Nanoscale
·
2024
·
IF 5.8
Yufeng Wu,Zhiyan Hou,Changlong Wang
Renewable electricity-powered electrooxidation of 5-hydroxymethylfurfural (HMFOR) to FDCA offers a green and sustainable approach to producing an essential monomer for bio-polymers, provided that a highly efficient electrocatalyst is present. Herein, we show that the doping of scandium (Sc) into an NiFe-LDH electrocatalyst (Sc-NiFe-LDH) considerably promotes HMFOR by enhancing the formation of high-valence NiIII–O active sites, facilitating electron transport and HMF adsorption and suppressing the oxygen evolution reaction. In the presence of the Sc-NiFe-LDH electrocatalyst, an FDCA faradaic efficiency and selectivity of 96.5% and 99.5%, respectively, were achieved at a current density of >600 mA cm−2. The high performance of the Sc-NiFe-LDH electrocatalyst is the best among those of other reported electrocatalysts for this reaction, showing great promise in upgrading biomass to valuable chemicals. This work would inspire further studies on the rational design of novel and efficient electrocatalysts for green and sustainable energy transformations.
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高影响因子
RSC Advances
·
2016
·Vol. 6
·期 53
·47890-47896
·
IF 3.289
Miaomiao Han,Xiao Liu,Guangcheng Huang,Yadong Liu,Shengxiang Ji
5-Hydroxymethylfurfural (HMF) is considered as a valuable platform chemical for fuels and chemical intermediates. Tremendous efforts have been made on the development of catalysts for the dehydration of saccharides to HMF with high conversion and selectivity. Here we reported a new solid acid, phosphoric acid doped polybenzimidazole (PA–PBI), for the dehydration of fructose to HMF with high selectivity (∼94%) at high fructose concentration (50 wt%) in a water–methyl isobutyl ketone (MIBK) biphasic system. PA–PBI was directly obtained by the one-pot polycondensation reaction and was very stable under harsh reaction conditions due to the strong acid–base interaction between PA and imidazole in PBI. PA–PBI was recycled to catalyze the dehydration of fructose four times without the loss of activity and could also catalyze a variety of disaccharides and polysaccharides to produce HMF. The high selectivity and the ease of recycling make PA–PBI a superior catalyst for the dehydration of saccharides to HMF.
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Journal of Energy Chemistry
·
2016
·
IF 2.322
Jiawei Zhong,Yuanyuan Guo,Jinzhu Chen
A serial of protonated and layered transition metal oxides , including layered HTaWO 6 , HNbMoO 6 as well as HNbWO 6 , were synthesized by solid-state reaction and ion-exchange. The layered HTaWO 6 has been systematically studied as a solid acid to realize the dehydration of fructose to 5-hydroxymethylfurfural (HMF). The transition metal oxide samples were characterized with ICP-OES, EDS, XRD , XPS , SEM, TGA, FT-IR, N 2 adsorption–desorption and NH 3 -TPD. The influential factors such as reaction temperature, reaction time, solvent, catalyst amount and substrate concentration were deeply investigated. The optimized fructose conversion rate of 99% with HMF yield of 67% were achieved after 30 min at 140 °C in dimethylsulfoxide.
