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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY · 2023 · IF 6.1

Producing Lignin and Ethyl Levulinate from Wheat Stalk Using 1-(3-Sulfobutyl) Triethylammonium Hydrogen Sulfate and USY Zeolite

Dingkai Wang,Mingyu Cui,Yanjun Li,Wei Zhao,Shangshang Ma,Zhijie Jiang,Xutang Liu,Chong Liang,Rujuan Li,Long Ma,Yanmin Song,Xian-Yong Wei

The facile, green, and efficient strategy for the separation of lignin from straw and subsequent production of value-added chemicals is crucial to the current utilization of straw. Herein, up to 23.72% of lignin was isolated from wheat stalk over cheap and green 1-(3-sulfobutyl) triethylammonium hydrogen sulfate ([BSTEA]HSO4) in aqueous ethanol (Vethanol: Vwater = 4:1). The acquired lignin was verified as a p-hydroxyphenyl-guaiacyl-syringyl type, which had a narrower molecular weight distribution, better thermal stability, and higher purity compared with those of the lignin obtained using 1-methyl-3-(4-sulfobutyl)-imidazolium hydrogen sulfate and 1-(3-sulfobutyl) pyridinium hydrogen sulfate. Moreover, a carbohydrate-rich liquid containing [BSTEA]HSO4 was obtained by water removal from the waste liquid after lignin separation and further converted to ethyl levulinate (EL) by a one-pot process in the presence of inexpensive and stable USY zeolite. The yield of EL reached 30.23% at 200 °C for 60 min over the presence of 40% [BSTEA]HSO4 and 60% USY zeolite. Under optimal conditions, the yields of lignin and EL can respectively reach 83.89 and 72.28% of those catalyzed by a fresh catalyst after five cycles. In short, the above-mentioned methods present a green, economic, and efficient route for the extraction of lignin and further treatment of the liquid waste generated during the extraction process.

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ENVIRONMENTAL RESEARCH · 2022 · IF 8.431

Enhanced photo-Fenton degradation of tetracycline hydrochloride by 2, 5-dioxido-1, 4-benzenedicarboxylate-functionalized MIL-100(Fe)

Mingyu Li,Yuhan Ma,Jingjing Jiang,Tianren Li,Chongjun Zhang,Zhonghui Han,Shuangshi Dong

Heterogeneous photo-Fenton technology has drawn tremendous attention for removal of recalcitrant pollutants. Fe-based metal-organic frameworks (Fe-MOFs) are regarded to be superior candidates in wastewater treatment technology . However, the central metal sites of the MOFs are coordinated with the linkers, which reduces active site exposure and decelerates H 2 O 2 activation. In this study, a series of 2, 5-dioxido-1, 4-benzenedicarboxylate (H 2 DOBDC)-functionalized MIL-100(Fe) with enhanced degradation performance was successfully constructed via solvothermal strategy. The modified MIL-100(Fe) displayed an improvement in photo-Fenton behaviors. The photocatalytic rate constant of optimized MIL-100(Fe)-1/2/3 are 2.3, 3.6 and 4.4 times higher compared with the original MIL-100(Fe). The introduced H 2 DOBDC accelerates the separation and transfer in photo-induced charges and promotes Fe(II)/Fe(III) cycle, thus improving the performance. •OH and •O 2 − are main reactive radicals in tetracycline (TCH) degradation. Dealkylation, hydroxylation, dehydration and dealdehyding are the main pathways for TCH degradation.

