JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2019
·
IF 4.978
Huai Liu,Xuejuan Cao,Ting Wang,Junnan Wei,Xing Tang,Xianhai Zeng,Yong Sun,Tingzhou Lei,Shijie Liu,Lu Lin
The conversion of concentrated 5-hydroxymethylfurfural (HMF) or fructose to 2,5-furandicarboxylic acid (FDCA), a renewable alternative to petroleum-derived terephthalate acid, is highly desirable but challenging for FDCA production in an industrial scale. In this contribution, DMSO/H 2 O mixture was demonstrated as an effective medium for the production of FDCA from high concentration of HMF or fructose. For example, FDCA yield up to 93% was achieved at 10 wt% HMF concentration in DMSO/H 2 O over commercially available Ru/C (2 equiv. NaHCO 3 , 130 °C, 4 MPa O 2 and 12 h). Furthermore, an overall FDCA yield of 65% was achieved from concentrated fructose (19 wt%) through a facile two-step process. Notably, it is so far the highest HMF or fructose concentration employed for FDCA formation. As compared to pure water or DMSO , DMSO/H 2 O mixed system is able to stabilize HMF in an alkaline environment, which allows the efficient oxidation of HMF at high concentrations.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2020
·
IF 6.551
Srinivasan Vinju Vasudevan,Xianghai Kong,Mengjie Cao,Mei Wang,Hanping Mao,Quan Bu
Tungstophosphoric acid (TPA) encapsulated dendritic fibrous silica KCC-1 was prepared via a microemulsion system with the simple reflux method using cetyltrimethylammonium bromide as a structure-directing agent. The TPA impregnated on KCC-1 (ITPA-KCC-1) was also prepared for comparative. Various physicochemical techniques were used to characterize the synthesized materials and their activity evaluated in the 5-hydroxymethylfurfural (HMF) formation from carbohydrates derivatives of fructose, glucose and cellulose . The effect of various factors such as catalyst to substrate ratio, different solvents and temperature were investigated on the formation of HMF. The resultant encapsulated catalyst was very active in fructose dehydration with the yield of 92% HMF and full conversion of fructose at 120 °C for 30 min under the microwave heating condition without any salt additive in the THF solvent system as well as 95% in MIBK solvent. The HMF yield was achieved by 58% and 16.2% from glucose and cellulose in the DMSO solvent, respectively. The TPA-KCC-1 can be separated easily after reaction from the reaction mixture and reused atleast five times without substantial loss in catalytic activity. This study provides an easy encapsulation method for TPA in dendritic fibrous silica KCC-1 as a heterogeneous catalyst , and it should have great application potential in other biomass valorization processes.
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Journal of Materials Chemistry A
·
2017
·Vol. 6
·期 4
·1496-1503
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IF 8.867
Xiangdong Ma,Xiaoxi Zuo,Jinhua Wu,Xiao Deng,Xin Xiao,Jiansheng Liu,Junmin Nan
A new polyethylene (PE)-supported ultra-thin blended polymer electrolyte based on polyvinylidene fluoride/hydroxyethyl cellulose (PVDF/HEC) was prepared by a simple dipping method for 5 V high voltage lithium-ion batteries (LIBs). The performances of the prepared membranes and the resulting GPEs were investigated by scanning electron microscopy, electrochemical impedance spectroscopy, linear potential sweep voltammetry, and charge–discharge cycling. The effects of the ratio of PVDF to HEC on the performance of the composite separator were further discussed. It was found that PE-supported polymer separators (PVDF : HEC = 3 : 1, by weight) present the best mechanical, thermal and wettability performance. The ionic conductivity of this GPE is 0.78 mS cm−1, which is much higher than that of PE separators (0.39 mS cm−1) at room temperature. The electrochemical stability of this GPE can reach up to 5.25 V (vs. Li/Li+). A LiNi0.5Mn1.5O4 cathode with this GPE exhibits a superior cycling stability and rate performance at room temperature. This suggests that the polyethylene (PE)-supported ultra-thin blended polymer electrolyte can be used for 5 V LIBs due to its good performance, low cost and strong operability.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Jingyu Liu,Chaoyue Zhang,Daiyu Song,Yihang Guo,Jiyan Leng
