electrochemical impedance spectroscopy and polarization curves in 3.5 wt% NaCl solution for a week. Superhydrophobic surfaces also exhibited chemical stability, physical stability and ultraviolet light tolerance. In addition, the TiO 2 containing in the film had a certain photocatalytic performance on decomposition of organic contaminants. Combining the self-cleaning property, the surface showed excellent adaptability to the outdoor environment.

CAS / MDL: 26062-79-3 78-10-4
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EUROPEAN JOURNAL OF INORGANIC CHEMISTRY · 2019 ·Vol. 2019 ·期 9 ·1212-1219 · IF 2.578

Recognition of Different Metal Cations by a trans-4-[4-(Dimethylamino)styryl]-1-methylpyridinium Iodide@Tetramethylcucurbit[6]uril Probe

Xin Yu Deng,Kai Chen,Ming-Dong Chen,Li Bin Lü,Zhu Tao

Graphical The probe responds to Cs + cations in alkali metal systems, Ba 2+ and Sr 2+ cations in alkaline earth metal systems; Eu 3+ , Tm 3+ , and Yb 3+ cations in lanthanide systems, and Cr 3+ , Fe 3+ , and Hg 2+ cations in systems containing transition and other metal cations, by obvious fluorescence quenching. Based on the study of a known host–guest inclusion complex comprising cucurbit[6]uril (Q[6]) and a hemicyanine dye, trans -4-[4-(dimethylamino)styryl]-1-pyridinium iodide ( t -DSMI), a water-soluble symmetric tetramethylcucurbit[6]uril (TMeQ[6]), was selected to construct a t -DSMI-based probe to test the response to various metal cations in neutral water. The experimental results revealed that the probe responded to Cs + cations in alkali metal systems, Ba 2+ and Sr 2+ cations in alkaline earth metal systems, Eu 3+ , Tm 3+ and Yb 3+ cations in lanthanide systems, and Cr 3+ , Fe 3+ and Hg 2+ cations in systems containing transition and other metal cations, via obvious fluorescence quenching.

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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Surface Coating Approach to Overcome Mucosal Entrapment of DNA Nanoparticles for Oral Gene Delivery of Glucagon-like Peptide 1

Tianqi Nie,Zhiyu He,Yang Zhou,Jinchang Zhu,Kuntao Chen,Lixin Liu,Kam W. Leong,Hai-Quan Mao,Yongming Chen

Oral delivery of nucleic acid therapy is a promising strategy in treating various diseases because of its higher patient compliance and therapeutic efficiency compared to parenteral routes of administration. However, its success has been limited by the low transfection efficiency resulting from nucleic acid entrapment in the mucus layer and epithelial barrier of the gastrointestinal (GI) tract. Herein, we describe an approach to overcome this phenomenon and improve oral DNA delivery in the context of treating type II diabetes (T2D). Linear PEI (lPEI) was used as a carrier to form complexes with plasmid DNA encoding glucagon-like peptide 1 (GLP-1), a common target in T2D treatments. These nanoparticles were then coated with a mixture of 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC) and 1,2-dimyristoyl-rac-glycero-3-methoxy poly(ethylene glycol)-2000 (DMG-PEG) to render the nanoparticle surface hydrophilic and electrostatically neutral. The surface-modified lPEI/DNA nanoparticles showed higher diffusivity and transport in the mucus layer of the GI tract and mediated high levels of transfection efficiency in vitro and in vivo. Moreover, these modified nanoparticles demonstrated high levels of GLP-1 expression for more than 24 h in the liver, lungs, and intestine in a T2D murine model after a single dose, as well as controlled blood glucose levels within a normal range for at least 18 h with repeatable therapeutic effects upon multiple dosages. Taken together, this work demonstrates the feasibility of an oral plasmid DNA delivery approach in the treatment of T2D through a facile surface modification to improve the mucus permeability and delivery efficiency of the nanoparticles.