CAS / MDL: 554-95-0
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Bioengineered · 2022 · IF 6.832

Application of serum exosomal hypoxia-inducible factor-1 alpha (HIF-1α) as potential circulating biomarker for bacterial peritonitis

Xiao-Yi Chen,Qian-Long Wang,Wei-Xue Huang,Long-Wei Li,Lan-Cong Liu,Yi Yang,You-Jiao Wu,Shan-Shan Song,Hao Ma,Hua Zhou,Pei Luo

Bacterial peritonitis is a severe disease that diagnosis remains challenging for clinicians. Measuring biomarkers might be a rapid diagnostic method. The objective of this study was to analyze and evaluate the dynamic changes in HIF-1α concentration in serum exosomes during bacterial peritonitis. The pre-clinical application value of serum exosomal HIF-1α was evaluated via imipenem and cilastatin sodium (ICS) intervention in the bacterial peritonitis model. The new colorimetric method to quantitate dynamic expression changes of HIF-1α in serum exosomes during bacterial peritonitis was established by our team via using the gold seed-coated with aptamer-functionalized Au @ Au core-shell peroxidase mimic. The typical inflammatory cytokines of bacterial peritonitis were also measured. Following intramuscular administration with ICS, In-Vivo Xtreme imaging system was used to visualize abdominal infection extent. Meanwhile, HIF-1α concentration in rat serum exosomes and pro-inflammatory factors levels in serum were detected. The serum typical inflammatory cytokines levels were elevated in GFP-labeled E.coli induced bacterial peritonitis. The serum exosomal HIF-1α levels clearly increased at 12 h, reached the peak during 24–48 h, and then gradually decreased at 72 h. Following intramuscular administration with ICS, the abdominal infection extent, HIF-1α concentration in serum exosomes, and the serum pro-inflammatory factors levels were reduced at 24 h in GFP-labeled E. coli induced bacterial peritonitis model. The serum exosomal HIF-1α can be used as a biomarker in the early stage of bacterial peritonitis, which might provide the basic research in the pre-clinical for further predicting and monitoring the pathological process of bacterial peritonitis.

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RESEARCH ON CHEMICAL INTERMEDIATES · 2022 ·Vol. 48 ·期 3 ·983-1001 · IF 3.134

Synthesis of 1, 3, 5-trisubstituted-4,5-dihydro-1H-pyrazole catalyzed by vitamin B1 and its fluorescence properties

Zhang Dawei,Ren Lu,Liu Ailing,Zhang Yumin,Lv Yang,Gu Qiang

Abstract An efficient synthesis of 1,3,5-trisubstituted-1 H -pyrazoles was developed via cyclocondensation in 78–92% yields starting from α , β -unsaturated aldehydes/ketones with substituted phenylhydrazine using vitamin B 1 as a catalyst, and was characterized by HR-MS, FT-IR, 1 H NMR and 13 C NMR spectroscopy. The reaction has simple operation, metal-free catalysis, acid or base free catalysis. As a green catalyst, vitamin B 1 was found to possess favorable catalytic activity and reusability for the condensation reaction. 1,3,5-trisubstituted-1 H -pyrazole shows from orange-red to cyan in different solvents when the electron withdrawing group is attached to acetophenone (taking compound 5i as an example). Compound 5i as a metal ion fluorescent probe has excellent selectivity for Ag + detection. The crystal structure of the compound 3-(4-chlorophenyl)-1,5-diphenyl-4,5-dihydro-1 H -pyrazole ( 5b ) in the orthorhombic space group Pca 21 was presented and formed racemic crystals. Graphical abstract

CAS / MDL: 100-52-7
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Natural Product Communications · 2022 · IF 1.496

Synthesis and Evaluation of Acylated Derivatives of Hederagenin as Inhibitors of HIV-1 and HCV NS3/4A Proteases

Qing Liu,Ying Wei,Yongjia Hao,Jian Yang,Bowen Pan,Xiaosheng Yang,Ying Zhou,Xia Wang

Viral infection imposes a major threat to human health. To develop new potent antiviral agents, Hederagenin (HE), a known inhibitor of HIV-1 and HCV NS3/4A proteases, was used as a starting material to synthesize 4 types of HE derivatives, HE-3,23-diacyl, HES-3,23-diacyl, HES-3-acyl, and HES-3-oxo-23-acyl. We evaluated the in vitro inhibitory activities of the derivatives against HIV-1 and HCV NS3/4A proteases. (3β,23)-Di-O-diglutaryl-hederagenin (1b) and (3β,23)-di-O-(3′,3′-dimethylsuccinyl-hederagenin ethyl ester (2b) exhibited potent inhibitory activities against the HIV-1 and/or HCV NS3/4A proteases with IC50 values < 10 μM, but did not appreciably inhibit general human proteases renin and trypsin. The SARs showed that dicarboxylic acid hemiesters of HE significantly enhance the antiviral activities when C3 or C23 are linked with 6 carbon acyl chains.