Brønsted acidic ionic liquid (BAIL) functionalized dendritic fibrous nanosilica sphere catalysts, [C 3 PrIm][SO 3 CF 3 ]-DFNS (C 3 = PrSO 3 H), are prepared via a hexadecylpyridinium bromide reverse micelle-directed co-condensation of tetraethoxysilane and 3-chloropropyltriethoxysilane in a water-in-oil emulsion system followed by successive chemical modification with imidazole , 1,3-propanesultone and trifluoromethane sulfonic acid , and the particle diameter, fiber thickness and fiber density of the catalysts are well-adjusted by changing the composition of the starting materials. The [C 3 PrIm][SO 3 CF 3 ]-DFNS catalysts are successfully applied in transformation of 5-hydroxymethylfurfural (HMF) to ethyl levulinate (EL). Combination of superstrong Brønsted acidity and unique open three-dimensional dendritic fibrous nanostructures , the [C 3 PrIm][SO 3 CF 3 ]-DFNS can transform HMF in ethanol media rapidly and completely; nevertheless, the selectivity to EL remarkably depends on the fiber thickness and fiber density, which affect diffusion and mass transfer of the reactants and products as well as the accessibility to the acid sites. Among the tested [C 3 PrIm][SO 3 CF 3 ]-DFNS catalysts, the [C 3 PrIm][SO 3 CF 3 ]-DFNS- 1 with the thinnest fiber sheet and considerably high fiber density exhibits the highest selectivity to EL (93.0%). The [C 3 PrIm][SO 3 CF 3 ]-DFNS catalysts also show good reusability, and they can be reused at least for five times without obvious changes of the reactivity, total selectivity, morphology, textural properties and chemical structure .
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Green Chemical Engineering
·
2023
·
IF 0
Jian Yang,Jia Zhang,Enrico Benassi,Xuemei Li,Hailong Liu,Weiguo Fang,Junying Tian,Chungu Xia,Zhiwei Huang
Al 2 O 3 -supported monometallic Ni, Co, and bimetallic Ni–Co nanocatalysts originated from layered double hydroxide precursors were synthesized by co-precipitation method, and used for the synthesis of useful 5-amino-1-pentanol (5-AP) and 1,5-pentanediol (1,5-PD) by reductive amination (RA) or direct hydrogenation of biofurfural-derived 2-hydroxytetrahydropyran (2-HTHP), respectively. In both reactions, the yield of the target products decreased monotonously with the increasing amounts of Co in the NiCo/Al 2 O 3 catalysts, owing probably to the replacement of highly reactive Ni by Co component with inferior hydrogenation activity at the low reaction temperature of 60 °C. However, the incorporation of Co could improve the reducibility of the NiCo/Al 2 O 3 bimetallic catalysts and promote the reaction stability of the catalysts, especially for Ni 2 Co 1 /Al 2 O 3 , in both reactions with over 180 h time-on-stream. Characterization of the catalysts before and after the reaction showed that the incorporating Co could inhibit the sintering of metal particles and hinder the surface oxidation of the more reactive Ni 0 species, thanks to the formation of Ni–Co alloy in the bimetallic catalysts. DFT-based modeling of the reaction mechanisms is also performed, supporting the reaction pathway proposed previously and also the much higher activity of Ni in the RA of 2-HTHP as compared with Co.
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RSC Advances
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2014
·Vol. 5
·期 5
·3792-3798
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IF 3.708
Chao Qi,Ying-Jie Zhu,Guan-Jun Ding,Jin Wu,Feng Chen
In this paper, we report a simple and green strategy for the synthesis of hydroxyapatite (HAP) nanostructures with various morphologies (including nanoparticles, microtubes, nanorods and nanorod-assembled flower-like hierarchical structures) using adenosine 5′-monophosphate sodium salt (AMP) as an organic phosphorus source by solvothermal treatment in different solvents. The effects of the solvents and the reaction time on the morphology of the product as well as the formation mechanism of HAP nanostructures are investigated. In this strategy, the AMP biomolecules act as an organic phosphorus source for the formation of HAP nanostructures, and the solvents have effects on the morphology of the product. This strategy is environmentally friendly and surfactant-free. The as-prepared products are characterized by X-ray powder diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM) and thermogravimetric analysis (TG).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Xiaofeng Wang,Chengcheng Zhang,Zuyi Zhang,Yaoming Gai,Qingbo Li
The interface site between metal and support possess unique electronic and morphological structure, providing distinct active centers for favorable reaction in catalytic conversion of biomass derivatives to valuable chemicals. In this study, a series of Cu-Co/CeO x catalysts were prepared for hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF) via reduction of the corresponding layered double hydroxide precursors. The characterizations indicated the formation of CoCe-Vö interface (Vö denotes oxygen vacancy) and the effect of hydrogen spillover from Cu species to CoCe-Vö interface. Furthermore, the experiments and theoretical calculations verified that CoCe-Vö interface could activate the C O bond. The optimized catalyst showed a DMF yield of > 90% at 180 °C and 1.5 MPa H 2 with no deactivation in the cycling tests. This study reveals the interfacial effects of the nanocatalysts, including the oxygen vacancies and hydrogen spillover, on hydrogenolysis of HMF, which provided a simple and efficient approach for synthesis of high-performance non-noble metal nanocatalysts applied to the hydrogenolysis of various biomass derivatives.
