ACS Catalysis
·
2023
·
IF 12.9
Luyao Guo,Xiaoyan Liu,Ziang Zhao,Ronghe Lin,Yu Meng,Xinzheng Ma,Yihui Li,Xiaoling Mou,Li Yan,Hejun Zhu,Yunjie Ding
Nanostructured bimetallic Pt–Bi catalysts are designed by defect engineering of N-doped carbons as the hosts. The optimal catalyst delivers good yields (>98%) in the direct oxidation of C5–C9 linear α-alcohols to corresponding fatty acids, significantly outperforming activated carbon-supported benchmarks and rivaling the state-of-the-art systems. A combined kinetic and computational study on n-heptanol oxidation as a model reaction unveils the kinetic and thermodynamic origins of the better performance of the PtBi alloy than neat or Bi-modified Pt(111) surfaces. Structure–performance correlations further identify that the metal particle size, surface Bi/Pt ratio, and strong basicity strongly influence the catalyst performance in alcohol oxidation. The creation of nitrogen defects facilitates the formation of the surface PtBi alloy and brings strong basicity, accounting for the boosted performance. These findings enable a step closer toward the manufacture of valuable fatty acids from abundant coal by coupling the advanced oxidation with the recently piloted higher alcohol synthesis via the Co–Co2C-catalyzed Fischer–Tropsch reaction.
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Biomed Research International
·
2021
·
IF 3.411
Qin Hu,Shu Zhang,Jun Zhu,Lina Yin,Suping Liu,Xiaowei Huang,Guihao Ke
Endometrial cancer (EC) is a common gynecological malignancy worldwide whose therapy mainly depends on chemotherapy. In past years, an increasing number of studies indicate that hollow MnO2 could serve as a nanoplatform in the drug delivery system. The Brucea javanica oil emulsion (BJOE) has been illustrated to play a vital role in cancers. However, knowledge about the combined effect of H-MnO2-PEG/BJOE in endometrial cancer remains ambiguous up to now. In the present work, we prepared a drug-delivery vector H-MnO2-PEG by chemical synthesis and found that H-MnO2-PEG significantly inhibited cell proliferation in endometrial cancer cells. Moreover, the combination of H-MnO2-PEG/BJOE could repress cell proliferation more efficiently and promote cell apoptosis. Mechanistically, we found that BJOE exerted its role as a promoter of endometrial apoptosis by regulating relative protein expressions. In general, the present study demonstrates that H-MnO2-PEG functions as a critical vector in the tumor microenvironment of endometrial cancer and the significant effect of H-MnO2-PEG/BJOE on cancer cells, suggesting a new paradigm for the treatment of endometrial cancer.
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Journal of Cleaner Production
·
2021
·
IF 9.297
Ya Gao,Tong Yue,Wei Sun,Dongdong He,Chenglong Lu,Xinzhuang Fu
Acid recovering and iron recycling from pickling waste acid are the desired goal of the steel mills for current ecological requirements and economic benefit. This study proposed a novel method to treatment the pickling waste acid using extraction separation of ferric chloride and hydrochloric acid , following by the spray pyrolysis of ferric chloride stripping liquor. Comparing the Ruthner method, the significant technical advantages of this method is the lower treatment load and operating costs for the spray pyrolysis process, attributing to the reuse of most hydrochloric acid without iron powder neutralizing. Different extractants (TBP, CYC, IA, OA, and PA) are compared to extract ferric ion from high-concentration hydrochloric acid solution and the optimum conditions are researched. Spectroscopic analysis is performed to characterize iron state in extractants. For the stripped solution, spray pyrolysis is employed to produce high-purity Fe 2 O 3 fine particles, meanwhile hydrochloric acid is recovered for following pickling procedure. The results showed that the effect of CYC under lower O/A ratio was better than that of TBP, and the opposite occurred at higher ratios. Three-stage extraction efficiency can reach over 80% at O/A = 2:1. The final O/A ratio of 1:1 was chosen for the stripping of iron-loaded extractants. Raman and UV–visible found that it was [FeCl 4 ] - anion that existed in Fe-loaded TBP and CYC. Spray pyrolysis at 1000 °C can obtain fine pure Fe 2 O 3 and hydrochloric acid. Eventually, a feasible technological process was put forward to recycle all chemicals and achieve zero emission of water and solid waste in the whole process.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2021
·
IF 3.178
Xuemei Zhang,Feiyan Yang,Chungui Jian,Hongwei Wang,Wangxin Kong,Guangjin Shangguan,Meifang Xia
