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Molecular Catalysis · 2019 · IF 2.938

Ru/HZSM-5 as an efficient and recyclable catalyst for reductive amination of furfural to furfurylamine

Chenglong Dong,Hongtao Wang,Haochen Du,Jiebang Peng,Yang Cai,Shuai Guo,Jianli Zhang,Chanatip Samart,Mingyue Ding

Furfurylamine converted from biomass-based platform molecules furfural was proven a significant intermediate in the synthesis of different valuable compounds. The combination of Ruthenium with HZSM-5 was acted as an excellent selective and reusable catalyst for the reduction amination of furfural with environmentally friendly ammonia and hydrogen. Incorporation of Ru species into HZSM-5 had a significant enhancement to the acid sites of Ru/HZSM-5. The Ru/HZSM-5(46) catalyst with optimized acid sites and interaction of the Ru-O-Al bond displayed an excellent catalytic performance, producing 76 % yield of furfurylamine at only 15 min, and could be recycled five times without loss of performance. Synergistic effect between RuO 2 and metallic Ru in the Ru/HZSM-5 catalyst facilitated the reduction amination of furfural.

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JOURNAL OF POLYMER RESEARCH · 2019 ·Vol. 26 ·期 12 ·1-12 · IF 1.53

Synthesis and properties of processable poly(benzimidazole-imide)s based on 2-(3-aminophenyl)-5-aminobenzimidazole

Jiao Yang,Chen Guofei,Zhou Haijun,Zhang Feng,Chen Xiaoqi,Li Yantao,Xiao Xueshan,Fang Xingzhong

A series of poly(benzimidazole-imide)s (PBIPIs) derived from different dianhydrides and 2-(3-aminophenyl)-5-aminobenzimidazole ( m -BIA) were synthesized via thermal imidization to form flexible films. This series of PBIPIs showed great T g s ranging from 296 to 484 °C, excellent thermal stability performed in 5% weight loss temperatures ( T d5% s) of 502–529 °C in N 2 and good mechanical properties (tensile strengths of 89–127 MPa, tensile moduli of 2.9–4.1 GPa and elongations at break of 3.9–6.9%). Compared with PIs derived from 6-amino-2-(4-(4-aminophenoxy)phenyl)-1H-benzimidazole ( p -BIODA), m -BIA based PBIPI films exhibited higher T g , and better solubility. Besides, the thermoplastic PBIPI resin (PI-6-PA) derived from 2,2-bis[4-(3,4-dicarboxyphenoxy)phenyl]propane dianhydride (BPADA) and m -BIA exhibited good melt processability with high T g of 273 °C, melt flow index (MFI) of 7.76 g/10 min, minimum complex viscosity of 11.9 × 10 3  Pa·s at 402 °C and low melt viscosity ratio of 2.46 at 400 °C.

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Asian Pacific Journal of Tropical Medicine · 2019 · IF 1.772

Feng-liao-chang-wei-kang is synergistic with 5-fluorouracil in inhibiting proliferation of colorectal cancer

Ni Pan-Li,Tian Shu-Hong,Yang Zhao-Xin,Zhang Jun-Qing,Yang Fan,Zhong Li-Fan,Gan Lian-Fang,Huang Mian-Qing,Huang Ling

Objective: To explore the effect of Feng-liao-chang-wei-kang ( FLCWK ) on acute and chronic gastroenteritis, synergistic effect on the growth inhibitory effect with 5-fluorouracil (5-FU) on colorectal cancer and its underlying mechanisms. Methods: In the in vitro study, HT-29 cells were divided into 5-FU alone, FLCWK alone and coadministration groups. The MTT assay was used to analyze the proliferation of HT-29 cells at 24 h. Flow cytometry was used to observe the apoptosis, cycle of colorectal cancer HT-29 cells at 24 h. In the in vivo experiment, The subcutaneous transplantation tumor model of colorectal cancer HT-29-Luc was established with nude mice. All mice were randomly divided into 5-FU alone, FLCWK alone and coadministration groups according to body weight. During administration, the Interactive Video Information System small animal live imaging system was used to monitor the growth of subcutaneous transplantation in nude mice. The model of colitis-associated colorectal cancer (CACC) was established with BALB/c mice. BALB/c mice were randomly divided into the normal control group, the model control group, and the FLCWK group. At the end of the administration, the pathological status was detected by HE staining. Cell apoptosis of tumor tissue tumor and colon tissues were observed by TUNEL staining and TUNEL green fluorescence. The protein expression of Caspase 3, p-STAT3, Bcl-2, Bax and P-gp in tumor tissues tumor and colon tissues were tested by using immunohistochemical assay. Results: FLCWK and 5-FU coadministration suppressed HT-29 cell viability and induced S phase arrest and apoptosis compared to treatment with 5-FU alone. Furthermore, compared to treatment with 5-FU alone, coadministration of FLCWK and 5-FU obviously reduced tumor volume and weight and induced apoptosis through decreasing p-STAT3 and P-gp and increasing Caspase 3 protein expression in a murine xenograft tumor model. Moreover, the result revealed decreased number and size of tumors following FLCWK protective administration, downregulated p-STAT3 and Bcl-2 levels and upregulated Bax and Caspase 3 expression in mice with CACC. Conclusions: FLCWK has synergistic effects with 5-FU on colorectal cancer by suppressing the STAT3 pathway and downregulating P-gp expression. Furthermore, FLCWK administration suppresses CACC tumorigenesis by inhibiting the STAT3 pathway.