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TALANTA
·
2021
·
IF 6.057
Qian Wang,Huanshun Yin,Jia Ding,Xi Fang,Yunlei Zhou,Shiyun Ai
The endogenous epigenetic marker 5-formylcytosine (5 fC) is introduced by 5-methylcytosine (5 mC) oxidation under action of enzyme oxidation, and plays an important role in many life activities. Since the content of 5 fC in mammalian tissues and cells is very low, it is necessary to exploit a sensitive and specific detection method to further understand the function of 5 fC. In this work, a sensitively and selectively photoelectrochemical (PEC) biosensor was developed for 5-formyl-2′-deoxycytidine (5fdC) detection. CuBi 2 O 4 /ZnPc@WS 2 was used as photoactive material, where the formed ternary heterojunction structure greatly enhanced the PEC response and increased the detection sensitivity. Positively charged polyethyleneimine (PEI) was employed as 5fdC recognition and capture unit, where the amine group on PEI specifically reacted with aldehyde group of 5fdC to form stable amide bond. 4-Carboxyphenylboronic acid (4-CPBA) was adopted as crosslinker for 5fdC and amino functionalized CuBi 2 O 4 based on the covalent interaction between 1,3-diol bond on 5fdC and boric acid structure on 4-CPBA, and the covalent interaction between –COOH on 4-CPBA and –NH 2 on amino functionalized CuBi 2 O 4 . On the basis of the positive synergistic effect of ZnPc and CuBi 2 O 4 on improving the photoelectric performance of WS 2 , the separation of photo-generated electron-hole pairs in semiconductors were promoted, and the examination range was expanded from 0.1 to 500 nM, and the detection limit was 0.0483 nM (3σ). Based on the unique covalent reaction between –NH 2 and –CHO, the PEC biosensor has excellent detection sensitivity, and can even separate 5fdC from 5-methylcytosine deoxyribonucleoside and 5-hydroxymethylcytosine deoxyribonucleoside. The effect of antibiotics and heavy metals on the 5fdC content in wheat tissue genome has also been further investigated using this sensor.
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JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Hongbing Wang,Yifei Yang,Shixiang Yu,Beibei Zhang,Junzhong Xie,Jun Chen,Dongping Wang,Bomin Feng,Changyin Zhong,Linsen Zhou,Wei Cui,Ding Ma,Yunxi Yao
Liquid-phase hydrogen isotopes exchange between hydrogen and water is a promising route for the hydrogen isotopes separation from water, catalyzed by the metal Pt with hydrophobic coating to surmount the flooding of reactive sites. However, poor water activation ability on Pt has limited the catalytic efficiency of Pt-based catalysts and hindered their application. Herein, we report a bifunctional Pt/ZSM-5 catalyst with hydrophobic modification by surface silylation for H 2 -HDO isotope catalytic exchange. The integration of metallic Pt and Brønsted acid (BA) sites in the microporous ZSM-5 boosts the catalytic efficiency of deuterium extraction by two orders of magnitude compared to commercial Pt-C at the optimum condition. In-situ spectroscopic and theoretical studies demonstrated that HDO-H 2 O preferentially adsorbs on BA sites (-Si-OH-Al) to form protonated water clusters stabilized by hydrogen-bonded network or to undergo the proton exchange to leave deuterium on zeolite framework as a new acidic site ([AlO 4 D]). Under the attractive interaction, the dissociated hydrogen on Pt clusters releases partial electrons to form positively-charged hydrogen, which further transfers to the [AlO 4 D] sites or protonated water clusters by interfacial spillover to produce the overcharging intermediates. These intermediates cleave their O-D bonds to form positively charged D, which ultimately spills back to Pt cluster and combines with the remaining electron to desorb in the form of HD. The synergistic effect between Pt and BA sites creates a new pathway of hydrogen transfer, which enables the more efficient hydrogen-water isotope exchange on the bifunctional Pt/ZSM-5 catalyst.