Liquid-liquid equilibrium (LLE) data for the ternary system of (2-methyl-2-butanol + water + n -octanol) were determined at 303.15 K, 313.15 K, and 323.15 K under atmospheric pressure. The Hand equation, the Othmer-Tobias equation, and the mass balance between the feed and the conjugated phases were used to test the reliability of the experimental LLE data. The results show that the correlation coefficients ( R 2 ) of the equations are close to 1, and the relative error of mass balance is less than 0.5%. The selectivity ( S ) was used to evaluate the capacity of n -octanol to extract 2-methyl-2-butanol from the water, which is much greater than 1. Furthermore, S decreases with the mass fraction of 2-methyl-2-butanol in the aqueous phase and increases with equilibrium temperature. The NRTL and UNIQUAC models were applied to correlate the experimental LLE data, and the binary interaction parameters were obtained. The root-mean square deviations (RMSDs) for the two models obtained are less than 1.1%.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2021
·
IF 3.178
Hao Wang,Nianzu Zhang,Xiaopo Wang
In this work, the density and viscosity data for binary mixtures of dimethyl carbonate with 1-heptanol, 1-octanol, 1-nonanol, and 1-decanol were presented from 303.15 K to 333.15 K at atmospheric pressure over different concentration ranges. The density and viscosity measurement was carried out based on the vibrating-tube densimeter and Ubbelohde capillary viscometer, respectively. Derived properties, such as excess molar volumes and viscosity deviations, were calculated from the experimental values, and were correlated based on the Redlich-Kister equation. In addition, excess molar volumes and viscosity deviations of the studied mixtures were analyzed and compared with other DMC/1-alcohols mixtures reported in the literatures.
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Journal of Environmental Sciences
·
2021
·
IF 5.565
Qiongyang Zhou,Ying Wang,Xiaochen Wang,Yuanqi Bai
Aiming to investigate the impacts of n -octanol addition on the oxidation reactivity, morphology and graphitization of diesel exhaust particles, soot samples were collected from a four-cylinder turbocharged diesel engine fueled with D100 (neat diesel fuel), DO15 (85% diesel and 15% n -octanol, V/V ) and DO30 (70% diesel and 30% n -octanol, V/V ). All tests were conducted at two engine speeds of 1370 and 2150 r/min under a fixed torque of 125 N·m. The soot properties were characterized by thermogravimetric analyzer (TGA), transmission electron microscopy (TEM) and Raman spectroscopy (RS). The higher volatile organic fraction content, lower soot oxidation temperatures and lower activation energy from TGA results indicated that both the increasing n -octanol concentration and engine speed enhanced the soot oxidation reactivity. Additionally, quantitative analysis of TEM images showed that the soot derived from DO30 had the smallest primary particle diameters and fractal dimension, followed by those of soot produced by DO15 and D100. The RS results demonstrated that the n -octanol addition and higher engine speed led to a larger D1-FWHM (D1-full width at half maximum), A D1 /A T (area ratio of D1 band and the total spectral) and A D3 /A T (area ratio of D3 band and the total spectral) as well as a smaller L a (crystallite width), revealing a lower degree of graphitization. Furthermore, the correlations between characterization parameters of soot properties and reactivity were nonlinear.
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ChemNanoMat
·
2021
·Vol. 7
·期 5
·553-560
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IF 3.154
Meihua Gao,Zhiyin Yao,Na Du,Quanhua Deng,Lijing Liu,Jianqiang Liu,Wanguo Hou
Graphical Sodium monododecylphosphate can form vesicles in alcohol/water mixtures. The vesicles show remarkable stability but are metastable in thermodynamics. Sodium monododecylphosphate (SDP), a typical single-chain amphiphile (SCA), exhibits extremely low solubility in water, which limits the investigation on its aggregation behavior. In the current work, we introduced short- and medium-chain alcohols into the SDP-water system to improve its solubility. An isotropic phase was found to be formed in the presence of alcohol with a suitable dielectric constant (11–25) or alkyl chain (2–7 carbons). In addition, vesicular, dendritic, and micellar structures were identified in the isotropic phase, depending on the composition of the SDP/alcohol/H 2 O ternary systems. The structure, stability, permeability, and formation mechanism of the vesicles formed in the SDP/ n -pentanol (NPT)/H 2 O system were investigated. The vesicles have a unilamellar structure, with size-selective permeability. They show remarkable stability upon long-term storage, exposure to high temperature, and freeze-thawing cycles, but are metastable in thermodynamics. The hydrogen bonding between SDP molecules plays an important role in the formation of vesicles. Furthermore, the SDP/NPT/H 2 O vesicles were used to construct three spatially segregated enzyme-loaded compartments to support a cascade enzyme reaction. The chemical signal transduction among the enzyme-loaded vesicles was achieved. This study provides a deeper understanding of the features of SDP vesicles and demonstrates their potential applications such as in biomembrane mimicking and micro-reactors.