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JOURNAL OF CHROMATOGRAPHY A
·
2017
·
IF 3.981
Qian Wang,Xiao-Mei He,Xi Chen,Gang-Tian Zhu,Ren-Qi Wang,Yu-Qi Feng
Phosphorylation is a crucial post-translational modification, which plays pivotal roles in various biological processes. Analysis of phosphopeptides by mass spectrometry (MS) is intractable on account of their low stoichiometry and the ion suppression from non-phosphopeptides. Thus, enrichment of phosphopeptides before MS analysis is indispensable. In this work, we employed pyridoxal 5′-phosphate (PLP), as an immobilized metal affinity chromatography (IMAC) ligand for the enrichment of phosphopeptides. PLP was grafted onto several substrates such as silica (SiO 2 ), oxidized carbon nanotube (OCNT) and silica coated magnetic nanoparticles (Fe 3 O 4 @SiO 2 ). Then the metal ions Fe 3+ , Ga 3+ and Ti 4+ were incorporated for the selective enrichment of phosphopeptides. It is indicated that Fe 3 O 4 @SiO 2 -PLP-Ti 4+ has a superior selectivity towards phosphopeptides under as much as 1000-fold interferences of non-phosphopeptides. Further, Fe 3 O 4 @SiO 2 -PLP-Ti 4+ exhibited high efficiency in selective enrichments of phosphopeptides from complex biological samples, including human serum and tryptic digested non-fat milk. Finally, Fe 3 O 4 @SiO 2 -PLP-Ti 4+ was successfully employed in the sample pretreatment for profiling phosphopeptides in a tryptic digest of rat brain proteins. Our experimental results evidenced a great potential of this new chelator-based material in phosphoproteomics study.
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高影响因子
Asian Journal of Pharmaceutical Sciences
·
2017
·
IF 0
Li Sun,Yunna Chen,Yali Zhou,Dongdong Guo,Yufan Fan,Fangyan Guo,Yufeng Zheng,Weidong Chen
The sustained-release properties of the biodegradable nano-drug delivery systems were used to improve the residence time of the chemotherapeutic agent in the body. These drug delivery systems were widely used to deliver chemotherapeutic drugs. The 5-fluorouracil loaded chitosan nanoparticles prepared in this paper have the above advantage. Here, we found that when the mass ratio of 5-fluorouracil and chitosan was 1:1, the maximum drug loading of nanoparticles was 20.13 ± 0.007%, the encapsulation efficiency was 44.28 ± 1.69%, the particle size was 283.9 ± 5.25 nm and the zeta potential was 45.3 ± 3.23 mV. The prepared nanoparticles had both burst-release and sustained-release phases in vitro release studies. In addition, the inhibitory effect of the prepared nanoparticles on gastric cancer SGC-7901 cells was similar to that of 5-fluorouracil injection, and the blank vector had no obvious inhibitory effect on SGC-7901 cells. In the pharmacokinetic study of rats in vivo , we found that AUC (0−t) , MRT (0−t) and t 1/2z of nanoparticles were significantly increased in vivo compared with 5-fluorouracil solution, indicating that the prepared nanoparticles can play a role in sustained-release.
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CHINESE JOURNAL OF CHEMISTRY
·
2017
·Vol. 35
·期 11
·1739-1748
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IF 1.852
Wenwen Yuan,Yi Huang,Chunyan Wu,Xiang Liu,Yongmei Xia,Haijun Wang
The development of novel methods to obtain biofuels and chemicals from biomass has been an immediate issue in both academic and industrial communities. In this work, a series of novel catalysts were prepared and characterized by FT-IR, TGA, XRD, SEM, TEM, ICP-AES, NH 3 -TPD and BET, which were applied for the conversion of hexose to 5-hydroxymethylfurfural (HMF). The Cr(Salten)-MCM-41-[(CH 2 ) 3 SO 3 HVIm]HSO 4 catalyst was the most active catalyst, and a glucose conversion of 99.8% with 50.2% HMF yield was obtained at 140 °C for 4 h in dimethyl sulfoxide (DMSO). The effects of reaction temperature, reaction time, solvents and catalyst dosages were investigated in detail. MCM-41 immobilized acidic functional ionic liquid and chromium(III) Schiff base complexes as heterogeneous catalysts can be easily recovered by simple filter treatment, exhibiting excellent stability and activity towards hexose conversion. Thus the heterogeneous catalysts were environment-friendly for transforming biomass carbohydrates into fine chemicals.
