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Benzenesulfonic acid-grafted UIO-66 with improved hydrophobicity as a stable Brønsted acid catalyst

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1389-1398 doi: 10.1007/s11705-022-2285-5

摘要： Hydrothermal and catalytic stability of UIO-66 MOFs with defective structures are critical aspects to be considered in their catalytic applications, especially under the conditions involving water, moisture and/or heat. Here, we report a facile strategy to introduce the macromolecular acid group to UIO-66 to improve the stability of the resulting UIO-66−PhSO3H MOF in aqueous phase catalysis. In detail, UIO-66−PhSO3H was obtained by grafting benzenesulfonic acid on the surface of the pristine UIO-66 to introduce the hydrophobicity, as well as the Brønsted acidity, then assessed using catalytic hydrolysis of cyclohexyl acetate (to cyclohexanol) in water. The introduction of hydrophobic molecules to UIO-66 could prevent the material from being attacked by hydroxyl polar molecules effectively, explaining its good structural stability during catalysis. UIO-66−PhSO3H promoted the conversion of cyclohexyl acetate at ca. 87%, and its activity and textural properties were basically intact after the cyclic stability tests. The facile modification strategy can improve the hydrothermal stability of UIO-66 significantly, which can expand its catalytic applications in aqueous systems.

关键词： metal−organic frameworks (MOFs)     UIO-66     hydrolysis of cyclohexyl acetate     hydrophobicity     Brønsted acidity    

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Biodiesel production by the transesterification of cottonseed oil by solid acid catalysts

CHEN He, PENG Baoxiang, WANG Dezheng, WANG Jinfu

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 11-15 doi: 10.1007/s11705-007-0003-y

摘要： Methyl esters (biodiesel) were produced by the transesterification of cottonseed oil with methanol in the presence of solid acids as heterogeneous catalysts. The solid acids were prepared by mounting HSO on TiO · nHO and Zr(OH), respectively, followed by calcining at 823K. TiO-SO and ZrOSO showed high activity for the transesterification. The yield of methyl esters was over 90% under the conditions of 230°C, methanol/oil mole ratio of 12:1, reaction time 8 h and catalyst amount (catalyst/oil) of 2% (w). The solid acid catalysts showed more better adaptability than solid base catalysts when the oil has high acidity. IR spectral analysis of absorbed pyridine on the samples showed that there were Lewis and BrØnsted acid sites on the catalysts.

关键词： BrØnsted     reaction     presence     cottonseed     biodiesel    

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Study on extraction of thiophene from model gasoline with br?nsted acidic ionic liquids

Xiaomeng WANG, Mingjuan HAN, Hui WAN, Cao YANG, Guofeng GUAN

《化学科学与工程前沿（英文）》 2011年 第5卷 第1期   页码 107-112 doi: 10.1007/s11705-010-0539-0

摘要： Br?nsted acidic ionic liquids (ILs), -methylimidazole hydrogen sulfate ([HMIm]HSO ) and -methylpyrrolidone hydrogen sulfate ([HNMP]HSO ), are synthesized and employed as extractants to extract thiophene from model gasoline (thiophene dissolved in -octane). The effect of extraction temperature, extraction time and volume ratio of ILs to model gasoline on desulfurization rates is investigated. Then, the optimal desulfurization conditions are obtained: the ratio of ILs to model gasoline is 1∶1, extraction temperature is 50°C for [HMIm]HSO and 60°C for [HNMP]HSO , extraction time is 60 min. Meanwhile, the desulfurization rate of [HNMP]HSO for model gasoline is 62.8%, which is higher than that of [HMIm]HSO (55.5%) under optimal conditions. The reason is discussed on the basis of the interaction energy between thiophene and ILs at the B3LYP/6-311++ G(d,p) level. Furthermore, the total desulfurization rate of [HNMP]HSO and [HMIm]HSO reaches 96.4% and 94.4%, respectively, by multistage extraction. Finally, the used ILs can be reused by vacuum drying, and their desulfurization rates are not significantly decreased after recycling 7 times in single-stage desulfurization.