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TALANTA
·
2021
·
IF 6.057
Hua-Ming Xiao,Shuai Zhao,Ru-Ting Fan,Dilshad Hussain,Xian Wang
Short-chain fatty alcohols (SCFAs) are one of the reactants for the production of biodiesels. The SCFA residues at the trace level have a significant impact on biodiesel quality. However, the analysis of SCFAs in aged biodiesels has not been reported so far, which is probably due to the unavailability of an appropriate analytical method for the simultaneous determination of SCFAs. Herein, we developed a novel analytical approach with high sensitivity and selectivity for the simultaneous identification and determination of SCFAs in seed oil and biodiesel samples during the simulated real-time aging by stable isotope labeling assisted liquid chromatography-mass spectrometry (SIL-LC-MS). A pair of isotope labeling reagents, pyridine (Py) and [ 2 H 5 ]pyridine ([ 2 H 5 ]Py), were used to label SCFAs in biodiesels and standards, respectively. The [ 2 H 5 ]Py labeled SCFAs were used as internal standards to compensate for the detection of variances. The simultaneous determination of SCFAs was performed by LC-MS with an improved detection selectivity and sensitivity. The limits of detection (LODs) values were ranged from 0.2 to 0.5 ng mL −1 for the investigated SCFAs. Good linearity was observed in the studied ranges (R 2 > 0.99) and good precision with relative standard deviations (RSDs) was in the range of 4.9–18.1%. Average recoveries were obtained in the range of 80.3%–115.4%. The matrix effects were in the range of 70.0–104.3%. The validated SIL-LC-MS method was applied to the simultaneous quantitative analysis of SCFAs in seed oil and biodiesel samples and the LC-MS analysis could be done within 3 min. The formation mechanism of SCFAs in aged oil and biodiesel samples was also investigated by this method. The results suggest that SCFAs were formed and their composition changed during the simulated real-time aging of long-chain fatty acid (LCFA), long-chain fatty acid methyl ester (FAME), seed oil, and biodiesels. Moreover, we found that the formation of 1-pentanol and 1-hexanol was associated with the number and position of double bonds in LCFAs and FAMEs .
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Catalysts
·
2021
·Vol. 11
·期 4
·499
·
IF 4.146
Tiefeng Wang,Xu Li,Xiaosheng Zhang,Jinxiang Dong
Dimethyl-carbonate (DMC) is a green carboxymethylation agent for synthesis of the versatile long-chain alkyl carbonates through base-catalyzed transesterification with aliphatic alcohols. Herein, we demonstrated the facile preparation of a novel heterogeneous base catalyst α-KMgPO4using commercially cheap metal salts via hydrothermal-calcination procedure. The combination of temperature programmed desorption (TPD) and FTIR measurements with CO2pre-adsorbed revealed the presence of weak and medium base sites on α-KMgPO4. Furthermore, α-KMgPO4catalyzed transesterification of DMC and n-octanol was performed in a sealed-vessel reactor (Monowave 50). The results show that the reaction was completed in only 10 min with the 97.5% conversion of n-octanol and >99% selectivity to asymmetric methyl-octyl carbonate under the optimal conditions. Additionally, the possible catalytic mechanism is proposed. As an extended contribution, the tribology performance of the asymmetric methyl-alkyl carbonates was further evaluated.Keywords:catalyst;α-KMgPO4;transesterification;asymmetric carbonates;Monowave 50 reactor
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JOURNAL OF CHROMATOGRAPHY A
·
2020
·
IF 4.049
Xiao Yu,Xinlin Li,Sunzhao You,Yuhang Shi,Ruiqin Zhu,Ying Dong,Chuixiu Huang