CAS / MDL: 112926-00-8 18623-11-5
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FUEL · 2022 · IF 8.035

Symbiosis of 1 T and 2H phases in the basal plane of defective MoS2 nanoflowers for efficient hydrodesulfurization

Zhe Bai,Luyao Wang,Hongwei Cao,Xiangwen Zhang,Guozhu Li

Hydrodesulfurization (HDS) is an effective way to reduce sulfur content in oil for the enforcement of more stringent environmental regulations. MoS 2 has been widely used as an effective component for catalyzing HDS, and needs to be extensively studied in depth. Herein, MoS 2 nanoflowers with the symbiosis of 1T-2H phases in the basal planes and coexistence of S and Mo vacancies are prepared via the assembly of many nanosheets by a one-pot solvothermal method. The morphology, crystal phase structure and defects of these 1T-2H MoS 2 samples were well characterized. The 1T/2H ratio and the state of vacancies were effectively tuned by changing the solvothermal conditions. Active and stable 1T-2H mixed MoS 2 nanoflowers with high content of 1T phase and moderate S and Mo vacancies were obtained by the regulation of oxalic acid in the mixture of ethanol and water. In the HDS of dibenzothiophene at 300 °C and 4 MPa, the optimal catalyst of MoS 2 -water–ethanol-OA exhibited a substrate conversion of 89.3% in 10 h. Moreover, the activity of MoS 2 -water–ethanol-OA was well retained without any decrease in the recycling experiment.

CAS / MDL: 12054-85-2
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FUEL · 2022 · IF 8.035

Synthesis of advanced fuel with density higher than 1 g/mL by photoinduced [2 + 2] cycloaddition of norbornene

Yi Liu,Ying Chen,Shuang Ma,Xianlong Liu,Xiangwen Zhang,Ji-Jun Zou,Lun Pan

High-energy–density (HED) fuels have attracted extensive attention for volume-fixed aerospace vehicles because they can provide more propulsion energy to increase the payload and range of aerospace vehicles. Herein, we report a route for synthesis of HED fuel, pentacyclo[8.2.1.1 4,7 .0 2,9 .0 3,8 ]tetradecane (PCTD) with strained structure, by photoinduced intermolecular [2 + 2] cycloaddition of norbornene (NBE). The triplet quenching and phosphorescence quenching results indicate that NBE cycloaddition is conducted through the photosensitized processes containing triplet–triplet energy transfer, cyclization and relaxation. The reaction conditions are optimized to obtain the high photocatalytic activity, with the NBE conversion and PCTD selectivity reaching 78.7% and 94.4%, respectively. Moreover, a kinetic model is proposed with the reaction rate equation being correlated with the incident light flux, with the pseudo reaction kinetics parameters and reaction rate equations obtained. Importantly, PCTD shows high density of 1.024 g/mL and high volumetric net heat of combustion of 42.98 MJ/L, much higher than those of JP-10. In addition, blending with JP-10 or QC can significantly improve cryogenic properties of blended fuels, which is very promising for the practical application.

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REACTIVE & FUNCTIONAL POLYMERS · 2022 · IF 4.966

Fabricating hypercrosslinked aromatic-rich starch urethane polymer with enhanced adsorption performance for separation of acetophenone and 1-phenylethanol

Ziqi Zhao,Yulong Liu,Youquan Zhang,Mei Yang,Fang Shen,Zongwu Wei,Kungang Chai,Hongbing Ji

