HYDROMETALLURGY
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2026
·
IF 6.3
Gengjin Zhang,Yanfang Huang,Longfei Jia,Tianze Chen,Yizhuang Wang,Shengpeng Su,Wenjuan Wang,Hu Sun,Guihong Han
Novel peroxo-complexation strategy was used to purify Nb-rich solution. • NbOF 5 2− transformation to NbO 2 F 5 2− greatly lowers its binding energy with MIBK. • Selectivity coefficient for Sb over Nb was enlarged by over 2300 times. • Nb 2 O 5 product met the high-purity specifications regarding Ta and Sb impurities. The efficient separation of Ta and Sb from Nb in hydrometallurgical processes remains a significant challenge due to their similar chemical behaviors. In this study, a novel peroxo-complexation strategy was introduced to enhance the selectivity of methyl isobutyl ketone (MIBK) extraction in an HF-H 2 SO 4 system. With the addition of H 2 O 2 , the extraction efficiencies of Ta and Sb reached 99.6% and 99.7%, respectively, while the co-extraction of Nb was only 2.32%. The selectivity coefficients of Sb/Nb and Ta/Nb significantly increased from 0.63 and 34.7 to 1461 and 6501, respectively. Stepwise stripping using H 2 SO 4 and pure water effectively recovered Nb and Ta/Sb from the loaded organic phase. Raman spectroscopy and quantum chemical calculations elucidated the mechanism of the enhanced separation selectivity. The peroxo-ligand selectively coordinates with Nb to transform it from NbOF 5 2− to NbO 2 F 5 2− , thereby weakening the negative surface potential of the fluorine atoms bonded to Nb. The binding energy between Nb ions and MIBK decreases from −172 kJ mol −1 to −104 kJ mol −1 , and thus the disparity in the affinity of Nb ions and Ta/Sb ions for MIBK is magnified. Overall, this peroxo-coordination approach provides an efficient and simple pathway for the effective purification of Nb solutions. Download: Download high-res image (176KB) Download: Download full-size image
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ChemSusChem
·
2023
·Vol. 16
·期 12
·e202300133
·
IF 8.4
Changqu Lin,Hao Yang,Xin Gao,Yue Zhuang,Caojian Feng,Hongli Wu,Haifeng Gan,Fei Cao,Ping Wei,Pingkai Ouyang
Graphical An alkali catalytic system for the selective conversion of N -acetyl- d -glucosamine (NAG) into unsubstituted 3-acetamidofuran (3AF) via retro-aldol condensation has been developed. 3AF with 73.9 % yield is obtained in the presence of a ternary Ba(OH) 2 −H 3 BO 3 −NaCl catalytic system. Aminofurans are widely used in drug synthesis as aromatic modules analogous to aniline. However, unsubstituted aminofuran compounds are difficult to prepare. In this study, a process for the selective conversion of N -acetyl- d -glucosamine (NAG) into unsubstituted 3-acetamidofuran (3AF) is developed. The yield of 3AF from NAG catalyzed by a ternary Ba(OH) 2 −H 3 BO 3 −NaCl catalytic system in N -methylpyrrolidone at 180 °C for 20 min can reach 73.9 %. Mechanistic studies reveal that the pathway to 3AF starts with a base-promoted retro-aldol condensation of the ring-opened NAG, affording the key intermediate N -acetylerythrosamine. Judicious selection of the catalyst system and conditions enables the selective conversion of biomass-derived NAG into 3AF or 3-acetamido-5-acetylfuran.
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BIOELECTROCHEMISTRY
·
2023
·
IF 5
Zheng-Zhi Yin,Zixuan Liu,Min Zhou,Xu Yang,Guojun Zheng,Hongyu Zhang,Yong Kong
Sensitive detection of severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2) spike protein (S protein) is of significant clinical importance in the diagnosis of COVID-19 pandemic. In this work, a surface molecularly imprinted (SMI) electrochemical biosensor is fabricated for the detection of SARS-CoV-2 S protein. Cu 7 S 4 -Au is used as the built-in probe and modified on the surface of a screen-printed carbon electrode (SPCE). 4-Mercaptophenylboric acid (4-MPBA) is anchored to the surface of the Cu 7 S 4 -Au through Au–SH bonds, which can be used for the immobilization of the SARS-CoV-2 S protein template through boronate ester bonds. After that, 3-aminophenylboronic acid (3-APBA) is electropolymerized on the electrode surface and used as the molecularly imprinted polymers (MIPs). The SMI electrochemical biosensor is obtained after the elution of the SARS-CoV-2 S protein template with an acidic solution by the dissociation of the boronate ester bonds, which can be utilized for sensitive detection of the SARS-CoV-2 S protein. The developed SMI electrochemical biosensor displays high specificity, reproducibility and stability, which might be a potential and promising candidate for the clinical diagnosis of COVID-19.