关键词： br?nsted ionic liquids     model gasoline     thiophene     extraction     density functional theory    

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Ionic liquid mediated esterification of alcohol with acetic acid

Beilei ZHOU, Yanxiong FANG, Hao GU, Saidan ZHANG, Baohua HUANG, Kun ZHANG

《化学科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 211-214 doi: 10.1007/s11705-009-0054-3

摘要： Highly efficient esterification of alcohols with acetic acid by using a Br?nsted acidic ionic liquid, i.e., 1-methyl-2-pyrrolidonium hydrogen sulfate ([Hnmp]HSO ), as catalyst has been realized. The turnover numbers (TON) were able to reach up to 11000 and turnover frequency (TOF) was 846. The catalytic system is suitable for the esterification of long chain aliphatic alcohols, benzyl alcohol and cyclohexanol with good yields of esters. The procedure of separating the product and catalyst is simple, and the catalyst could be reused. [Hnmp]HSO had much weaker corrosiveness than H SO . The corrosive rate of H SO was 400 times more than that of [Hnmp]HSO to stainless steel.

关键词： ionic liquid     Br?nsted acid     esterification     catalyst    

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Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

《环境科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 186-193 doi: 10.1007/s11783-009-0016-5

摘要： The reaction mechanisms of selective catalytic reduction (SCR) of nitric oxide (NO) by methane (CH ) over solid superacid-based catalysts were proposed and testified by DRIFTS studies on transient reaction as well as by kinetic models. Catalysts derived from different supports would lead to different reaction pathways, and the acidity of solid superacid played an important role in determining the reaction mechanisms and the catalytic activities. Higher ratios of Br?nsted acid sites to Lewis acid sites would lead to stronger oxidation of methane and then could facilitate the step of methane activation. Strong Br?nsted acid sites would not necessarily lead to better catalytic performance, however, since the active surface NO species and the corresponding reaction routes were determined by the overall acidity strength of the support. The reaction routes where NO moiety was engaged as an important intermediate involved moderate oxidation of methane, the rate of which could determine the overall activity. The reaction involving NO moiety was likely to be determined by the step of reduction of NO. Therefore, to enhance the SCR activity of solid superacid catalysts, reactions between appropriate couples of active NO species and activated hydrocarbon intermediates should be realized by modification of the support acidity.

关键词： selective catalytic reduction (SCR)     nitric oxide (NO)     methane     support acidity     Br?nsted acid sites     NOy species    

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G-quadruplex formation of oligonucleotides containing ALS and FTD related GGGGCC repeat

Jasna Brčić,Janez Plavec

《化学科学与工程前沿（英文）》 2016年 第10卷 第2期   页码 222-237 doi: 10.1007/s11705-016-1556-4

摘要： A largely increased number of GGGGCC repeats located in the non-coding region of gene have been identified as the leading cause of two related neurological disorders, familial amyotrophic lateral sclerosis (ALS) and frontotemporal dementia (FTD). We examined G-quadruplex forming ability of GGGGCC-repeat containing oligonucleotides with four guanine tracts chosen as the smallest possible model to form a unimolecular G-quadruplex. These oligonucleotides are readily to folded into G-quadruplexes in the presence of K ions. However, the formation of multiple structures makes structural analysis challenging and time consuming. We observed that flanking sequences on 5'- and 3'-ends as well as mutations of loop residues have a profound effect on folding. Sequence d[(G C ) G ] was chosen for further scrutiny and optimization of nuclear magnetic resonance (NMR) spectroscopic properties with dG to 8Br-dG substitutions at specific positions in the sequence under different folding conditions. Expectedly, folding into desired predominant topology is facilitated when substituted residue adopted a conformation in the naturally-occurring structure. Single dG to 8Br-dG substitution at position 21 and fine tuning of folding conditions facilitate folding of d[(G C ) GG GG] into (mostly) a single G-quadruplex, and thus enable determination of its high-resolution structure by high-field NMR.