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JOURNAL OF APPLIED TOXICOLOGY · 2019 ·Vol. 39 ·期 12 ·1640-1650 · IF 3.065

Acetaminophen-induced hepatocyte injury: C2-ceramide and oltipraz intervention, hepatocyte nuclear factor 1 and glutathione S-transferase A1 changes

Yicong Chang,Feng Wang,Yang Yang,Yuanyuan Zhang,Ishfaq Muhammad,Rui Li,Changwen Li,Ying Li,Chenxi Shi,Xin Ma,Beili Hao,Fangping Liu

Acetaminophen (APAP) is an antipyretic and analgesic, which is commonly associated with drug-induced hepatic injury. C2-ceramide plays a key role in mediating cell life activities, and oltipraz was extensively studied as a cancer chemopreventive agent. Glutathione S -transferase A1 (GSTA1) acts as a vital liver detoxification enzyme. Hepatocyte nuclear factor 1 (HNF-1) regulates various cellular signaling pathways. In this study, we investigated the effects of C2-ceramide and oltipraz on APAP-induced hepatocyte injury and the changes of HNF-1 and GSTA1. Results showed that C2-ceramide (6 μmol/L) exacerbated APAP-induced hepatocyte injury and caused a significant decrease ( P < .01) in HNF-1 and GSTA1 expressions. Meanwhile, GSTA1 content in supernatant was significantly increased ( P < .01). In contrast, oltipraz (8 μmol/L) reduced the injury and significantly elevated ( P < .01) HNF-1 and GSTA1 expressions while GSTA1 content in supernatant was significantly decreased ( P < .01). In conclusion, these findings revealed that C2-ceramide inhibited HNF-1 and GSTA1 expression and exacerbated hepatocyte injury, while oltipraz treatment results in the reduction of hepatocyte injury, and promoted HNF-1 and GSTA1 expression. Additionally, the changes in HNF-1 and GSTA1 were related to APAP-induced hepatocyte injury. These results were useful to investigate the mechanism of an antipyretic and analgesic drug combination.

CAS / MDL: 103-90-2
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JOURNAL OF CHEMICAL AND ENGINEERING DATA · 2019 · IF 2.298

Densities and Viscosities for the Ternary Mixtures of exo-Tetrahydrodicyclopentadiene (1) + Isopropylcyclohexane (2) + Methyl Laurate (3) and Corresponding Binaries

Wenqi Zhao,Yitong Dai,Haiyun Sun,Yongsheng Guo,Wenjun Fang

Biofuel mixed with fossil jet fuels has a lot of potential in applications of jet fuel extenders. To understand the fundamental properties of this typical mixture, measurements on densities and viscosities for the ternary model system of exo-tetrahydrodicyclopentadiene (1) + isopropylcyclohexane (2) + methyl laurate (3) and three corresponding binary mixtures have been implemented over the entire composition range at eleven different temperatures from 293.15 to 343.15 K. The excess molar volumes (VmE) and viscosity deviations (Δη) of binary mixtures were calculated and correlated by the Redlich–Kister equation, while the corresponding data of ternary mixtures were fitted to Nagata–Tamura, Cibulka, Singh, and Redlich–Kister equations. Furthermore, the variations of VmE and Δη were represented and discussed based on molecular interactions and structural effects in detail.

CAS / MDL: 111-82-0
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

Evaluation of seven chemical pesticides by mixed microbial culture (PCS-1): Degradation ability, microbial community, and Medicago sativa phytotoxicity

Haiyun Li,Yizhi Qiu,Tuo Yao,Yachun Ma,Huirong Zhang,Xiaolei Yang,Changning Li

Environmental problems caused by the large-scale use of chemical pesticides are becoming more and more serious, and the removal of chemical pesticides from the ecological environment by microbial degradation has attracted wide attention. In this study, using enrichment screening with seven chemical pesticides as the sole carbon source, a mixed microbial culture (PCS-1) was obtained from the continuous cropping of strawberry fields. The microbial community composition, degradation ability, and detoxification effect of PCS-1 was determined for the seven pesticides. Inoculation with PCS-1 showed significant degradation of and tolerance to the seven pesticides. Microbial community composition analysis indicated that Pseudomonas , Enterobacter , Aspergillus , and Rhodotorula were the dominant genera for the degradation of the seven pesticides by PCS-1. The concentration of the seven pesticides was 10 mg L −1 in hydroponic and soil culture experiments. The fresh weight, plant height, and root length of PCS-1-inoculated alfalfa ( Medicago sativa ) significantly increased compared with those of non-PCS-1-inoculated M. sativa . PCS-1 not only effectively degraded the residual content of the seven pesticides in water and soil but also reduced the pesticide residues in the roots, stems, and leaves of M. sativa . This study shows that PCS-1 may be important in environmental remediation involving the seven pesticides.