Starch-based urethane polymers hold great potential for adsorptive separation of acetophenone (AP) and 1-phenylethanol (PE), which coexist commonly in the petrochemical by-products. Yet, the overall adsorption performance was restricted due to the poor porosity of adsorbent. We herein applied external crosslinking strategy to fabricate hypercrosslinked aromatic-rich starch urethane polymer (HASUP) with large surface area. The structural evolution, including chemical state, porosity and morphology were observed through various characteristic techniques. The adsorption properties of AP and PE onto HASUP were investigated in both single and binary systems. Compared to its non-porous precursor, HASUP exhibited significantly higher overall adsorption capacity while maintaining the AP selectivity with varying compositions . The further static and dynamic adsorption assessments demonstrated that HASUP showed exceptional performance to separate AP and PE. And HASUP also exhibited excellent anti-interference ability and recyclability for selective adsorption of AP over PE. Furthermore, theoretical results indicated that the multiple interactions including hydrophobic, π-π, and hydrogen bonding interactions account for selective adsorption of AP. In combination with high surface area, this synergistic effect enhanced the adsorption strength , affording a high AP uptake for HASUP. This work may provide an insight for designing novel porous starch-based adsorbents with high performance.

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BIOCHIMICA ET BIOPHYSICA ACTA-MOLECULAR BASIS OF DISEASE · 2022 · IF 6.633

Fluorofenidone ameliorates cholestasis and fibrosis by inhibiting hepatic Erk/-Egr-1 signaling and Tgfβ1/Smad pathway in mice

Huiwen Wang,Jian Zhang,Xiaoxun Zhang,Nan Zhao,Zongtao Zhou,Lijian Tao,Lei Fu,Shifang Peng,Jin Chai

Cholestasis is characterized by intrahepatic accumulation of bile acids (BAs), resulting in liver injury, fibrosis, and liver failure. To date, only ursodeoxycholic acid and obeticholic acid have been approved for the treatment of cholestasis. As fluorofenidone (AKF-PD) was previously reported to play significant anti-fibrotic and anti-inflammatory roles in various diseases, we investigated whether AKF-PD ameliorates cholestasis. A mouse model of cholestasis was constructed by administering a 0.1 % 3,5-diethoxycarbonyl-1,4-dihydroxychollidine (DDC) diet for 14 days. Male C57BL/6 J mice were treated with either AKF-PD or pirfenidone (PD) orally in addition to the DDC diet. Serum and liver tissues were subsequently collected and analyzed. We found that AKF-PD significantly reduced the levels of serum alanine aminotransferase (ALT), aspartate aminotransferase (AST), alkaline phosphatase (ALP) and total bile salts (TBA), as well as hepatic bile acids (BAs) levels. Hepatic histological analyses demonstrated that AKF-PD markedly attenuated hepatic inflammation and fibrosis. Further mechanistic analyses revealed that AKF-PD markedly inhibited expression of Cyp7a1, an enzyme key to BAs synthesis, by increasing Fxr nuclear translocation, and decreased hepatic inflammation by attenuating Erk/-Egr-1-mediated expression of inflammatory cytokines and chemokines Tnfα, Il-1β, Il-6, Ccl2, Ccl5 and Cxcl10. Moreover, AKF-PD was found to substantially reduce liver fibrosis via inhibition of Tgfβ1/Smad pathway in our mouse model. Here, we found that AKF-PD effectively attenuates cholestasis and hepatic fibrosis in the mouse model of DDC-induced cholestasis. As such, AKF-PD warrants further investigation as a candidate drug for treatment of cholestasis.

CAS / MDL: 7440-05-3
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Biomaterials Advances · 2022 · IF 0

ICAM-1 targeted thermal-sensitive micelles loaded with tofacitinib for enhanced treatment of rheumatoid arthritis via microwave assistance

Qiying Shen,Quan Hu,Ting Tang,Xiaoying Ying,Gaofeng Shu,Jiawei Shen,Chong Teng,Yongzhong Du

