CELLULOSE
·
2020
·Vol. 27
·期 6
·3037-3054
·
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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JOURNAL OF THE BRAZILIAN CHEMICAL SOCIETY
·
2021
·Vol. 32
·期 8
·1598-1606
·
IF 1.838
Zhang Yangyang,Shao Chuan,Qin Dongling,Yang Gang
Solid acid-catalyzed dehydration of fructose to produce 5-hydroxymethylfurfural (5-HMF) has been a hotspot in biomass conversion research in recent years. In this study, a novel SAPO-34-based catalyst was prepared by consecutive steps of titanium doping, sulfuric acid impregnation, and sulfonic acid functionalization. Characterization of the catalyst with X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), BrunauerEmmett-Teller (BET), inductively coupled plasma optical emission spectrometer (ICP-OES), and acid-base titration revealed different pore structures and more acid content compared to SAPO-34. The catalyst was applied to the preparation of 5-HMF by dehydration of fructose, and the maximum yield (74.0%) of 5-HMF was obtained by reacting in dimethyl sulfoxide (DMSO) at 170 °C for 50 min. In addition, the applicability of the catalytic system to other substrates and the stability of the catalyst after five cycles were investigated, which are valuable for further probing on the concerned aspects.
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Journal of Cleaner Production
·
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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Biomolecules
·
2021
·Vol. 11
·期 9
·1370
·
IF 4.879
Shuyi Liao,Wenmin Yang,Ting Yu,Lu Dai,Xiaoliang Liu,Jiangping Zhang,Jinghong Zhao,Chi Liu
Acute renal failure (ARF) is a clinical critical syndrome with rapid and severe decline of renal function. Complications of ARF, especially its cardiac complications (cardiorenal syndrome type 3, CRS-3), are the main causes of death in patients with ARF. However, the shortage and limited efficacy of therapeutic drugs make it significant to establish new large-scale drug screening models. Based on the Nitroreductase/Metronidazole (NTR/MTZ) cell ablation system, we constructed aTg(cdh17:Dendra2-NTR)transgenic zebrafish line, which can specifically ablate renal tubular epithelial cells. The absence of renal tubular epithelial cells can lead to ARF in zebrafish larvae. The ARF symptoms, such as heart enlargement, slow heart rate and blood stasis, are similar to the clinical manifestations of human CRS-3. Furthermore, two therapeutic drugs (digoxin and enalapril) commonly used in the clinical treatment of heart failure were also effective in alleviating the symptoms of CRS-3 in zebrafish, which proved the effectiveness of this model. Drug screening further discovered a potential drug candidate, α-lipoic acid, which can effectively alleviate the symptoms of CRS-3 through its antioxidant function. Accordingly, we established a new ARF model of zebrafish, which laid a foundation for large-scale screening of new therapeutic drugs for its complications.Keywords:acute renal failure (ARF);cardiorenal syndrome (CRS);zebrafish model;drug screening;nitroreductase (NTR);metronidazole (MTZ)
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ENERGY & FUELS
·
2019
·
IF 3.021
Yuan Zhao,Kaifeng Lu,Hao Xu,Yang Qu,Lingjun Zhu,Shurong Wang
5-Hydroxymethylfurfural (HMF), a well-known value-added platform chemical, can be produced by biomass dehydration for the synthesis of bio-based liquid fuels. In this study, several kinds of saccharides that are widely available from biomass resources, namely, sucrose, maltose, cellobiose, lactose, inulin, and cellulose, were selected as feedstocks. A sulfonated ionic liquid catalyst was employed for the production of HMF from the selected saccharides in a renewable butanone–water solvent mixture. The yields of primary dehydration products versus time on stream from the saccharides were comparatively studied, and the distribution of the liquid-phase product was also analyzed. Results showed that the proposed reaction system could achieve fast conversion of disaccharides and polysaccharides with high selectivity toward HMF. Complete conversion of disaccharide and up to 65.1% yield of HMF were achieved within 1 min. Sucrose and inulin, which are rich in the fructose unit, showed the highest HMF selectivity. The next were maltose, cellobiose, and cellulose, which mainly consist of the glucose unit. They produced more oxygenated aliphatics than sucrose and inulin via side reactions. Lactose had the lowest HMF selectivity and tended to be converted into furan byproducts during the dehydration process.