CAS / MDL: 67-68-5 298-93-1
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Iranian Journal of Basic Medical Sciences · 2019 · IF 1.854

Synthesis and evaluation of a prodrug of 5-aminosalicylic acid for the treatment of ulcerative colitis

Yan Yan,Fengling Ren,Pengchong Wang,Ying Sun,Jianfeng Xing

Objective(s): This study is aimed to design and synthesize a prodrug of 5-aminosalicylic acid and evaluate its ameliorative effect on experimental ulcerative colitis (UC). Materials and Methods: 5-Aminosalicylic acid-alanine (5-ASA-ALA) was synthesized and characterized. Its stability study was conducted in rat plasma and in the gastrointestinal tract environment, its transport characteristic was assessed using the Caco-2 cells. Its colon-targeting property was evaluated by the pharmacokinetic study, and incubation studies. A series of indicators were used to investigate its therapeutic effect on experimental colitis, including the survival rate and body weight of mice, the disease activity index (DAI), the colonic damage score and colon index, the myeloperoxidase (MPO) activity and the levels of malondialdehyde (MDA), total superoxide dismutase (SOD), glutathione (GSH) and glutathione peroxidase (GSH-Px) in colonic tissues. Results: 5-ASA-ALA was barely absorbed in the Caco-2 monolayer or into the rat blood. It was remarkably stable when incubated in the upper gastrointestinal tract, while gradually hydrolyzed in the colon of rats. When orally administered to mice, 5-ASA-ALA had significantly greater therapeutic effect on colitis than the positive control. Conclusion: 5-ASA-ALA is demonstrated to be a promising oral colon-targeting prodrug of 5-ASA and has potential application in UC treatment.

CAS / MDL: 57-09-0 9014-81-7
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ACS Omega · 2019 · IF 2.584

Novel Amino-pillar[5]arene as a Fluorescent Probe for Highly Selective Detection of Au3+ Ions

Jun-Li Yang,Yun-Han Yang,Yu-Peng Xun,Ke-Ke Wei,Jie Gu,Mei Chen,Li-Juan Yang

A novel fluorescent probe, amino-pillar[5]arene (APA), was prepared via a green, effective, and convenient synthetic method, which was characterized by nuclear magnetic resonance (NMR), infrared (IR), and high-resolution mass spectrometry. The fluorescence sensing behavior of the APA probe toward 22 metal ions in aqueous solutions were studied by fluorescence spectroscopy. The results showed that APA could be used as a selective fluorescent probe for the specificity detection of Au3+ ions. Moreover, the detection characteristics were investigated by fluorescence spectral titration, pH effect, fluorescence competitive experiments, Job’s plot analysis, 1H NMR, and IR. The results indicated that detection of Au3+ ions by the APA probe could be achieved in the range of pH 1–13.5 and that other coexisting metal ions did not cause any marked interference. The titration analysis results indicated that the fluorescence intensity decreased as the concentration of Au3+ ions increased, with an excellent correlation (R2 = 0.9942). The detection limit was as low as 7.59 × 10–8 mol·L–1, and the binding ratio of the APA probe with Au3+ ions was 2:1. Therefore, the APA probe has potential applications for detecting Au3+ ions in the environment and in living organisms.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

Controlled fabrication of mesoporous ZSM-5 zeolite-supported PdCu alloy nanoparticles for complete oxidation of toluene

Jiaqin He,Dongyun Chen,Najun Li,Qingfeng Xu,Hua Li,Jinghui He,Jianmei Lu

Mesoporous ZSM-5 zeolite-supported PdCu alloy nanoparticle catalysts are synthesized via a facile and environmentally friendly method. The mesoporous structure is formed through the loss of carbon black particles encapsulated by zeolite crystals during calcination. The ZSM-5-supported PdCu nanoparticles are shown to possess mesoporous structure, evenly distributed PdCu alloy nanoparticles, and excellent catalytic performance in toluene oxidation. The mesoporous structure of the ZSM-5-supported PdCu nanoparticles provides a large specific surface area and pore size, resulting in numerous accessible active sites. The alloying of Pd with Cu both increases the catalytic performance of the catalyst and lowers its cost. Overall, the catalyst with a Pd/Cu ratio of 8:2 showed the highest catalytic activity of the fabricated materials, achieving 100 % toluene conversion at 160 °C. The mechanism of toluene oxidation over these catalysts can be explained by the Mars–van Krevelen model.