Rheumatoid arthritis (RA) is an immune-mediated inflammatory disease without effective treatment. Tofacitinib (TOF) is a JAK inhibitor that can be used for RA therapy, but it still faces the problems of nonspecific distribution and relatively low therapeutic effect. Herein, ICAM-1-modified TOF-loaded P(AN-co-AAm)-PEG micelles (AI-TM) were developed, which can result in an enhanced RA therapy when combining with microwave hyperthermia (MH). It was found that AI-TM could rapidly release the encapsulated TOF under a thermal condition of >43 °C, which was due to the fact that the polymeric micelles has an upper critical solution temperature (UCST) of 43 °C. AI-TM could specifically distribute into the inflamed joints of RA mice, which is associated with the high affinity between anti-ICAM-1 and overexpressed ICAM-1 receptors. Moreover, the combination of AI-TM and MH could result in a remarkably enhanced anti-rheumatic activity, which was related to the RA-targeted ability of AI-TM, the rapid TOF release under MH, and the combined effect between TOF and MH treatment. Our study definitely provides a novel strategy for effective treatment of RA.

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MICROPOROUS AND MESOPOROUS MATERIALS · 2022 · IF 5.876

Promotion effect of the S-1 zeolite microenvironment on confined Pd nanoparticles for the selective hydrogenation of nitrile

Qiqi Lu,Xiu-Zhi Wei,Jianguo Liu,Longlong Ma

Zeolite-tailored encapsulation of metal nanoparticles exhibits prominent catalytic performance in many fields especially for selective hydrogenation reaction due to the modulation effect of the zeolite microenvironment. Here, Pd nanoparticles encapsulated in MFI zeolite by an in-situ encapsulation method were first used in the selective hydrogenation of nitrile into a primary amine. After introducing KOH for mediating the acid-base property of zeolite microenvironment, the as-synthesized [email protected] manifested an improved selectivity in the synthesis of primary amine from nitrile, while outperformed both commercial catalysts and conventional Pd supported on zeolite catalyst. The remarkable performance of [email protected] could be attributed to both the basic property of the S-1-K zeolite for inhibiting the side reactions and the highly dispersed and ultrasmall Pd clusters for superior catalytic activity. Besides, the best yield of 81% was achieved at 80 °C, 5 bar H 2 , 2 h in ammonia solution via optimization experiments, and the moderate applicability of [email protected] catalyst was obtained by substrate scope test.

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NANOTECHNOLOGY · 2022 ·Vol. 33 ·期 32 ·325601 · IF 3.953

Tunable synthesis of dendritic fibrous nano silica using 1-pentanol-water microemulsion at low oil to water ratio

Xuexue Liu,Xiang Zhang,Jian Chen,Changhao Zhang,Songke Feng,Weiguo Zhang

Dendritic fibrous nanosilica (DFNS) is a suitable nano-carrier for loading pesticides with radially oriented pores and a large surface area. The microemulsion method is standard method to prepare DFNS, and 1-pentanol is taken to replace cyclohexane as an oil solvent due to its high stability and nontoxic property. The results showed that the volume ratio of 1-pentanol (oil) to water (O/W) and the molar ratio of hexadecyltrimethylammonium bromide (CTAB) to tetraethylorthosilicate (TEOS) had effected on morphology and adsorption properties of DFNS in the water-CTAB-1-pentanol-ethanol-trimethylbenzene (TMB) microemulsion system. DFNS with bicontinuous concentric lamellar morphologies can be synthesized in this microemulsion at the meager O/W volume ratio (0.025–0.045). It features a tight mesoporous structure with a thin dendritic fibrous in 0.03 to 0.04 O/W volume ratio. The particle sizes, surface areas, and porosity of DFNS were positively correlated with the addition of the silica precursor TEOS. The size of DFNS increased from 123 to about 220 nm with the CTAB/TEOS molar ratio decreasing from 0.119 to 0.050. When the molar ratio of CTAB to TEOS  = 0.119, DFNS has a smaller particle size (123 nm) with a larger surface area and abundant honeycomb mesopores; the low O/W volume ratio strategy provides theoretical support for the industrialization development of DFNS and nano-pesticides, which plays a profound role in promoting the sustainable development of pesticide reduction, efficiency and green agriculture.

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