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JOURNAL OF MOLECULAR LIQUIDS
·
2023
·
IF 6
Guangzhi Xu,Zhuoheng Tu,Xingbang Hu,Mian Li,Xiaomin Zhang,Youting Wu
The utilization of biomass instead of fossil resources for the synthesis of various chemicals is regarded as one of the most important strategies to realize sustainable and environmentally-friendly chemical industry. The design and development of suitable catalysts for biomass conversion are of particular significance. Herein, ionic buffering biphase systems (IBBSs) consisting of ionic buffering catalysts (IBCs) and an organic phase as extractant are proposed and developed for the dehydration of xylose and hemicellulose to furfural (FF). The systems can efficiently catalyze the conversion of xylose and hemicellulose to FF and significantly reduce the use of NaCl. High FF yields of 76.4% or 85.1% were realized with almost complete conversion of hemicellulose or xylose. The IBBSs have advantages of simple preparation, thermal stability, and low cost, not to mention the facts that they enable both the excellent extraction of FF product from aqueous phase to oil phase and the easy recycling of ionic buffering catalyst. This work offers a new strategy of designing and developing catalytic reaction-separation coupling systems for the efficient conversion of xylose and hemicellulose to FF.
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Biomass Conversion and Biorefinery
·
2023
·
IF 4
Wu Jinsheng,Yang Ruinan,Zhao Shiqiang,Chen Wei,Chen Zhiyong,Chang Chun,Wu Haoran
The development of mild strategies to transform of fructose to prepare high-purity 5-hydroxymethylfurfural (HMF) is of great significance for biomass valorization, and the design of an efficient catalytic approach is crucial. Herein, a mild catalytic strategy was developed to achieve the preparation of high-purity HMF from fructose over Amberlyst-15 catalyst in a water-methyl isobutyl ketone (MIBK) biphasic system under atmospheric pressure and lower temperature (90 °C). The catalytic system was optimized and analyzed by response surface methodology and kinetics study. Results indicated that a 46.6% yield of HMF could be obtained under optimal conditions: 80 wt% Amberlyst-15 catalyst, the mass ratio of MIBK to H 2 O 10, and the reaction time of 7 h. Furthermore, a simple and efficient purification strategy of HMF was established. High purity (99.0%) and recovery rate (65.5%) of HMF were obtained. This work provides an efficient catalytic strategy to produce high-purity HMF from fructose under atmospheric pressure and lower temperature.
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JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Pengshuai Zhang,Haiyan Luo,Lan Cui,Jixiu Deng,Shiyu Xie,Danfeng Liu,Shuqi Wang,Xiaoying Si,Zichao Wang,Yameng Wan,En Zhang,Xing Li,Lu Zhang
Solid-liquid equilibrium solubility of artemisinin (ART) Form I in twelve mono-solvents namely N, N-dimethylformamide (DMF), oxolane (THF), n -propanol (NPA), 4-methylpentan-2-one (MIBK), ethyl formate (EF), butyl acetate (BAC), 2-ethoxyethanol (EGEE), 1,4-Dioxane, 2-methoxyethanol (EGME), 2-propoxyethanol (EGPE), propyl acetate (NPAC) and 2-butoxyethanol (EGBE) from 283.15 K to 323.15 K were determined by a laser dynamic method under 0.1 MPa. The minimum solubility of ART (Form I) was found in NPA at 283.15 K (0.004541), the maximum mole fraction solubility of ART (Form I) was observed as 0.2523 in DMF at 323.15 K. At the temperature of 298.15 K, the experimental mole fraction solubility order of ART Form I in the tested solvents was DMF (0.1559) > 1,4-Dioxane (0.09117) > THF (0.08301) > MIBK (0.05054) > EF (0.04902) > NPAC (0.03860) > BAC (0.03658) > EGME (0.02031) > EGEE (0.01859) > EGPE (0.01817) > EGBE (0.01689) > NPA (0.007185). The solubility behavior was computationally correlated by Margules model, Wilson model, NRTL model, NRTL-SAC model, Buchowski-Ksiazczak λh model and UNIQUAC model, the total RMSD was no>0.025 in the selected models. With the help of Hansen solubility parameters (HSPs) analysis, molecular similarities of ART (Form I) in twelve mono-solvents were investigated. Besides, Hirschfeld surface analysis (HSs) was considered to evaluate the intermolecular interaction of artemisinin. Moreover, thermodynamic properties including Δ mix H , Δ mix G , Δ mix S , lnγ 1 , l n γ 1 ∞ of ART (Form I) in the selected solvents were estimated. All the negative Δ mix G and positive Δ mix S values indicated that the mixing process were spontaneous and entropy-increasing.
