GREEN CHEMISTRY
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2015
·Vol. 18
·期 6
·1738-1750
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IF 8.02
Jiliang Ma,Linxin Zhong,Xinwen Peng,Runcang Sun
A simple and effective synthesis of 3,4-dihydropyrimidin-2(1H)-ones/thiones and their derivatives from aldehydes, β-dicarbonyl compounds and urea or thiourea using D-xylonic acid both as a green solvent and an effective catalyst is described. Taking the environment and economy into account, the work presented here has the merits of environmental friendliness, easy operation, simple work-up, excellent yields and the avoidance of organic solvents and inexpensive catalysts. In addition, the good properties of D-xylonic acid have also been validated by the synthesis of 5-phenyl-1(4-methoxyphenyl)-3[(4-methoxyphenyl)-amino]-1H-pyrrol-2(5H)-one and 12-phenyl-9,9-dimethyl-8,9,10,12-tetrahydrobenzo[a]xanthen-11-one. The synthesized compounds were characterized by FT-IR, 1H NMR, 13C NMR and melting point.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2016
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IF 2.653
Chuan-Chuan Zeng,Cheng Zhang,Jun-Hua Yao,Shang-Hai Lai,Bing-Jie Han,Wei Li,Bing Tang,Dan Wan,Yun-Jun Liu
In this article, the in vitro cytotoxicity of platycodin D was evaluated in human PC-12, SGC-7901, BEL-7402, HeLa and A549 cancer cell lines. PC-12 cells were sensitive to platycodin D treatment, with an IC 50 value of 13.5 ± 1.2 μM. Morphological and comet assays showed that platycodin D effectively induced apoptosis in PC-12 cells. Platycodin D increased the levels of reactive oxygen species (ROS) and induced a decrease in mitochondrial membrane potential. Platycodin D induced cell cycle arrest at the G0/G1 phase in the PC-12 cell line. Platycodin D can induce autophagy. In addition, platycodin D can down-regulate the expression of Bcl-2 and Bcl-x, and up-regulate the levels of Bid protein in the PC-12 cells. The results demonstrated that platycodin D induced PC-12 cell apoptosis through a ROS-mediated mitochondrial dysfunction pathway.
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TALANTA
·
2016
·
IF 4.035
Shu Min Lin,Shuo Geng,Na Li,Nian Bing Li,Hong Qun Luo
Mercury ion is one of the most hazardous metal pollutants that can cause deleterious effects on human health and the environment even at low concentrations. It is necessary to develop new mercury detection methods with high sensitivity, specificity and rapidity. In this study, a novel and green strategy for synthesizing D-penicillamine-capped copper nanoparticles (DPA-CuNPs) was successfully established by a chemical reduction method, in which D-penicillamine and ascorbic acid were used as stabilizing agent and reducing agent, respectively. The as-prepared DPA-CuNPs showed strong red fluorescence and had a large Stoke's shift (270 nm). Scanning electron microscopy, transmission electron microscopy , Fourier-transform infrared spectroscopy, fluorescence spectroscopy, and ultraviolet-visible spectrophotometry were utilized to elucidate the possible fluorescence mechanism, which could be aggregation-induced emission effect. Based on the phenomenon that trace mercury ion can disperse the aggregated DPA-CuNPs, resulting in great fluorescence quench of the system, a sensitive and selective assay for mercury ion in aqueous solution with the DPA-CuNPs was developed. Under optimum conditions, this assay can be applied to the quantification of Hg 2+ in the 1.0–30 μM concentration range and the detection limit (3σ/slope) is 32 nM. The method was successfully applied to determine Hg 2+ in real water samples.
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APPLIED CATALYSIS A-GENERAL
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2016
·
IF 4.012
Alberto Romero,Antonio Nieto-Márquez,Esther Alonso
Three different bimetallic Ru:Ni catalysts supported on a mesoporous silica MCM-48 were prepared by consecutive wet impregnations, with a total metal loading of ca. 3% (w w −1 ). Ru:Ni ratios spanned in the range of 0.15–1.39 (w w −1 ) and were compared with the corresponding monometallic Ni/MCM-48. The catalysts so prepared were characterized by X-Ray Diffraction, Transmission Electron Microscopy, adsorption/desorption of N 2 , Temperature Programmed Reduction, NH 3 − TPD and Atomic Absorption, and tested in the liquid phase hydrogenation of d -glucose into sorbitol in the temperature range 120–140 °C under 2.5 MPa of H 2 pressure. Bimetallic catalysts with Ru:Ni ratios higher than 0.45 enhanced the catalytic behavior of the monometallic Ni/MCM-48 in the reaction, increasing the reaction rate and showing complete selectivity to sorbitol by minimizing the production of mannitol. Ru:Ni/MCM-48 (0.45) was recovered from the reaction media and tested for three reaction cycles, showing good stability under the selected experimental conditions.
