CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Lu Li,Shenghui Li,Sheng Wang,Xiaoli Xing,Yating Zhang,Lin Su,Xiaoli Wu,Hanjie Wang,Jin Chang,Xiaoqun Gong
Diabetic cataract (DC) is a kind of worrying ocular complications that eventually leads to blindness. However, there are a narrow range of pharmacological interventions to enable control the progression of DC, especially the eye drops based on noninvasive routes. In this work, we developed a kind of strong antioxidant Pt nanoclusters coated with cell-penetrating peptide (TAT) conjugated dextran (DTPNCs). The DTPNCs were dispersed in 0.1% Pluronic F127 (W/V) to form eye drops, which have the ability of corneal permeation. The results indicate that the presence of 0.1% Pluronic F127 (W/V) resists the clearance of tear film against DTPNCs and TAT-conjugated dextran contribute to the interaction and permeation with corneal barriers with the help of electrostatic interaction in vivo. More importantly, the DTPNCs possess effective antioxidant capacities and can protect the lens epithelial cells against oxidative stress by eliminating ROS and impose restrictions on the α-crystallin glycation and crosslinking in vitro, further to slow down the process of DC. We hope that our approach will provide a promising non-invasive and painless treatment to DC.
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高影响因子
ChemSusChem
·
2020
·Vol. 13
·期 12
·3127-3136
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IF 7.962
Peter Kisszekelyi,Rifan Hardian,Hakkim Vovusha,Binglin Chen,Xianhai Zeng,Udo Schwingenschlögl,Jozsef Kupai,Gyorgy Szekely
Graphical Up the tempo : An efficient TEMPO-based electrocatalytic transformation of biomass-based C 6 -platform chemical 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) is reported. The molecular design and comparison of homogeneous (native, size-enlarged) and solid-supported (SiliaCAT, TurboBeads) TEMPOs is discussed for the oxidation in the ElectraSyn reactor with cost-effective electrodes and green solvents. Computational modeling reveals the synergistic effect of the catalyst/base system and facilitated the catalyst design. The catalytic transformation of bio-derived compounds, specifically 5-hydroxymethylfurfural (HMF), into value-added chemicals may provide sustainable alternatives to crude oil and natural gas-based products. HMF can be obtained from fructose and successfully converted to 2,5-diformylfuran (DFF) by an environmentally friendly organic electrosynthesis performed in an ElectraSyn reactor, using cost-effective and sustainable graphite (anode) and stainless-steel (cathode) electrodes in an undivided cell, eliminating the need for conventional precious metal electrodes. In this work, the electrocatalysis of HMF is performed by using green solvents such as acetonitrile, γ-valerolactone, as well as PolarClean, which is used in electrocatalysis for the first time. The reaction parameters and the synergistic effects of the TEMPO catalyst and 2,6-lutidine base are explored both experimentally and through computation modeling. The molecular design and synthesis of a size-enlarged C 3 -symmetric tris-TEMPO catalyst are also performed to facilitate a sustainable reaction work-up through nanofiltration. The obtained performance is then compared with those obtained by heterogeneous TEMPO alternatives recovered by using an external magnetic field and microfiltration. Results show that this new method of electrocatalytic oxidation of HMF to DFF can be achieved with excellent selectivity, good yield, and excellent catalyst recovery.
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PubMed
高影响因子
CELLULOSE
·
2020
·Vol. 27
·期 6
·3037-3054
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IF 4.21
Zhang Yunlei,Li Bing,Guan Wen,Wei Yanan,Yan Changhao,Meng Minjia,Pan Jianming,Yan Yongsheng
Nitrogen-doped carbon materials have attracted enormous interest in catalysis owing to their outstanding catalytic performance. In this work, nitrogen-doped carbonaceous catalysts (NCC) supported on inexpensive and naturally abundant halloysite nanotubes were successfully synthesized via precipitation polymerization, calcination, and sulfonation processes. The physical and chemical properties of the obtained catalysts were systematically characterized by different methods. The results indicated that NCC catalysts had mesoporous structures, excellent thermostability and acid-base bi-functional active sites. One-pot synthesis of 5-hydroxymethylfurfural (HMF) from glucose was performed to investigate the synthesized NCC catalysts. Benefiting from the synergistic effects of the acid-base bi-functional active sites, the highest HMF yield (62.8%) was achieved in an isopropanol-mediated DMSO system under optimal conditions. Moderate to excellent yields of HMF were also obtained from one-pot conversions of other carbohydrates, including inulin, sucrose, cellobiose, maltose and starch, with our developed catalytic system. The one-pot production of HMF from cellulose was also smoothly processed by the NCC bi-functional catalyst in an IL-based system. This work has developed a versatile strategy for designing nitrogen-doped carbonaceous catalysts that can be employed for the direct transformation of renewable carbohydrates to platform chemicals.