关键词： G-quadruplex     GGGGCC     NMR     ALS/FTD     polymorphism    

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Sulfonic acid-functionalized mesoporous silica catalyst with different morphology for biodiesel production

《化学科学与工程前沿（英文）》 2022年 第16卷 第8期   页码 1198-1210 doi: 10.1007/s11705-021-2133-z

摘要： Sulfonic acid functionalized mesoporous silica based solid acid catalysts with different morphology were designed and fabricated. The synthesized materials were characterized by various physicochemical and spectroscopic techniques like scanning electron microscope-energy dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, Brunauer–Emmett–Teller surface area, thermogravimetric analysis and n-butylamine acidity. The shape of catalysts particles plays an important role in its activity. The sulfonic acid functionalized mesoporous silica catalysts of spherical shape and the cube shape were assessed for catalytic activity in biodiesel production. The catalytic biodiesel production reaction over the catalysts were studied by esterification of free fatty acid, oleic acid with methanol. The effect of various reaction parameters such as catalyst concentration, acid/alcohol molar ratio, catalyst amount, reaction temperature and reaction time on catalytic activity were investigated to optimize the conditions for maximum conversion. It was sulfonated cubic shape mesoporous silica which exhibited better activity as compared to the spherical shape silica catalysts. Additionally, the catalyst was regenerated and reused up to three cycles without any significant loss in activity. The present catalysts exhibit superior performance in biodiesel production and it can be used for the several biodiesel feedstock’s that are rich in free fatty acids.

关键词： solid acid catalyst     mesoporous silica     sulfonic acid     biodiesel     esterification     oleic acid    

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Amino acid promoted hydrogen battery system using Mn-pincer complex for reversible CO hydrogenation toformic acid

《能源前沿（英文）》 2022年 第16卷 第5期   页码 697-699 doi: 10.1007/s11708-022-0843-7

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Enzyme@bismuth-ellagic acid: a versatile platform for enzyme immobilization with enhanced acid-base stability

《化学科学与工程前沿（英文）》 2023年 第17卷 第6期   页码 784-794 doi: 10.1007/s11705-022-2278-4

摘要： In situ encapsulation is an effective way to synthesize enzyme@metal–organic framework biocatalysts; however, it is limited by the conditions of metal–organic framework synthesis and its acid-base stability. Herein, a biocatalytic platform with improved acid-base stability was constructed via a one-pot method using bismuth-ellagic acid as the carrier. Bismuth-ellagic acid is a green phenol-based metal–organic framework whose organic precursor is extracted from natural plants. After encapsulation, the stability, especially the acid-base stability, of amyloglucosidases@bismuth-ellagic acid was enhanced, which remained stable over a wide pH range (2–12) and achieved multiple recycling. By selecting a suitable buffer, bismuth-ellagic acid can encapsulate different types of enzymes and enable interactions between the encapsulated enzymes and cofactors, as well as between multiple enzymes. The green precursor, simple and convenient preparation process provided a versatile strategy for enzymes encapsulation.

关键词： bismuth-ellagic acid     in situ encapsulation     enzyme@MOF biocomposites    

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Discovery of novel ursolic acid derivatives as effective antimicrobial agents through a ROS-mediated

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 2101-2113 doi: 10.1007/s11705-023-2361-5

摘要： In response to the reduction of food production and economic losses caused by plant bacterial diseases, it is necessary to develop new, efficient, and green pesticides. Natural products are rich and sustainable source for the development of new pesticides due to their low toxicity, easy degradation, and eco-friendliness. In this study, we prepared three series of ursolic acid derivatives and assessed their antibacterial ability. Most target compounds exhibited outstanding antibacterial activities. Among them, the relative optimal EC50 values of Xanthomonas oryzae pv. oryzae and Xanthomonas axonopodis pv. citri were 2.23 (A17) and 1.39 (A16) μg·mL–1, respectively. The antimicrobial mechanism showed that compound A17 induced an excessive accumulation and production of reactive oxygen species in bacteria and damaged the cell membrane integrity to kill bacteria. More interestingly, the addition of low concentrations of exogenous hydrogen peroxide enhanced the antibacterial efficacy of compound A17 against Xanthomonas oryzae pv. oryzae. These entertaining results suggested that compound A17 induced an apparent apoptotic behavior in the tested bacteria. Overall, we developed the promising antimicrobial agents that destroyed the redox system of phytopathogenic bacteria, further demonstrating the unprecedented potential of ursolic acid for agricultural applications.