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ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Di-Di Xing,Yun-Wan Jia,De-Fu Li,Xiu-Li Wang,Yu-Zhong Wang
For improving the thermal stability, glass transition temperature (Tg), stiffness, and hydrophilicity of poly(ε-caprolactone) (PCL), two glucose-based bicyclic rigid structures, namely 1,4:3,6-dianhydrohexitols-D-glucidol (isosorbide, Is) and dimethyl 2,4:3,5-di-O-methylene-D-glucarate (glu-diester) have been introduced into PCL via chain extension. The two series of multiblock copolyesters obtained, PCL-b-PIS and PCL-b-PBG, have high number-average molecular weights in the range of 9.6 × 104 to 12.4 × 104 g mol–1 and small PDI values. The thermal and crystallization behaviors, hydrophilicity, as well as the mechanical properties of PCL-b-PIS and PCL-b-PBG have been well investigated. In comparison, the improved effect on thermal stability and Tg of PCL is more pronounced for PCL-b-PBG than for PCL-b-PIS. Both glucose-based units retard the crystallinity of PCL. However, the crystal structure and melting temperature of PCL remain unchanged. The rigidness of PCL is enhanced when glucose-based bicyclic units are introduced as reflected by the increasing storage modulus over all of the studied temperatures. The mechanical properties of PCL-b-PIS are better than those of PCL-b-PBG, especially for the samples containing 30 wt % sugar units. This can be due to the good compatibility of PIS with the PCL block. Although both Is and glu-diester enhance the hydrophilicity of PCL, the PCL-b-PBG copolyester always shows higher hydrophilicity than that of PCL-b-PIS in the whole composition.
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JOURNAL OF MOLECULAR CATALYSIS B-ENZYMATIC
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2013
·
IF 2.823
Jian-Yong Zheng,Sheng-Fan Wang,Yin-Jun Zhang,Xiang-Xian Ying,Yu-guang Wang,Zhao Wang
A chemoenzymatic methodology for the asymmetric synthesis of d -biotin intermediate lactone ((3a S , 6a R )-tetrahydro-1,3-dibenzylhexahydro-1 H -Furo[3,4-d] imidazole-2,4-dione) 1 has been demonstrated. The key step of the synthetic routes is Lipozyme RM IM catalyzed desymmetrization of meso-diols 3 . The highest enantiomeric excess ( e.e. > 98%) and yield (>90%) of the product was achieved with Lipozyme RM IM in Dioxane/Toluene (1:3, v/v) at 35 °C. Furthermore, Lipozyme RM IM showed an excellent operational stability, retaining above 80% of the initial activity after 10 cycles of reaction. d -Biotin intermediate lactone 1 was obtained subsequently by Jones oxidation, basic hydrolysis and lactonization.
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FLUID PHASE EQUILIBRIA
·
2015
·
IF 2.2
Xuzhao Yang,Jun Wang,Hao Song,Wenyuan Zou
Heat capacity of methyl α- d -glucopyranoside (α-MeG) was measured by differential scanning calorimetry at the temperatures ranging from 298.15 to 513.15 K. Melting point, enthalpy and entropy of fusion, enthalpy H T – H 298.15 K , and entropy S T -S 298.15 K were determined. Thermal decomposition of α-MeG was investigated using thermogravimetric analysis under pure nitrogen atmosphere. Ozawa-Flynn-Wall and ASTM models were used to calculate the activation energy and pre-exponential factor. Solubilities of α-MeG in methanol were measured within the temperature range of 293.15–318.15 K by using a synthetic method under atmospheric pressure. The modified Apelblat, λh , Wilson and NRTL models were applied to correlate the experimental data. The calculated results show good agreement with the experimental data and Wilson model is slightly more accurate than modified Apelblat, λh and NRTL models. The dissolution enthalpy, entropy, and Gibbs free energy were calculated by the Van't Hoff equation. The excess enthalpy of the solution can be evaluated by the λh model.