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高影响因子
CHINESE JOURNAL OF CHEMISTRY
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2020
·Vol. 38
·期 5
·453-457
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IF 3.826
Chuang Li,Guangyue Xu,Xiang Zhang,Yao Fu
Summary of main observation and conclusion The conversion of fructose to 1,2-propylene glycol (PG) is an important process from cellulosic biomass to high-value added chemicals. Herein, Ru-WO x /hydroxyapatite (HAP) catalyst was employed for this reaction and reached up to 91.3% yield of PG at 180 °C, 1 MPa initial hydrogen for 8 h in water. On this catalyst, Ru and WO x were highly dispersed on HAP support and they interacted with each other to form a special catalytic center. The lack of isolated Ru or RuW alloy site led to a moderate activity for hydrogenolysis and hindered the further conversion of PG to propanol. The weak basic HAP support efficiently prevented the humin formation. This precisely controlled catalyst has potential in green PG production.
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高影响因子
Food Analytical Methods
·
2020
·Vol. 13
·期 4
·839-849
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IF 2.667
Zhou Ying,Cheng Fuliang,Hong Yanping,Huang Jianping,Zhang Xue,Liao Xiaoning
Isoproturon (ISO), an herbicide belonging to the phenyl urea family, is extensively used in modern agriculture to guarantee a bumper harvest. However, it has been evidenced that the ISO has heavy toxicity to the liver system and appears to be a tumor promoter. It is therefore urgent to develop sensitive and selective methods to screen its presence in food resources to meet the ever-increasing pollution restrictions. In this work, an electrochemical sensor based on graphene oxide–modified multi-walled carbon nanotubes hybrid material was firstly developed for the rapid and sensitive detection of ISO via square wave voltammetry (SWV). Under optimized experimental conditions, the sensor exhibits a relatively wide linear range from 0.30 to 15.0 μmol L −1 , a low limit of detection (LOD) of 0.10 μmol L −1 , as well as good repeatability, high reproducibility, excellent selectivity, and long-term stability. The sensor has also been successfully employed in various real samples such as rice field water, tomato, and lettuce analyses. The obtained recoveries are in the range of 97.33–105.0% with low relative standard deviation (less than 2.5%), which is very close to the results of the high-performance liquid chromatography (HPLC), showing the proposed electrochemical sensor has great potential in practical applications.
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高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 23
·期 21
·8458-8467
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IF 10.182
Shanshan Xiong,Chao Luo,Zhihao Yu,Na Ji,Lingjun Zhu,Shurong Wang
The isomerization–dehydration cascade conversion on the saccharide platform is a pivotal route for biomass valorization, although it exhibits a specific reaction complexity that makes achieving an efficient conversion a highly technical challenge. The rational design of novel versatile solid acids is deemed to be the key to improving the cascade catalytic performance. In this paper, a dual-functional carbon-based solid acid catalyst (DFCSA) with tunable Brønsted/Lewis acid sites was developed for the cascade conversion of saccharides. The combined modification of H3PO4 and HNO3 on the carbon substrate contributed to the grafting of protonated moieties with a reasonably porous structure. With the aid of AlPO4, which has an orthorhombic crystal structure, the newly developed catalyst was able to achieve good performance for the subsequent hydrothermal conversion. Under optimal conditions, glucose and xylose were transformed with high product yields: 38.2 mol% levulinic acid and 69.7 mol% furfural, respectively. In addition, the catalyst displayed excellent hydrothermal stability, with only a slight degradation in activity after 10 cycles, which was ascribed mainly to the high thermal stability of AlPO4 and the firm grafting of the surface functional groups. As shown by the kinetic analysis, the DFSCA catalyst had a higher conversion rate and lower activation energy in the cascade conversion of xylose than that of glucose, leading to a better yield of furfural.