关键词： ursolic acid     antibacterial activities     reactive oxygen species     apoptosis    

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Synergistic scale inhibition of polyaspartic acid composite with magnetic field

LIU Zhenfa, WANG Yanji, GAO Yuhua, ZHANG Lihui

《化学科学与工程前沿（英文）》 2007年 第1卷 第3期   页码 261-265 doi: 10.1007/s11705-007-0047-z

摘要： Polyaspartic acid (PASP) composite, a scale inhibitor, was prepared from PASP, itaconic acid–acrylic acid–acrylic ester (IA-AA-AE) terpolymer and 2-phosphonobutane- 1,2,4-tricarboxylic acid (PBTCA). The scale inhibition of PASP composite and the effect of its synergism with a magnetic field on scale inhibition were investigated. Calcium carbonate crystals in scale samples were characterized by means of SEM and XRD. The static and dynamic experiments show that the chelating function of PASP composite for Ca can be enhanced by synergism with a magnetic field. Under Ca 650 mg/L, HCO 1,300 mg/L and PASP composite 4 mg/L, the scale inhibition rate of PASP composite in magnetic water can increase by 10% in static state and by 20% in dynamic experiments. Scanning electron microscope (SEM) and X-ray diffraction (XRD) results show that calcite and aragonite can be completely transformed into vaterite by using PASP composite.

关键词： synergism     magnetic     PBTCA     dynamic     acid–acrylic acid–acrylic    

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Abiotic association of phthalic acid esters with humic acid of a sludge landfill

Xiaoli CHAI, Yongxia HAO, Xin ZHAO, Guixiang LIU, Ying ZHU, Rong JI, Jun WU, Huanhuan TONG, Youcai ZHAO

《环境科学与工程前沿（英文）》 2012年 第6卷 第6期   页码 778-783 doi: 10.1007/s11783-012-0434-7

摘要： The abiotic association between phthalic acid esters (PAEs) and humic substances (HS) in sludge landfill plays an important role in the fate and stability of PAEs. An equilibrium dialysis combined with C-labeling was used to study the abiotic association of two abundant PAEs (diethyl phthalate and di- -butyl phthalate) with humic acid (HA) isolated from a sludge landfill with different stabilization times and different molecular weights. Elemental analysis and Fourier Transform Infrared Spectrophotometer (FTIR) suggested that high value of HA was related to the high aromatic content and large molecular weight of HA. The results indicated that the association strength of PAEs with HA depended on both the properties of the PAEs and the characteristics of HA. The values of the association were strongly dependent on solution pH, and decreased dramatically as the pH was increased from 3.0 to 9.0. The results suggested that non-specific hydrophobic interaction between PAEs and HA was the main contributor to the association of the PAEs with HA. The interactive hydrogen-bonds between the HA and the PAEs molecules may also be involved in the association.

关键词： abiotic association     phthalic acid esters (PAEs)     humic acid     sludge     landfill    

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New perspectives in free nitrous acid (FNA) uses for sustainable wastewater management

《环境科学与工程前沿（英文）》 2023年 第18卷 第2期 doi: 10.1007/s11783-024-1786-5

摘要：

● The historical development of free nitrous acid (FNA) technologies is reviewed.