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高影响因子
AUSTRALIAN JOURNAL OF CHEMISTRY
·
2016
·Vol. 70
·期 6
·691-698
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IF 1.427
Yu Shen,Fumin Wang,Chaoqun Yang,Xubin Zhang
Hierarchical HZSM-5 were synthesised by controlled desilication in alkaline medium and characterised by field-emission scanning electron microscopy, X-ray diffraction, transmission electron microscopy, inductively coupled plasma–atomic emission spectrometry, N2 adsorption–desorption, and Fourier transform infrared spectroscopy. The catalytic performance of HZSM-5 towards the selective oxidation of 2,3,6-trimethylphenol by H2O2 was evaluated. Recyclability tests were also carried out. The results showed that 2,3,5-trimethyl-1,4-benzoquinone was produced in high yields (i.e. 90 %), corresponding to a 2,3,6-trimethylphenol percentage of 98 %. The N2 adsorption–desorption and XRD studies suggested that mesopores with an average size of 5 nm were produced and that the structural character of HZSM-5 was preserved after desilication. Transmission electron microscopy analysis of the spent catalyst indicated good stability of the hierarchical structure. The Fourier transform infrared spectroscopy studies revealed the development of acid sites. The combined results suggested that the nature of the solvent, intrinsic acidity, and shape selectivity of the hierarchical structure of the catalyst ensured high catalytic properties.
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高影响因子
RSC Advances
·
2016
·Vol. 6
·期 107
·105723-105728
·
IF 3.289
Cheng Chen,Yan Li,Lijian Liu
Oligomers as fluorescent macromolecules are of significant importance and are fairly attractive for high quantum yield two-way conversion luminescence. We report a high conversion rate (ΦF = 0.5184) for a fluorescent oligomer, 1,4-butanediol-bis(5-carbonyl-3-carbethoxy-2-pyrazoline). It was prepared by the novel cyclopolycondensation of 1,4-butanediol-bis(5-carbonyl-3-carbethoxy-2-pyrazoline), a chromophore with good fluorescence (ΦF = 0.0573). After polymerization, a green fluorescent protein (GFP)-mimetic structure was formed, in which a methylene chain (–CH2–CH2–CH2–CH2–) as a flexible group is beneficial due to its folding, and an azo group sits in the rigid pyrazoline ring because of a resonance effect. These factors collectively contribute to the excellent efficiency of the fluorescence performance of the oligomer. Additionally, the oligomer exhibited a weak red shift and a significant fluorescence enhancement compared with the monomer, and we achieved good quality live-cell imaging. The oligomer also allowed for the enhancement of fluorescence intensity through the two-wavelength excitation of a cell rather than increasing the dosage of the dye or the power of the laser.
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ELECTROCHIMICA ACTA
·
2016
·
IF 4.803
Yonghao Zhang,Tingting Yu,Weiqing Han,Xiuyun Sun,Jiansheng Li,Jinyou Shen,Lianjun Wang
A novel tubular porous electrode electrocatalytic reactor was employed to undertake electrochemical treatment of actual anticancer drugs wastewater containing 5-Fluoro-2-Methoxypyrimidine. Effects of operating parameters on the performance of the reactor were studied with the discussion of energy consumption. The results indicated that the optimal condition was flow rate of 0.31 L min −1 , pH value of 5.0, current density of 5 mA cm −2 and without supporting electrolyte. In addition, the degradation intermediates and final products of 5-Fluoro-2-Methoxypyrimidine were analyzed by GC-MS and IC system. A pathway for the electrochemical degradation was proposed as well by quantum chemical calculation using DFT method. After treatment in the reactor, COD and 5-Fluoro-2-Methoxypyrimidine of the wastewater were removed by 84.1% and 100%. Particularly, the BOD 5 /COD value and EC 50,48h value of wastewater were increased from 0.14 and 16.4% to 0.53 and 51.2% respectively, indicating a great biodegradability enhancement. Besides, the electric energy consumption and operating cost of the reactor were only 1.5 kWh kg −1 COD and $ 0.78 per ton, lower than the other conventional electrochemical reactors. The excellent performance as well as the low energy consumption of the electrocatalytic reactor confirmed that electrochemical oxidation is highly applicable for the treatment of anticancer drugs wastewater.