CAS / MDL: 4499-86-9 78-10-4
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JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY · 2019 ·Vol. 143 ·期 1 ·609-618 · IF 2.471

Thermal decomposition behavior, kinetics, thermal safety and burning characteristics of guanidinium-5-aminotetrazole (GA) based propellants

Cao Chengyang,Zhang Dan,Lu Song,Liu Changcheng

Guanidinium-5-aminotetrazole (GA) was synthesized by mixing 5-aminotetrazole (5-AT) and guanidine carbonate in heated deionized water. The composite propellants containing GA and differential oxidizers (Sr(NO 3 ) 2 , KNO 3 , NaNO 3 ) were prepared, and its structural characteristics, thermal decomposition behavior, kinetics, thermal safety and burning characteristics were investigated. The thermal analysis results showed that the decomposition of GA based propellants could be separated into five stages, consisting of one phase change reaction, one exothermic reaction and three endothermic reactions. The reaction mechanisms of each decomposition stage were also researched and considered it was following reaction order models. The thermal safety evaluations were conducted using the obtained related parameters of the exothermic reaction. Combined with the burning characteristics measurement results, GA coupled with Sr(NO 3 ) 2 represented a higher thermal safety and more stale combustion process than other two propellant samples, which is also act as a promising formulation to substitute 5-AT based propellant in fire-fighting area.

CAS / MDL: 4418-61-5 593-85-1
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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

Selective Hydrodeoxygenation of 5-Hydroxymethylfurfural to 2,5-Dimethylfuran over Alloyed Cu−Ni Encapsulated in Biochar Catalysts

Changhui Zhu,Haiyong Wang,Hu Li,Bijuan Cai,Wei Lv,Chiliu Cai,Chenguang Wang,Long Yan,Qiying Liu,Longlong Ma

Alloyed Cu−Ni encapsulated in carbon was prepared by loading Ni and Cu onto biochar (BC) through an initial wetness impregnation method under mild conditions. The bimetallic catalysts were exploited to perform selective hydrodeoxygenation (HDO) of 5-hydroxymethylfurfural (HMF). 2,5-Dimethylfurfural (DMF), a promising liquid fuel/fuel additive, could be obtained from HMF with the highest yield of 93.5% under the optimized conditions. During HMF HDO, two key intermediates, 5-methylfurfural (MFF) and 2,5-dihydroxymethylfuran (DHMF), dominating two distinct conversion pathways were systematically investigated by Arrhenius kinetics analysis. In addition, the turnover frequencies (TOFs) of HDO reaction over Cu−Ni/BC corresponding with Cu amount were thoroughly discussed, finding that the electron transfer from Cu to Ni in the alloy structure was beneficial to the HDO reaction and the conversion pathways can be regulated by reaction temperature variation. Importantly, the synergy of HDO of HMF by alloyed Cu−Ni metal and Lewis acid sites from oxide NiOx were hence clarified by systematic catalyst characterizations. The Cu−Ni/BC catalyst is stable for at least five consecutive runs to obtain the stabilized 81.9% of DMF since the third run.

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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2022 · IF 3.898

Enhanced production of cytidine 5′-monophosphate using biocatalysis of di-enzymes immobilized on amino-functionalized sepharose

Xiaohong Zhou,Wenfeng Zhou,Wei Zhuang,Chenjie Zhu,Hanjie Ying,Hongman Zhang

Cytidine 5′-monophosphate (5′-CMP) is an essential nucleotide for additives. In this study, enhanced production of 5′-CMP was realized by the transformation of cytidine using co-immobilized di-enzymes, uridine-cytidine kinase (UCK) and acetate kinase (AcK). The immobilization yield of the enzyme had a clear correlation with the surface charges as zeta potential ( ξ ). Among them, ε -polylysine-functionalized sepharose (SA-EPL, ξ  = 9.31 mV) showed high immobilization yield (78.8%), which was 4.9-fold than that of nitrilotriacetic acid functionalized sepharose (SA-NTA, ξ  = −12.6 mV). The residual activity of affinity co-immobilized enzyme (EPL-Ni/ [email protected] ) was higher than 70.6% after recycled 10 times. Thus, this study provides an effective approach for the production of 5′-CMP with the advantages of low adenosine 5′-triphosphate (ATP) consumption, reduced side reactions, and improved reusability by co-immobilized UCK and AcK on the functionalized Sepharose.