CAS / MDL: 55406-53-6 74610-55-2
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APPLIED ORGANOMETALLIC CHEMISTRY · 2019 ·Vol. 33 ·期 10 ·e5145 · IF 3.259

Synthesis of alcohol ester 12 in 1, 8-diazabicyclo [5.4.0] undec-7-ene (DBU)-based Self-separation catalytic system

Zhiguo Lv,Shuying Zhang,Zhenmei Guo,Xi Cheng,Jiaomei Wang,Chao Zhang

The synthesis of alcohol ester 12 is one of the valuable industrial processes, but it was impeded by poor separating property and recycling ability of the catalytic systems. Herein, four novel DBU-based basic ionic liquids (DBILs) of [BDBU]IM, [BDBU]OH, [ODBU]IM, [[ODBU]OH were synthesized successfully by introducing the alkyl chains of 1-bromobutane or 1-bromooctane to 1,8-diazabicyclo [5.4.0] undec-7-ene (DBU), and then, employing imidazole (IM − ) or hydroxide (OH − ) as counter ions. The above obtained four ionic liquids were applied in the synthesis of alcohol ester 12 in isobutyraldehyde (IBD)/aqueous media for the first time. Interestingly, after reaction, production of alcohol ester 12 can be self-separated from ionic liquids/water (ILs/W) catalytic system automatically. Furthermore, the self-separated ILs/W can be recycled and used in next catalytic reaction for at least 5 times without obvious loss of catalytic performance. In this work, the structure, purity, thermal stability and alkalinity of DBILs were characterized systematically. [BDBU]IM shows high alkalinity and thus enhances yield of 66.17%. From thermo gravimetric analyzer (TGA), [BDBU]IM also exhibits excellent thermal stability. So [BDBU]IM was chosen for the further studying. Furthermore, quantum chemistry is applied to calculate the interaction forces and electron energies of reactants by DFT, and the calculation results illustrate the feasibility of synthetic process of DBILs. The self-separation strategy of DBILS in this work may open up a new avenue for the clean synthesis of other industrial products.

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JOURNAL OF NANOBIOTECHNOLOGY · 2018 ·Vol. 16 ·期 1 ·1-14 · IF 5.294

Anti-ICAM-1 antibody-modified nanostructured lipid carriers: a pulmonary vascular endothelium-targeted device for acute lung injury therapy

Li Shujuan,Chen Li,Wang Guokang,Xu Lexing,Hou Shanshan,Chen Ziwei,Xu Xiaoling,Wang Xiaojuan,Liu Fuhe,Du Yong-Zhong

Background Acute lung injury (ALI) is a life-threatening clinical syndrome without effective treatment. Targeting delivery of glucocorticoid to lung shows potential efficacy for ALI based on their anti-inflammatory and anti-fibrotic properties, breaking through their clinical application limitation due to systemic side effects. This work was aimed to establish lung-targeted dexamethasone (DEX) loaded nanostructured lipid carriers (NLCs) with opposite surface charge and investigate their therapeutic effects on lipopolysaccharide (LPS)-induced ALI mice.Results The diameter of anionic anti-intercellular adhesion molecule 1 (anti-ICAM-1) antibody-conjugated DEX-loaded NLCs (ICAM/DEX/NLCs) and the cationic ones with octadecylamine (ODA) modification (ICAM/DEX/ODA-NLCs) was about 249.9 and 235.9 nm. The zeta potential of ICAM/DEX/NLCs and ICAM/DEX/ODA-NLCs was about − 30.3 and 37.4 mV, respectively. Relative to the non-targeted control and ICAM/DEX/ODA-NLCs, ICAM/DEX/NLCs exhibited higher in vitro cellular uptake in LPS-activated human vascular endothelial cell line EAhy926 after CAM-mediated endocytosis, and stronger in vivo pulmonary distribution in the ALI model mice. In vivo i.v. administration of ICAM/DEX/NLCs significantly attenuated pulmonary inflammatory cells infiltration, and the production of pro-inflammatory cytokine TNF-α and IL-6 in ALI mice. H&E stain also revealed positive histological improvements by ICAM/DEX/NLCs.Conclusion sICAM/DEX/NLCs may represent a potential pulmonary endothelium targeted device, which facilitate translation of DEX into clinical ALI treatment.