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Molecular Catalysis
·
2024
·
IF 3.9
Yun Zhang,Guangfei Qu,Zhishuncheng Li,Junhong Zhou,Rui Xu,Junyan Li
This research has made significant advancements in the field of high-value bio-oil production, specifically focusing on the synthesis of the rare sugar D-Allose. Notably, synthesizing D-Allose through cellulose pyrolysis has long been challenging due to its high synthetic difficulty, which has limited related studies. By employing a one-pot synthesis approach using Al x -Fe y nano-catalysts prepared through a unique cellulose pretreatment method, this experiment successfully achieved efficient generation of D-Allose during rapid pyrolysis. Systematic experimentation demonstrated that at 330 °C with the Al 1 -Fe 5 nano-catalyst, the yield of D-Allose from cellulose pyrolysis reached an impressive 50.69 %, accompanied by a detection of 14.35 % furfural in the bio-oil. This breakthrough not only significantly contributes to the high-value utilization of bio-oil but also provides robust support for further development in this area. Simultaneously, the success of this research extends beyond high-value bio-oil utilization and makes a substantial impact on both the scientific community and industry.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Qingxiu Wang,Weisong Liu,Lijing Chang,Kuncheng Zhang,Yanbing Shen,Lingling Zhang
L-guluronic acid, a patented drug with immunomodulatory and anti-inflammatory properties, is traditionally sourced from natural seaweed species or synthesized chemically. Both methods suffer from low selectivity and environmental concerns and there is a high demand to develop a green and efficient approach for L-guluronic acid production. Herein, we successfully developed a two-step enzymatic route to synthesize L-guluronic acid from D-glucose by two oxidases, glucose oxidase (GOx) and galactose oxidase (GOase). Due to the sluggish kinetics of GOase in catalyzing the oxidation of D-gluconic acid, rational design was implemented. Through molecular docking and iterative saturation mutagenesis, a variant, GOase T406R/K330R/Y329F, was obtained. The variant exhibited a remarkable 13-fold higher oxidation activity towards D-gluconic acid, reaching 7.8 U mg-1. The substitutions synergistically switch the D-gluconic acid molecule to a favorable conformation and facilitate the specific activation of the primary alcohol group at C6 position. In a cascade reaction, complete conversion of 40 mM D-glucose to L-guluronic acid was achieved in 2 h with 100% selectivity, presenting a promising and green bio-manufacturing strategy for the scalable production of L-guluronic acid.
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Food Bioscience
·
2024
·
IF 4.8
Han Zhang,Zhen Sun,Xinling Du,Qianqian Cheng,Fuchun Ji,Zishen Nie,Julei Zhan,Zhouping Wang,Aitao Li,Irina Delidovich,Yu Xia
d- Allulose is a rare sugar with multiple physiological functions whose application has been restricted by low conversion rate, weak thermostability of the used enzymes, and complex production. In this study, a simplified multienzyme cascade strategy was designed for biosynthesis of d- allulose from d- glucose, and a detailed investigation of the crucial enzyme allulose 6-phosphate phosphatase was conducted. Under optimized conditions, the yield of d- allulose reached 4.12 ± 0.14 and 80.20 ± 3.20 mmol/L using 10.0 and 200.0 mmol/L d- glucose as substrate, respectively. Furthermore, the influence of various factors on the cooling crystallization of d- allulose was investigated, and the crystallization process was optimized. Consequently, a crystallization recovery rate of 77.43% ± 2.50% and a purity of 98.70% ± 0.05% were achieved. Moreover, the obtained crystals of d -allulose were characterized by XRD, TGA-DSC, and optical microscopy.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Shiyong Mou,Siyuan Liu,Weidong Dai,Yanjuan Sun,Fan Dong
Electrochemical oxidative amidation (EOA) strategies offer a sustainable and potentially promising route for amide synthesis. However, the efficiency and activity of catalysts under oxidative conditions are highly dependent on noble metals. Herein, we present our experimental findings and fundamental understanding that fluorine-doped Nb 2 O 5 nanosheet arrays on carbon paper (F-Nb 2 O 5 /CP) serve as an efficient and robust non-noble catalyst for the electrochemical synthesis of formamide from ammonia and methanol under ambient conditions. In 0.5 M KHCO 3 solution, this catalyst achieved a high Faradaic efficiency of 52.0 %, with an N selectivity of 79.1 % at 1.5 V versus Hg/HgO electrode. The catalyst exhibited remarkable stability, maintaining its performance over 120 h. By integrating in-situ spectroscopy studies with density functional theory calculations, we revealed that fluorine doping induces a shift in the d-band center of the Nb site. This shift alters the adsorption behavior of OH - and *NH 2 intermediate on the F-Nb 2 O 5 (100) surface, thereby effectively lowering the C-N coupling energy barrier, and boosting the production of formamide.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Long Haoyu,Zhang Xidong,Zhang Zhenyi,Zhang Jianjun,Yu Jiaguo,Yu Huogen
The H 2 -evolution kinetics play a pivotal role in governing the photocatalytic hydrogen-evolution process. However, achieving precise regulation of the H-adsorption and H-desorption equilibrium (H ads /H des ) still remains a great challenge. Herein, we propose a fine-tuning d - p hybridization strategy to precisely optimize the H ads /H des kinetics in a Ni-B x modified CdS photocatalyst (Ni-B x /CdS). X-ray absorption fine-structure spectroscopy and theoretical calculations reveal that increasing B-atom amount in the Ni-B x cocatalyst gradually strengthens the d - p orbital interaction between Ni 3 d and B 2 p , resulting in a consecutive d -band broadening and controllable d -band center on Ni active sites. The above consecutive d -band optimization allows for precise modulation of the H ads /H des dynamics in the Ni-B x /CdS, ultimately demonstrating a remarkable H 2 -evolution activity of 13.4 mmol g -1 h -1 (AQE = 56.1 %). The femtosecond transient absorption spectroscopy further confirms the rapid electron-transfer dynamics in the Ni-B x /CdS photocatalyst. This work provides insights into the optimal design of prospective H 2 -evolution catalysts.
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