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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

The reaction behaviors of acetonitrile and ethyl acetate simultaneous degradation over Cu–Ce/ZSM–5 catalyst

Yaoyu Zhang,Yuxiong Wang,Yue Liu,Huimin Xu,Zhongbiao Wu

Aiming at the coexistence of pollutants in the actual industrial process, the catalytic oxidation of acetonitrile and ethyl acetate mixture on the Cu–Ce/ZSM–5 catalyst was studied. The mutual inhibition effect during catalytic removal of acetonitrile and ethyl acetate mixture was observed. Acetonitrile showed a more obvious inhibitory effect on the conversion of ethyl acetate, and the introduction of ethyl acetate reduced the N 2 selectivity of acetonitrile oxidation. The simulation results demonstrated acetonitrile could be preferentially adsorbed on Cu center of the catalyst surface, leading to significant inhibition of the initial conversion of ethyl acetate. In addition, the coexistence of ethyl acetate would weaken the hydrolysis of acetonitrile to generate carboxylic acid and –NH x species. As such, no enough adsorbed NH x species could be used to reduce the NO x produced by excessive oxidation of acetonitrile, resulting in a decreased in N 2 selectivity. This study could provide reference on the application of catalysts for cyanide–containing waste gas degradation.

CAS / MDL: 10294-41-4 10031-43-3
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Catalysts · 2022 ·Vol. 12 ·期 10 ·1216 · IF 4.501

Generation of ZSM-5 Nanocrystallites and Their Assembly into Hierarchical Architecture in a Phase-Transfer Synthesis

Xiaoling Zhao,Jinlong He,Jinjin Li

A method of phase-transfer water/toluene synthesis was developed to fabricate mesocrystals of Zeolite Socony Mobil-5 (ZSM-5) that contain both meso-/micropores and nanometer crystallites. The construction of a hierarchical architecture from nanozeolites via oriented attachment growth was achieved by a simple phase-transfer water/toluene synthesis by minimizing classical atom-by-atom crystallization. This opens the way to the cheap, highly efficient engineering of zeolitic morphologies. The physicochemical properties of the crystal were revealed by powder X-ray diffraction (XRD), N2physical adsorption, inductively coupled plasma atomic emission spectroscopy (ICP-AES), scanning electron microscopy (SEM), transmission electron microscopy (TEM), ammonia temperature-programmed desorption (NH3-TPD) and pyridine infrared spectroscopy (Py-IR), indicating that the material has a high specific surface area, mesopore volume and Lewis acid content. The hierarchical ZSM-5 exhibits a prolonged catalytic lifetime in dimethyl ether–methyl ether (DTO) conversion and enhanced selectivity for propylene owing to the enhanced structural properties. The method can be extended to the synthesis of other graded zeolites controlled by the crystallization process and produce crystals comprising traversing mesoporosity and ultrasmall crystallites that are crucial for mass transfer enhancement.Keywords:phase-transfer water/toluene synthesis;ZSM-5;hierarchical architecture;dimethyl ether–methyl ether

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CATALYSIS LETTERS · 2022 ·Vol. 153 ·期 4 ·1170-1179 · IF 2.936

Influence of Preparation Method on HZSM-5 Supported Cerium Catalyst for Alkylation of Phenol with Methanol

Luo Mingsheng,Li Hong,Song Huanqiao,Shao Changke,Wang Aimei

The alkylation of phenol with methanol was studied in vapor phase over 5 wt% cerium supported on HZSM-5 catalyst prepared by three different methods, such as impregnation, ball mixing and solid-state ion-exchange. The catalytic activities are tested in a fixed-bed reactor, and the physicochemical properties of the catalyst are characterized with X-ray powder diffraction, scanning electron microscope, nitrogen physical sorption, Fourier Transform Infrared Spectrometer, Infrared spectra of pyridine adsorption, X-ray photoelectron spectroscopy and temperature-programmed desorption of ammonia. It was found that the dispersion form of cerium was greatly affected by the preparation method, and difference in acidity affects catalytic performance in the alkylation reaction of phenol and methanol. Ball milling method generated greater amount of strong Brønsted acidic sites and lower specific surface area than other catalysts, which led to higher carbon deposition rate and lower catalyst activity. The catalyst prepared by impregnation method yields higher Lewis acid concentration (2.09 μmol/g) and more chemisorbed oxygen due to the increased Ce 3+ concentration in the lattice, resulted in an improved o-cresol selectivity of 48%. Furthermore, the catalyst prepared by solid-phase ion-exchange method produces a catalyst with appropriate B/L ratio of 60.6 and large specific surface area of 389.0 m 2 /g, which yields the highest phenol conversion of 23%. Graphical Abstract

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