CAS / MDL: 50-02-2
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES · 2018 ·Vol. 34 ·期 3 ·350-357 · IF 1.248

Sustainable Synthesis of Hierarchically Porous Silicalite-1 Zeolite by Steam-assisted Crystallization of Solid Raw Materials Without Secondary Templates

Liu Xiaofang,Zeng Shangjing,Wang Runwei,Zhang Zongtao,Qiu Shilun

Hierarchical silicalite-1 zeolites were obtained from the direct conversion of a mixture of ground solid raw materials via a steam-assisted crystallization(SAC) method without involvement of any mesoscale template. Only a trace amount of water was necessary during the crystallization, implying that the amount of water can be dramatically reduced, which still offers easy separation and high yields. The simple procedure involved only grinding and heating, which not only saves resources and energy, but also significantly reduces the discharge of eco-friendly synthesis of zeolites for practical applications. Compared to conventional bulk silicalite-1, the nanosized hierarchical zeolites with MFI structure show enhanced removal capabilities for methylene blue owing to their hierarchical porosity.

CAS / MDL: 112926-00-8
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Catalysis Science & Technology · 2018 ·Vol. 8 ·期 18 ·4718-4725 · IF 5.365

Significantly increased catalytic activity of Candida antarctica lipase B for the resolution of cis-(±)-dimethyl 1-acetylpiperidine-2,3-dicarboxylate

Jiang-Wei Shen,Jia-Mei Qi,Xiao-Jian Zhang,Zhi-Qiang Liu,Yu-Guo Zheng

Candida antarctica lipase B (CALB) is a versatile and robust lipase with high activity and enantioselectivity in the resolution of alcohols and amines. Poor specific activity toward carboxylic esters that are branched or substituted in close proximity to the carboxyl group limits the application of CALB. In this study, a semi-rational engineering approach was successfully applied to tailor CALB for efficient synthesis of the moxifloxacin chiral intermediate through enzymatic resolution of cis-(±)-dimethyl 1-acetylpiperidine-2,3-dicarboxylate. The combinatorial active-site saturation test was performed on CALB and two key residue sites, 189 and 190, were identified in the determination of hydrolytic activity. The specific activity and catalytic efficiency (kcat/Km) of the best variant mut-I189K were increased by 286- and 193-fold, respectively, without impacting its enantioselectivity. With 0.1 g L−1 of purified mut-I189K loading, 1 M substrate was asymmetrically hydrolyzed with 49.9% conversion within 5 h, resulting in a space–time yield of 583.8 g L−1 d−1. These results demonstrated that mut-I189K is a competitive biocatalyst for large-scale preparation of the moxifloxacin chiral intermediate.

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CATALYSIS COMMUNICATIONS · 2018 · IF 3.463

Some catalytic characteristics of compositional catalysts of immobilized N-hydroxyphthalimide and metal salts in aerobic oxidation of 1-phenylethanol

Baojiao Gao,Coco Bi

N-hydroxyphthalimide (NHPI) was synchronously synthesized and immobilized on crosslinked polystyrene (CPS) microspheres via a short-cut of polymer reactions, obtaining the heterogenous catalyst. Some compositional catalysts were constituted by CPS-NHPI microspheres and metal salts, and they were used in the oxidation reactions of 1-phenylethanol with molecular oxygen as oxidant. Among four co-catalysts, vanadyl acetacetonate (VO(acac) 2 ), Co(OAc) 2 , CoCl 2 and Mn(OAc) 2 , the catalytic activity of VO(acac) 2 is the best although cobalt and manganese salts are conventional co-catalysts of NHPI. Under mild conditions, CPS-NHPI microspheres in combination with VO(acac) 2 can transform selectively 1-phenylethanol into acethenone with a conversion of 40%.

CAS / MDL: 1204-28-0
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