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PROCESS BIOCHEMISTRY
·
2019
·
IF 2.883
Ping Zhu,Yan Zeng,Peng Chen,Yan Men,Jiangang Yang,Xiaoping Yue,Jiangang Zhang,Yueming Zhu,Yuanxia Sun
A one-pot two-enzyme reaction system was developed to produce high-fructose syrup (HFS) containing healthy rare sugar d-allulose from Jerusalem artichoke (JA). Inulin in JA was converted through the cascade reaction of a novel exo-inulinase from Bacillus velezensis (BvInu) and D-allulose 3-epimerase from Ruminococcu s sp. (RDAE). BvInu and RDAE were expressed in Bacillus subtilis and successfully secreted into the supernatant, which decrease the production cost and avoid enzyme purification. The optimal temperature and stability of extracellular BvInu significantly increased, thereby promoting the catalytic activity of the two enzymes for the cascade reaction in one pot. Inulin in JA powder was almost completely converted into monosaccharides in the treatment with the optimal ratio of BvInu : RDAE (80 : 40 U/g inulin) at 50 °C for 2 h. The ratio of D-glucose, D-fructose, and D-allulose in the product was approximately 1:3:1, and the yield on JA powder was 67%. The system exhibits potential high-valued application of non-grain crops on producing HFS with D-allulose.
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 14
·3930-3939
·
IF 9.405
Guo Qiu,Chongpin Huang,Xiuliang Sun,Biaohua Chen
Bio-based platform chemical 5-hydroxymethylfurfural (5-HMF) can be converted into large-scale, high value-added compounds generally obtained from petroleum. Hence, developing an efficient catalytic system to transform glucose (a cheap and abundant branch of biomass) into 5-HMF has drawn significant attention. Earlier reports have concentrated on a two-step conversion of glucose to 5-HMF involving glucose isomerization into fructose and subsequent dehydration. In this work, efficient heterogeneous niobium-loaded montmorillonite (Nb-MMT) catalysts containing Lewis and Brønsted acid sites have been synthesized by a readily cation-exchanged synthetic method and were used to convert glucose and showed high selectivity and conversion. An optimum 5-HMF yield of 70.52% with a 99% conversion of glucose was achieved in a biphasic solvent of methyl isobutyl ketone (MIBK)/water at 170 °C for 3 h. The catalytic system also exhibited an excellent activity in the conversion of disaccharides and polysaccharides to 5-HMF with satisfactory yields. In addition, Nb-MMT was effectively reused four times without significant loss of activity. Nb-MMT also featured good catalytic activity and selectivity towards carbohydrate conversion in water. Furthermore, the reaction mechanism for the transformation of glucose to 5-HMF over Nb-MMT was investigated by density functional theory (DFT) calculations, and the results showed that niobium oxyhydroxide species of Nb-MMT played an essential role in glucose conversion, and the catalytic mechanism was a synergetic proton transfer process via hydrogen bonding. This study paves the way for improvements in Nb-containing solid acid catalysts for conversion of carbohydrates.
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CHEMICAL ENGINEERING SCIENCE
·
2019
·
IF 3.372
Jun Zhang,Kaijun Dong,Weimin Luo
A facile and mild method for the catalytic production of 2,5-dimethylfuran (DMF) from 5-hydroxymethylfurfural (HMF) was developed, which utilized commercial PdCl 2 as the catalyst together with the green, non-toxic and low-cost hydride source, polymethylhydrosiloxane (PMHS). A synergistic effect among hydrogen donor, in situ generated metallic Pd 0 species and acid site HCl in the reaction played a key role in DMF formation. Gratifyingly, the desirable yield of hydrodeoxygenation product DMF as high as 89.7% from HMF was attained at room temperature (298 K) in 0.5 h. Meanwhile, biomass derived sugars also could be converted into DMF in relative high efficiency via a one-pot reaction in the present system. A plausible pathway for the hydrodeoxygenation of HMF into DMF in the present system was also proposed. The study thus highlights a new perspective for a simple, green, and efficient hydrodeoxygenation of biomass derivatives under milder conditions, employing a readily available, inexpensive and practical catalytic system of PdCl 2 -PMHS-ethanol, but without any external hydrogen supplies and pre-reduction treatments.