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2021
·
IF 3.171
Yanan Wei,Yunlei Zhang,Bing Li,Wen Guan,Changhao Yan,Xin Li,Yongsheng Yan
5-Hydroxymethylfurfural (5-HMF), as a key platform compound for the conversion of biomass to various biomass-derived chemicals and biofuels, has been attracted extensive attention. In this research, using Pickering high internal phase emulsions (Pickering HIPEs) as template and functional metal-organic frameworks (MOFs, UiO-66-SO 3 H and UiO-66-NH 2 )/Tween 85 as co-stabilizers to synthesis the dual acid-base bifunctional macroporous polymer catalyst by one-pot process, which has excellent catalytic activity in the cascade reaction of converting cellulose to 5-HMF. The effects of the emulsion parameters including the amount of surfactant (ranging from 0.5% to 2.0% (mass)), the internal phase volume fraction (ranging from 75% to 90%) and the acid/base Pickering particles mass ratio (ranging from 0:6 to 6:0) on the morphology and catalytic performance of solid catalyst were systematically researched. The results of catalytic experiments suggested that the connected large pore size of catalyst can effectively improve the cellulose conversion, and the synergistic effect of acid and base active sites can effectively improve the 5-HMF yield. The highest 5-HMF yield, about 40.5%, can be obtained by using polymer/MOFs composite as catalyst (Poly-P12, the pore size of (53.3 ± 11.3) μm, the acid density of 1.99 mmol·g −1 and the base density of 1.13 mol·g −1 ) under the optimal reaction conditions (130 °C, 3 h). Herein, the polymer/MOFs composite with open-cell structure was prepared by the Pickering HIPEs templating method, which provided a favorable experimental basis and theoretical reference for achieving efficient production of high added-value product from abundant biomass.
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高影响因子
Journal of Cleaner Production
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2021
·
IF 9.297
Fengjiao Lai,Feng Yan,Pengju Wang,Chunyan Li,Xuehua Shen,Zuotai Zhang
The development of heterogeneously functional catalysts is of great significance in selective catalysis for biomass valorization. Herein, we report for the first time the applicability of chitin/Ag co-modified H 3 PW 12 O 40 composites (Chx-AgPW) as catalysts for producing valuable furans from carbohydrates and biomass. The as-prepared Ch15-AgPW catalyst exhibited the best catalytic performance, due to the dual Brǿnsted-Lewis acidity and appropriate chitin content. When the amount of Ch15-AgPW catalyst was 0.25 mmol, an excellent 5-hydroxymethylfurfural (HMF) yield of 78.3% could be achieved at 150 °C for 3 h with nearly 100% glucose conversion in the H 2 O/MIBK (V H2O:MIBK = 4:6) solvent system. Furthermore, high-yield HMF could also be obtained from other carbohydrates such as fructose (85.3%), sucrose (72.3%), cellobiose (65.6%), starch (52.7%) and inulin (43.5%). Additionally, corn stover , rice straw and sugarcane bagasse under typical reaction conditions simultaneously produced furfural and HMF in yields of 64.6%–72.2% and 18.5%–25.6%, respectively. Combined with the characterization, mechanism study demonstrated that the surface functional groups in chitin were conductive to rapid absorption of the substrates; the Brǿnsted acid sites from heteropoly anion (H 2 [PW 12 O 40 ] - ) promoted the initial depolymerization of biomass and the final dehydration to furans; the introduction of Ag + favored the isomerization of intermediates. After reaction finished, the Ch15-AgPW catalyst could be easily recovered by filtration and effectively reused at least eight cycles without substantial loss in catalytic activity . This work provides a novel strategy to synthesize stable heterogeneous catalysts with tunable acidity for producing bio-based fuels and chemicals from renewable resources .
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高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Jianjun Xiao,Qinfang Chen,Rui Yu,Jiayi Qian,Zihao Liu,Teng Li,Haiping Yang,Jing'ai Shao,Weiran Yang,Hanping Chen
Developing cost-effective and high-performance catalysts in biomass chemistry is motivated by creating sustainable technologies dependent on inexpensive and abundant resources. The existing methods for the direct preparation of 5-methylfurfural (5-MF) from biomass-derived fructose mediated by hydrogen iodide (HI) mainly require precious metal catalysts. This research showed that low-cost tungsten carbide (WC) was capable to produce HI from iodine (I 2 ) via liquid-phase hydrogenation, but a pivotal limitation was the poor stability under the combination effects of water and I 2 . To solve this problem, the bulk WC and the high dispersion supported WC were modified by hydrophobic organosilicones through simple liquid phase deposition. Both of the two superhydrophobic WC materials had better stability and their catalytic activity were comparable to the expensive palladium-carbon (Pd/C) catalyst in the preparation of 5-MF, especially the superhydrophobic high dispersion supported WC. This work highlights the potential of the low-cost WC with simple superhydrophobic modification in assisting the direct preparation of 5-MF from fructose mediated by HI, which has high significance to the sustainable development of the low-cost biomass chemical engineering.