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FUEL
·
2022
·
IF 8.035
Puxiang Yan,Haiyong Wang,Yuhe Liao,Pengyao Sun,Chenguang Wang
Catalytic valorization of biomass into chemicals and fuels plays a key role in order to achieve net-zero greenhouse gas emissions. Herein, a series of hierarchical ZSM-5 zeolites were synthesized by the post-treatment method to transform furfural alcohol (FAL) to levulinic acid (LA). ZSM-5 obtained from tandem alkaline treatment (0.2 M NaOH) and acid washing (0.1 M HCl), denoted as ZSM-5-OH 0.2 -H, exhibited the highest activity, affording 76.2% LA yield in 9:1 acetone–water mixed solvents at 393 K for 0.5 h. The enhanced adsorption capacity and acid accessibility of FAL on zeolite mediated by the introduction of mesopores, as well as the reduced secondary reactions of the generated LA due to few Al atoms in straight and sinusoidal channels (as confirmed by UV–vis diffuse reflectance), were responsible for the outstanding catalytic performance of ZSM-5-OH 0.2 -H. The structure–activity relationship revealed that regulating the porous structure and Al distribution of ZSM-5 was an effective strategy to enhance its hydrolytic performance of FAL to LA. Moreover, ZSM-5-OH 0.2 -H could be reused for three reaction cycles without significant loss in catalytic activity.
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FLUID PHASE EQUILIBRIA
·
2019
·
IF 2.514
Yameng Wan,Haixia He,Pengshuai Zhang,Rui Zhao,Jiao Sha,Tao Li,Baozeng Ren
Mole-fraction solubility of 5-norbornene-2,3-dicarboximide (NODI) in eleven solvents including methanol (MtOH), ethanol (EtOH), 2-ethoxyethanol, methyl acetate (MAC), ethyl acetate (EAC), n-propyl acetate (NPAC), isopropyl acetate (IPAC), n-butyl acetate (NBAC), acetone (DMK), N,N-dimethylformamide (DMF) at (278.15–323.15) K and 1,4-dioxane at (288.15–323.15) K was experimentally measured by laser monitoring technique under 0.1 MPa. Solubility of NODI increased with the increasing temperature. Hansen Solubility Parameter was employed to explain the solubility behavior. The Kamlet-Taft parameters were calculated to investigate the solvent effect based on linear solvation energy relationships concept. Thermodynamic modeling including the Two-Suffix Margules model, Wilson model, NRTL model, NRTL-SAC model and UNIQUAC model were employed to correlate the experimental solubility. Wilson model and NRTL-SAC model were more suitable in correlation with solubility data. Furthermore, thermodynamic properties of mixing process (Δ mix G , Δ mix H , Δ mix S , ln γ 1 ∞ , H 1 E,∞ , ζ TS and ζ H ) were discussed based on Wilson equation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Deyu Si,Meihua Zhu,Xinmei Sun,Miao Xue,Yuqin Li,Ting Wu,Tian Gui,Izumi Kumakiri,Xiangshu Chen,Hidetoshi Kita
The formation progress of the high aluminum ZSM-5 zeolite membrane was investigated and characterized with the organic template-free and fluoride-containing initial synthesis gel. The nano spherical Silicalite-1 seed crystals were dissolved into amorphous by the fluoride-containing precursor synthesis gel. The amorphous contained elementary structural units (TO 4 ) and isolated five-membered ring structure of MFI zeolites. These were retained to provide the nucleation sites for high aluminum ZSM-5 zeolite. The ZSM-5 zeolite nucleus was grown into fine needle-like ZSM-5 zeolites, which were gradually grown into twin crystals, aggregation and compact ZSM-5 zeolites layer on the support without the organic template initial synthesis gel. In addition, the high aluminum ZSM-5 zeolite membranes kept the identical morphology and structure for separation of high concentration acetic acid (H 2 O/HAc) or inorganic acid (1 M H 2 SO 4 ) aqueous mixtures by XRD, SEM and NMR characterization. Furthermore, the membrane had a good dehydration performance and acid-stability by pervaporation. The flux and separation factor of the membrane for 10 wt% H 2 O/HAc mixtures were 0.98 kg∙m −2 ∙h −1 and 3200 at 348 K, respectively.
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