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Catalysts
·
2022
·Vol. 13
·期 1
·37
·
IF 4.501
Qizhen Yang,Zhengyu Tang,Jiale Xiong,Yucai He
Valorization of the abundant renewable lignocellulose through an efficient chemoenzymatic strategy to produce the furan-based platform compounds has raised great interest in recent years. In this work, a newly prepared sulfonated tin-loaded rice husk-based heterogeneous chemocatalyst UST-Sn-RH was utilized to transform corncob (75.0 g/L) into furfural (72.1 mM) at 170 °C for 30 min in an aqueous system. To upgrade furfural into furfuryl alcohol, whole cells of recombinantE. coli KPADH harboring alcohol dehydrogenase were employed to transform corncob-derived furfural into furfuryl alcohol at 30 °C and pH 7.5. In the established chemoenzymatic cascade process, corncob was efficiently transformed to furfuryl alcohol with a productivity of 0.304 g furfuryl alcohol/(g xylan in corncob). In general, biomass could be efficiently valorized into valuable furan-based chemicals in this tandem reaction with the chemocatalyst (bio-based UST-Sn-RH) and the biocatalyst (KPADH cell) in an aqueous system, which has potential application.Keywords:furfural;furfuryl alcohol;heterogeneous catalyst;chemoenzymatic strategy
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Frontiers in Bioengineering and Biotechnology
·
2023
·
IF 5.7
Huang Lizhen,Bian Zelun,Li Dalin,Cheng Xin,Luo Xiaolin,Shuai Li,Liu Jing
Biobased furfural is a sustainable alternative to petrochemical intermediates for bulk chemicals and fuel production. However, existing methods for the conversion of xylose or lignocelluloses in mono-/bi-phasic systems to furfural involve non-selective sugar isolation or lignin condensation, limiting the valorisation of lignocelluloses. Herein, we used diformylxylose (DFX), a xylose derivative that is formed during the lignocellulosic fractionation process with formaldehyde protection, as a substitute for xylose to produce furfural in biphasic systems. Under kinetically optimized conditions, over 76 mol% of DFX could be converted to furfural in water-methyl isobutyl ketone system at a high reaction temperature with a short reaction time. Finally, isolation of xylan in eucalyptus wood as DFX with formaldehyde protection followed by converting DFX in a biphasic system gave a final furfural yield of 52 mol% (on the basis of xylan in wood), which was more than two times of that without formaldehyde. Combined with the value-added utilization of formaldehyde-protected lignin, this study would enable the full and efficient utilization of lignocellulosic biomass components and further improve the economics of the formaldehyde protection fractionation process.