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高影响因子
DYES AND PIGMENTS
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2021
·
IF 4.889
Shijun Lin,Shuwen Liu,Guofei Dai,Xiaojin Zhang,Fan Xia,Yu Dai
Gold nanoparticles (AuNPs), as one of the major tools of fluorescence-quenching sensors, have been widely used in biochemical analysis through fluorescence resonance energy transfer (FRET) effect. With the development of chemistry and biochemistry, reaction-based fluorescent sensors have attracted increasing attention because of their unique selectivity, high sensitivity and rapid detection. Here we report a click-induced fluorescence-quenching sensor based on AuNPs for detection of copper ion (Cu 2+ ) and ascorbic acid (AA). A fluorescent dye Rhodamine B-(CH 2 CH 2 O) 4 -azide (RB-PEG 4 -N 3 ) is conjugated to the surface of AuNPs via Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) in the presence of Cu 2+ and AA, leading to the fluorescence quenching of Rhodamine B. The sensor responds quickly (within less than 3 min). The fluorescent intensity linearly correlates with the concentration of Cu 2+ in the range of 0–108 μM. The limit of detection (LOD) for Cu 2+ is 5.8 μM. The concentration range for detection of AA is 0–3 mM. The LOD for AA is 0.13 mM. In addition, the application of the sensor is verified by performing detection in real samples such as fresh orange, juice, VC tablet, and lake water. This work expands the application of AuNPs-based fluorescence-quenching sensors for multi-component detection.
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高影响因子
FUEL
·
2021
·
IF 6.609
Xin Yu,Lincai Peng,Jun Dai,Hui Li,Chaonan Tao,Fa Yang,Junhua Zhang
Conversion of carbohydrates at concentrated feeds represents highly desirable for the industrial deployment of biobased fuels and chemicals but challenging. One key bottleneck is that the excessive formation of polymeric humins greatly diminishes the utilization rate of feedstocks and the destination product yield. We report that the use of ethylene glycol as co-solvent for acid-catalyzed conversion of concentrated sugars enhances desirable alkyl levulinate (AL) production compared to reactions carried out in single monohydric alcohols (e.g., methanol, ethanol). Ethylene glycol served not only as a solubilizer of sugars in the reaction medium to lessen their tendency to polymerize by protecting reactive hydroxyl groups in sugars with alcohols, but also as a supporter to restrain the condensation of furan intermediates. With 10 vol% ethylene glycol as the co-solvent of ethanol, an improved yield of ethyl levulinate (EL) from 45% to 56% was accomplished from concentrated feeds of glucose (200 g/L). In particular, high space time yield and EL concentration respectively up to 30 kg/m 3 ·h and 90 g/L were obtained in a batch reactor. The solvents and catalyst could be isolated from the products, and showed good reusability. This contribution opens a reliable avenue for converting highly concentrated feeds of biomass-related sugars to oxygenated liquid fuels and versatile chemicals.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaoqi Lyu,Hong Li,Huaizhong Xiang,Yibing Mu,Na Ji,Xuebin Lu,Xiaolei Fan,Xin Gao
Microwave (MW)-assisted process intensification of catalytic conversion of saccharides is a promising route for energy efficient production of value-added chemicals and fuels. This work presents the development of the MW-responsive catalysts (i.e., the acid functionalized spherical carbon superstructure, SCS) for converting fructose to 5-HMF effectively and efficiently under MW irradiation. Under a mild MW condition (at 70 °C, atmospheric pressure), the SCS catalyst (with surface sulfonic and carboxylic acid groups) achieved fructose conversion of ~ 97.8% and selectivity to 5-HMF of ~ 90.6% after 5 min reaction time with good recyclability, being significantly higher than that obtained by the system under the conventional heating. Importantly, the MW-assisted system showed very high energy efficiency coefficient of 1.01 mmol kJ −1 L −1 compared to that (0.09 mmol kJ −1 L −1 ) of the conventional thermal catalysis. The mechanism of process intensification of the system developed may be attributed to the combination of the dipole polarization of the MW-responsive sulfonic groups and the selective heating of the MW-absorbing SCS support under the MW condition.
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高影响因子
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