Separation of antipsychotic drugs from whole blood and urine is of great importance for clinic and forensic laboratories. In this work, chlorprothixene, haloperidol and risperidone representing the first and second generations of antipsychotic drugs were studied. Among them, chlorprothixene and risperidone were investigated for the first time by electromembrane extraction (EME). After the screening, 2-nitrophenyl octyl ether (NPOE) was used as the supported liquid membrane (SLM). The EME performance for spiked water (pH 2), whole blood and urine was tested and optimized individually. Using NPOE and 60 V, efficient EME was achieved from urine and whole blood with trifluoroacetic acid as the acceptor solution. The equilibrium time required for EME was dependent on the sample matrices. The steady-state of EME was reached in 30 min and 20 min for whole blood and urine, respectively. At steady-state, the EME recoveries of the targets from different sample matrices were satisfactory, and were in the range of 74%-100%. The proposed EME approach combined with liquid chromatography-tandem mass spectrometry (LC-MS/MS) was evaluated using whole blood and urine. The obtained linearity was 1-200 ng mL −1 , and the coefficient of determination (R 2 ) was ≥ 0.9853 for haloperidol and ≥ 0.9936 for chlorprothixene and risperidone. The limit of detection (LOD) and accuracy for all the targets ranged from 0.2-0.6 ng mL −1 and 102%-110%, respectively, and the repeatability at low (1 ng mL −1 ), medium (10 ng mL −1 ) and high (200 ng mL −1 ) concentration was ≤ 12% (RSD). Finally, the validated approach was successfully used to determine chlorprothixene, risperidone and haloperidol in whole blood and urine from rats, which were treated with chlorprothixene, risperidone and haloperidol at low therapeutic dose, respectively.
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Nano Research
·
2021
·Vol. 14
·期 8
·2846-2852
·
IF 8.897
Wang Dongdong,Al-Mamun Mohammad,Gong Wanbing,Lv Yang,Chen Chun,Lin Yue,Wang Guozhong,Zhang Haimin,Zhao Huijun
The cyclopentanone and derivatives are a class of crucial fine chemicals for various industries and currently produced by conventional petrochemical synthetic routes. Here, we demonstrated a new synthetic approach to directly fabricate N-doped carbon nanotube (N-CNTs) networks with confined Co nanoparticles from Co 2+ -impregnated bulk g-C 3 N 4 as high performance hydrogenation rearrangement (HR) catalyst to efficiently convert a wide spectrum of biomass-derived furanic aldehydes to the corresponding cyclopentanones in water under a record-low H 2 pressure of 0.5 MPa and mild temperature. We unveiled a Co-catalysed bulk g-C 3 N 4 decomposition/carbonisation CNTs formation mechanism. A new HR pathway was also unveiled.
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JOURNAL OF MOLECULAR LIQUIDS
·
2020
·
IF 5.065
Xiao-Hong Fan,Li-Tao Wang,Yuan-Hang Chang,Juan-Yan An,Ya-Wei Zhu,Qing Yang,Dong Meng,Yu-jie Fu
Establishing an efficient and eco-friendly extraction method of bioactive ingredients from plant materials is highly needed to insure a better human health by combating different diseases. In this work, a two-phase system formed by green and recyclable menthol-based hydrophobic deep eutectic solvent (DES) aqueous was synthesized and evaluated its application for simultaneous extraction of seven main target taxanes in the Taxus chinese needles. The formation of micelles from two-phase system in the menthol-based DES aqueous simultaneously enhanced the mass transfer and enrichment for target taxanes. Under the optimal conditions of menthol/1-butanol ratio 1:1 (mol/mol), water content 50%, solid-liquid ratio 1:30 g/mL, extraction time 30 min and ultrasonic power 250 W, the extraction yields of seven main taxanes were 1.27–2.65 folds higher than the conventional organic solvents. The recovery yields after enrichment with the two-phase system of the menthol-based DES aqueous were higher than 95.31%. Furthermore, the menthol-based DES aqueous could be recycled at least three times with perfect extraction efficiency for target compounds. This work proved that the natural menthol-based DES aqueous solution is an effective and non-toxic green extraction solvent, which has the potential to effectively extract phytochemicals from plant materials in the future.
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