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高影响因子
FOOD SCIENCE AND BIOTECHNOLOGY
·
2023
·Vol. 32
·期 7
·903-909
·
IF 2.9
He Yangzheng,Chen Li,Liu Wenqun,Deng Ze-yuan,Li Jing
In this study, gas chromatography–mass spectrometry (GC–MS) coupled with Partial least squares Discriminant Analysis (PLS-DA) was used to analyze the volatiles in Chinese breast milk from different cities (Wuhan, Qingdao and Hohhot) and different lactation stages (colostrum and mature milk). The results showed that breast milk contained 122 volatile substances in 9 major groups, with the largest number of olefins (36) and the highest content of acids. The different volatile compounds of breast milk in three cities were heptanal, 2-pentylfuran, (E)-2,4-decadienal, (E)-2-heptenal, (E)-2-nonenal and 1-octen-3-one, colostrum and mature milk were (E)-2-heptenal, (E)-2-decenal, lauric acid, n -decanoic acid, (E)-2-nonenal and octanoic acid. This study might provide scientific data for the development and optimization of formulas that were more suitable for the health of Chinese infants.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2022
·
IF 4.831
Jialu Shen,Guoqing Chen,Zichen Yang,Yamin Wu,Chaoqun Ma,Lei Li,Taiqun Yang,Jiao Gu,Hui Gao,Chun Zhu
The accurate detection of fructose in human urine can help prevent and screen for diseases such as fructokinase deficiency and hereditary fructose intolerance. Surface-enhanced Raman spectroscopy (SERS) is an analytical technique with selectivity and high sensitivity, which has been widely applied to the detection of targets with complex backgrounds. In this work, 4-mercaptophenylboronic acid (4-MPBA) was modified on the surface of silver nanoparticles (AgNPs) under mild conditions to obtain a boronic acid-functionalized SERS substrate for the detection of fructose in artificial urine. The detection mechanism was based on the deboronization reaction of 4-MPBA on the surface of AgNPs, which was induced by fructose, and the Raman signal of the generated thiophenol (TP) molecules was significantly enhanced by the silver nanoparticles, with a linear increase in SERS peak intensity at 1570 cm −1 . We achieved the detection limits of 0.084 µmol/L in water and 0.535 µmol/L in urine by this method. The relative standard deviation (RSD) in the recovery experiments of urine ranged from 1.01 % to 2.22 %, and the whole detection time was less than 10 min, which indicated that this method is highly reliable for fructose detection and has a good prospect in bioassay and clinical medicine.
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INDUSTRIAL CROPS AND PRODUCTS
·
2022
·
IF 6.449
Miao Zuo,Qiang Niu,Yanzhong Zhu,Sijin Li,Wenlong Jia,Zheng Zhou,Xianhai Zeng,Lu Lin
This study prepared a series of biochar-based catalysts using different parts of Larix principis-rupprechtii as feedstock , to promote the 5-Hydroxymethylfurfural (HMF) synthesis from glucose and fructose. Sulfonated biochar showed high converting efficiency of fructose in both dimethyl sulfoxide (DMSO) and aqueous-natural deep eutectic solvent (A-NADES) reaction systems, with HMF yield of 96.3% prepared from the pine needle-derived acidic catalyst under mild condition. Bifunctional acidic biochar catalysts containing both Lewis acid and Brønsted acid functional groups could effectively enhance the glucose conversion with 57.2% of the HMF yield obtained in A-NADES. After the detailed characterization of the biochar catalysts, the potential mechanism of the bifunctional catalyst for the synthesis of HMF by conversion of glucose and fructose was proposed. The possible promoting mechanism of carbohydrate conversion by A-NADES through intermolecular hydrogen bonding was also explored.
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FUEL
·
2023
·
IF 7.4
Guangzhi Xu,Zhuoheng Tu,Xingbang Hu,Mian Li,Xiaomin Zhang,Youting Wu
Furfural (FF) is an important platform molecule originated from biomass, but it’s synthesis through the traditional acid-catalyzed dehydration reaction of xylose and hemicellulose remains problematic due to the poor activity and equipment corrosion. Therefore, a series of [HSO 4 ]-based protic Brønsted acidic ionic liquids (BAILs) are employed as green catalysts to achieve efficient and sustainable preparation of FF from xylose or hemicellulose in this work. Furfural yields of 75.4% or 80.4% were achieved under optimal operating conditions with [Hpy][HSO 4 ] as catalyst, hemicellulose or xylose as substrates, higher than those catalysed with most ionic liquids reported so far. The chemical structures of BAILs were confirmed by NMR and FT-IR spectroscopy, and the Hammett acidity ( H 0 ) were determined using UV–vis spectroscopy with 4-nitroaniline as probe. The acidity of BAILs were tuned through methyl substitution on the pyridinium ring, and its effect on the catalysis performance was investigated. In addition, the reaction constants and the corresponding activation energies of BAILs for dehydration of xylose to FF were calculated by kinetic equations. Overall, the highly efficient catalysis performance, good recyclability and low cost enables [Hpy][HSO 4 ] to be potentially applied for large-scale preparation of FF.
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