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Foods
·
2019
·Vol. 8
·期 6
·181
·
IF 3.011
Rui Li,Qi Ding,Xin-Huai Zhao
The impact of milk fortification on the microbiological and physicochemical properties of a set-type skimmed yoghurt using three commercial soluble prebiotics (inulin, iso-malto-oligosaccharides, and xylo-oligosaccharides) at either 3 or 5 g/kg was assessed. The three prebiotics had an insignificant impact on yoghurt fermentation because all yoghurt samples had similar titratable acidity and similar pH values after their lactic acid fermentation. Regarding the control yoghurt samples without prebiotics usage, the prebiotics-fortified yoghurt samples showed no difference in their main chemical compositions, hardness, syneresis extent, and apparent viscosity (p> 0.05), but had a slightly higher lactic acid content and a viable quantity of starter strains. All yoghurt samples had the same acetic acid content, while propionic and butyric acids were not produced. Yoghurt storage at 4 °C for 21 day gave these yoghurt samples decreased pH values and a viable quantity of starter strains (especiallyLactobacillus delbrueckiisubsp.bulgaricus) and unchanged acetic acid; however, it increased lactic acid contents. Overall, prebiotics fortification up to 5 g/kg had a completely insignificant impact on the fermentation and quality attributes of yoghurt samples but could possibly improve the health of consumers due to higher dietary fibers and starter strain populations.Keywords:set-type skimmed yoghurt;inulin;iso-malto-oligosaccharides;xylo-oligosaccharides;yoghurt quality
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2018
·
IF 3.909
Peilin Chen,Qingxiang You,Xin Li,Qing Chang,Yi Zhang,Baodong Zheng,Xiaoke Hu,Hongliang Zeng
In this study, the relationships between the proliferation effect of polysaccharide fractions from the citrus shrub Fortunella margarita on Bifidobacterium adolescentis ATCC 15703 and their resulting structural changes were investigated. Four polysaccharide fractions, FP20, FP40, FP60, and FP80, were obtained by graded precipitation at ethanol concentrations of 20%, 40%, 60% and 80%, respectively. The results showed that polysaccharide fractions, especially FP20, FP40, and FP60, enhanced the proliferation of B. adolescentis ATCC 15703 and their effects were better than those of FP80, inulin or glucose. Moreover, acetic acid was mainly produced during fermentation. After fermentation, the molecular weight of polysaccharide fractions decreased and the tightly structural chain conformations of FP20, FP40, and FP60 changed to highly branched structures. The prebiotic effect of these polysaccharide fractions might be related to their molecular weight and chain conformation. Thus, these polysaccharides could be used as potential prebiotics.
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ChemSusChem
·
2013
·Vol. 6
·期 5
·820-825
·
IF 7.475
Qingbin Wu,Yani Yan,Qian Zhang,Jinhua Lu,Zhijian Yang,Yahong Zhang,Yi Tang
Graphical Between the sheets: A simple and efficient microwave-assisted HNb 3 O 8 catalytic process is proposed for the dehydration of carbohydrates in a sustainable pure aqueous system, in which the fast in situ exfoliation of the layered HNb 3 O 8 under microwave irradiation is crucial for the remarkable catalytic performance. A simple and efficient microwave-assisted HNb 3 O 8 catalytic process is proposed for the dehydration of carbohydrates in the aqueous phase. A 5-hydroxymethylfurfural (HMF) yield of 55.9 % was achieved at a high substrate/catalyst weight ratio of 50 from a 10 wt % fructose solution, which is close to the yield achieved by homogeneous aqueous systems. The critical factor for this performance is the fast in situ exfoliation of layered HNb 3 O 8 with the aid of microwave irradiation, which leads to quasi-homogeneous catalytic behavior. Importantly, the catalytic system is also applicable for the one-pot production of HMF from di- and polysaccharides, such as inulin, through a consecutive hydrolysis–dehydration reaction. Additionally, the unique restacking feature of the exfoliated HNb 3 O 8 ensures the good reusability of the catalyst.
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RSC Advances
·
2013
·Vol. 3
·期 20
·7360-7366
·
IF 2.562
Shimin Kang,Jun Ye,Yu Zhang,Jie Chang
Amorphous carbon-based sulfonated catalysts were generated from four kinds of biomass (lignin, cellulose, wood meal and D-xylose) by hydrothermal carbonization at various temperatures (225, 245 and 265 °C) followed by sulfonation, with a yield of 36–56%. All of these catalysts showed aromatic structure, hydroxyl and carboxyl groups, with a density of SO3H groups between 0.56 and 0.87 mmol g−1. 5-Hydroxymethylfurfural (HMF) was produced from inulin in ionic liquids (ILs) in one step with the addition of carbon-based sulfonated catalysts, with a factual yield of 47–65% at 100 °C, 60 min. Moderate extension of reaction time (from 30 to 90 min) and increase of temperature (from 80 to 120 °C) promoted HMF production. Ethyl acetate was used as extractant, and about 39–55% of HMF can be recovered from ILs. One problem with these carbon-based sulfonated catalysts was that they would be partly deactivated in ILs for separate reuse, however, they can be easily regenerated by dilute sulfuric acid treatment. The carbon-based sulfonated catalysts exhibited good catalytic activity compared with traditional solid acid catalysts, and the carbon-based sulfonated catalyst/ILs reaction system showed high reusability. In consideration of the renewable as well as the high catalytic activity abilities, these biomass derived carbon-based sulfonated catalysts would be promising for industrial application.
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