关键词： Free nitrous acid     Acid-tolerant ammonia oxidizer     In situ generation     Wastewater management    

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Genomic and metabolomic analysis of with enhanced poly--glutamic acid production through atmospheric

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1751-1760 doi: 10.1007/s11705-022-2211-x

摘要： Poly-γ-glutamic acid is an extracellular polymeric substance with various applications owing to its valuable properties of biodegradability, flocculating activity, water solubility, and nontoxicity. However, the ability of natural strains to produce poly-γ-glutamic acid is low. Atmospheric and room temperature plasma was applied in this study to conduct mutation breeding of Bacillus licheniformis CGMCC 2876, and a mutant strain M32 with an 11% increase in poly-γ-glutamic acid was obtained. Genome resequencing analysis identified 7 nonsynonymous mutations of ppsC encoding lipopeptide synthetase associated with poly-γ-glutamic acid metabolic pathways. From molecular docking, more binding sites and higher binding energy were speculated between the mutated plipastatin synthase subunit C and glutamate, which might contribute to the higher poly-γ-glutamic acid production. Moreover, the metabolic mechanism analysis revealed that the upregulated amino acids of M32 provided substrates for glutamate and promoted the conversion between L- and D-glutamate acids. In addition, the glycolytic pathway is enhanced, leading to a better capacity for using glucose. The maximum poly-γ-glutamic acid yield of 14.08 g·L–1 was finally reached with 30 g·L–1 glutamate.

关键词： ARTP mutagenesis     Bacillus licheniformis     poly-γ-glutamic acid     metabolomics    

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Proline-2′-deoxymugineic acid, a phytosiderophore analog, drives beneficial rhizobacterial community

《农业科学与工程前沿（英文）》 doi: 10.15302/J-FASE-2023531

摘要：

● Proline-2′-deoxymugineic (PDMA) significantly altered the bacterial community in the peanut rhizosphere.

关键词： Beneficial rhizobacteria recruitment     peanut     plant-soil micronutrition enhancement     proline-2′-deoxymugineic acid     stable microbial network    

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标题 作者 时间 类型 操作

Benzenesulfonic acid-grafted UIO-66 with improved hydrophobicity as a stable Brønsted acid catalyst

期刊论文

Biodiesel production by the transesterification of cottonseed oil by solid acid catalysts

CHEN He, PENG Baoxiang, WANG Dezheng, WANG Jinfu

期刊论文

Study on extraction of thiophene from model gasoline with br?nsted acidic ionic liquids

Xiaomeng WANG, Mingjuan HAN, Hui WAN, Cao YANG, Guofeng GUAN

期刊论文

Ionic liquid mediated esterification of alcohol with acetic acid

Beilei ZHOU, Yanxiong FANG, Hao GU, Saidan ZHANG, Baohua HUANG, Kun ZHANG

期刊论文

Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

期刊论文

G-quadruplex formation of oligonucleotides containing ALS and FTD related GGGGCC repeat

Jasna Brčić,Janez Plavec

期刊论文

Sulfonic acid-functionalized mesoporous silica catalyst with different morphology for biodiesel production

期刊论文

Amino acid promoted hydrogen battery system using Mn-pincer complex for reversible CO hydrogenation toformic acid

期刊论文

Enzyme@bismuth-ellagic acid: a versatile platform for enzyme immobilization with enhanced acid-base stability

期刊论文

Discovery of novel ursolic acid derivatives as effective antimicrobial agents through a ROS-mediated

期刊论文

Synergistic scale inhibition of polyaspartic acid composite with magnetic field

LIU Zhenfa, WANG Yanji, GAO Yuhua, ZHANG Lihui

期刊论文

Abiotic association of phthalic acid esters with humic acid of a sludge landfill

Xiaoli CHAI, Yongxia HAO, Xin ZHAO, Guixiang LIU, Ying ZHU, Rong JI, Jun WU, Huanhuan TONG, Youcai ZHAO

期刊论文

New perspectives in free nitrous acid (FNA) uses for sustainable wastewater management

期刊论文

Genomic and metabolomic analysis of with enhanced poly--glutamic acid production through atmospheric

期刊论文

Proline-2′-deoxymugineic acid, a phytosiderophore analog, drives beneficial rhizobacterial community

期刊论文