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RSC Advances
·
2017
·Vol. 7
·期 34
·21145-21152
·
IF 3.108
Bingfeng Chen,Fengbo Li,Guoqing Yuan
Selective hydrodeoxygenation of 5-hydroxy-2(5H)-furanone (HFO) derived from furfural oxidation to γ-butyrolactone (GBL) provides a sustainable alternative to the petroleum-based process for γ-butyrolactone production. Furfural is first converted to HFO through selective photocatalytic oxidation by using air oxygen as the oxidant (yield: 85.0%). HFO is further converted to GBL through hydrodeoxygenation over noble-metal nanoparticles on mesoporous Nb–Zr mixed oxides. The conversion of HFO to GBL involves two reactions: hydrogenation catalyzed by active metal and dehydration over mesoporous solid acids. The catalytic properties of M/Nb–Zr mixed oxides (M = Pt, Ir, Ru, Rh and Pd) are related to the composition of support and active metal. The incorporation of zirconia into matrixes improves the thermal stability of mesoporous mixed oxides and increases the amounts of surface acid, which contributes to its catalytic selectivity to GBL. Pt/Nb5Zr5-550 exhibited the best catalytic performances with 97.3% selectivity of GBL at full conversion. The excellent performance can be correlated with the cooperative effect between active metal species and acid sites. The Pt-solid acid bifunctional catalysts show superior catalytic performance compared with conventional catalysts, such as Pt/H-ZSM-5, Pt/C, Rh/C or Pd/C. An overall GBL yield of 82.7% from furfural was obtained.
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KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2017
·Vol. 35
·期 1
·99-109
·
IF 2.007
Hu Lei,Yang Mei,Xu Ning,Xu Jiaxing,Zhou Shouyong,Chu Xiaozhong,Zhao Yijiang
An economical and effective approach for the selective transformation of biomass-derived 5-hydroxymethylfurfural (HMF) into 2,5-dihydroxymethylfuran (DHMF) was developed by catalytic transfer hydrogenation over various magnetic zirconium hydroxides (MZHs). As expected, MZH with a moderate Zr/Fe molar ratio of 2 displayed the highest catalytic activity, resulting in 98.4% HMF conversion and 89.6% DHMF yield at 150 °C for 5 h in the presence of 2-butanol that simultaneously acted as the hydrogen donor and reaction solvent, which was ascribed to its appropriate specific surface area, pore size and acid-base content. Moreover, a plausible reaction mechanism for the catalytic transfer hydrogenation of HMF into DHMF over MHZ(Zr/Fe=2) was also proposed, in which the basic hydroxyl groups with the aid of acidic zirconium metal centers were considered to be responsible for the pivotal hydride transfer via a six-membered ring structure.
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RSC Advances
·
2015
·Vol. 5
·期 69
·56286-56292
·
IF 3.84
Bo Zhang,Zhaoping Zhong,Qinglong Xie,Paul Chen,Roger Ruan
In order to reduce coke yield during catalytic fast pyrolysis of biomass, MgO and 2,4-dimethylquinoline (2,4-DMQ) were selected to reduce the number of external acid sites of HZSM-5. Both MgO and 2,4-DMQ deposition could cause a reduction in total acid sites (both weak acid sites and strong acid sites) and external acid sites of HZSM-5. The modified catalysts were used for the catalytic conversion of bio-derived furan. For the MgO/HZSM-5 catalyst, the effects of amount of MgO deposited and deposition time were studied. The carbon yields of aromatics, C2–C5 olefins, total chemicals, CO2 and CO increased at first and then decreased slightly when the deposited amount increased, while the carbon yield of coke decreased first and then increased gradually. Furthermore, as the deposited time increased, the carbon yields of petrochemicals, CO2 and CO increased greatly, whereas that of coke decreased. For the 2,4-DMQ/HZSM-5 catalyst, the effects of 2,4-DMQ treatment amount and treatment time were investigated. The experimental results showed that an increase in 2,4-DMQ treatment amount or treatment time could retard the generation of the target products, CO2 and CO but promote coke formation.
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