Biomass Conversion and Biorefinery
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2021
·Vol. 13
·期 3
·2017-2028
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IF 4.987
Zhang Zhenshu,Du Boyu,Zhu Hongwei,Chen Changzhou,Sun Yang,Wang Xing,Zhou Jinghui
To improve lignin depolymerization reaction performance of HZSM-5 zeolite catalyst, we reported the effective catalytic depolymerization of rice husk lignin (RHL) to lignin phenolic monomer (LP) products over the different Si/Al mole ratios of HZSM-5 zeolite catalyst. Firstly, five samples comprising different Si/Al mole ratio of HZSM-5 zeolite catalyst were prepared by the physical method. The X-ray powder diffraction (XRD), scanning electron microscope (SEM), Brunauer–Emmett–Teller (BET), pyridine adsorption Fourier transform infrared spectroscopy (FT-IR), and temperature-programmed desorption of ammonia (NH 3 -TPD) were used to characterize various catalysts. Secondly, gas chromatography–mass spectrometry (GC-MS), 2D heteronuclear single quantum coherence (2D-HSQC), and gel permeation chromatography (GPC) were used to characterize various catalytic depolymerization products. The effect of different Si/Al molar ratios on the lignin conversion to LP products and the structural changes of residual lignin were analyzed. Finally, according to the results of LP products, we discovered that after the use of different Si/Al molar ratios of HZSM-5 zeolite catalysts, the content of acid in the different catalysts which increased with decreasing the Si/Al mole ratios. Among them, the A4P PM products (A4P: having a saturated or unsaturated aliphatic side chain in C4 position) increased from 0.58% (SA560, Si/Al: 560) to 1.83% (SA70, Si/Al: 70), the C6P PM products (C6P: having no side chain in C4 position of G, S, and H structure) increased from 1.53% (SA560, Si/Al: 560) to 3.41% (SA70, Si/Al: 70). Finally, the highest 6.05% PM products yield appeared in the SA70 (Si/Al: 70) catalytic system. It is worth noting that PM products produced by this HZSM-5 zeolite catalyst SA70 have great potential to be a promising renewable alternative to fossil resources. Graphical abstract
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Yaoyu Zhang,Yuxing Wang,Yue Liu,Qingji Ying,Zhongbiao Wu
A sequence of CuCeO x -HZSM-5 composite catalysts at different Cu-Ce loading synthesized by the citric acid complex impregnation method were evaluated for the catalytic oxidation of acetonitrile. Among which, the 2CuCeO x -HZSM-5 sample exhibited the best degradation efficiency. In the temperature range of 225–350 °C, its activity and mineralization rate were approximately 100%, and the N 2 selectivity remained more than 93%. The characterization results revealed that all the samples showed an existence of isolated Cu 2+ species. And more Cu-Ce mixed oxides covered on HZSM-5 at an elevated Cu-Ce content, leading to the enhanced reducibility. In situ DRIFTS results showed that both oxidation and hydrolysis reaction routes proceeded during the degradation of acetonitrile over the composite catalysts. Their synergism was crucial to guarantee both high activity and N 2 selectivity. The highly dispersed CuO x species ensured the superior activity of the 2CuCeO x -HZSM-5 sample. And Cu 2+ exchanged HZSM-5 zeolite would be beneficial to N 2 selectivity owing to the improved internal SCR (Selective Catalytic Reduction) reaction to reduce NO x from oxidation routes. Additionally, the mineralization rate was lowered with the formation of carbonaceous products like CH 4 and CO for the catalysts at low Cu-Ce loading due to the lack of redox capacity.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2020
·
IF 4.244
Tao Yang,Wenzhi Li,Ajibola T. Ogunbiyi,Shengxin An
A novel solid acid catalyst (SO 3 H-NG-C) was synthesized from biomass-derived glucosamine hydrochloride by carbonization, activation and sulfonation processes. The SO 3 H-NG-C was characterized by SEM, TEM, N 2 adsorption-desorption, elemental analysis, XRD, FTIR, Py-IR and XPS to reveal its physical and chemical properties. The SO 3 H-NG-C was used as a catalyst for converting corn stover into furfural and 5-hydromethylfurfural (5-HMF) via a one-step process. The effects of reaction temperature and time, solvent types, water concentrations, corn stover concentration, catalyst loading and catalyst stability were investigated systematically. 53 % furfural yield and17 % 5-HMF yield were obtained from 200 mg corn stover at 190 °C in 80 min using 100 mg SO 3 H-NG-C in Ƴ-valerolactone (GVL). Moreover, the used catalyst was separated from corn stover residue via sieve, and the catalyst showed reasonable stability for corn stover conversion.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2020
·
IF 3.905
Haohao Wu,Lu Wang,Guangbo Ji,Hanwu Lei,Hao Qu,Juan Chen,Fangbin Wang,Jian Liu
In this work, we evaluated the potential for the production of nitrogen-containing compounds (NCCs) and hydrocarbons by investigating the effects of different metal-doped catalysts (Zn/Cu/Ni/HZSM-5) on catalytic pyrolysis of chlorella using microwave heating. All bio-oils exhibited stratification with the upper/lower layer corresponding to the oil/water phase. The results showed that NCCs and hydrocarbons were the most abundant in the oil phase. The yields of these compounds were enhanced by the application of Zn/HZSM-5 and Cu/HZSM-5, reaching 55.5 area% and 47.5 area%, respectively, compared with the unmodified HZSM-5 (40.9 area%). In the water phase, the NCCs content achieved 42.3 area% with Zn/HZSM-5, 29.6 area% with Cu/HZSM-5, and 39.5 area% with Ni/HZSM-5, respectively, all higher compared with the unmodified HZSM-5 (22.4 area%). This study provides an effective method for green production of NCCs and hydrocarbons that are important structural components in many industries and promotes the application of biomass resources.
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Frontiers of Chemical Science and Engineering
·
2020
·Vol. 15
·期 2
·269-278
·
IF 3.552
Hou Yuexin,Li Xiaoyun,Sun Minghui,Li Chaofan,Bakhtiar Syed ul Hasnain,Lei Kunhao,Yu Shen,Wang Zhao,Hu Zhiyi,Chen Lihua,Su Bao-Lian
Hierarchical single-crystal ZSM-5 zeolites with different Si/Al ratios (Hier-ZSM-5- x , where x = 50, 100, 150 and 200) were synthesized using an ordered mesoporous carbon-silica composite as hard template. Hier-ZSM-5- x exhibits improved mass transport properties, excellent mechanical and hydrothermal stability, and higher catalytic activity than commercial bulk zeolites in the benzyl alcohol self-etherification reaction. Results show that a decrease in the Si/Al ratio in hierarchical single-crystal ZSM-5 zeolites leads to a significant increase in the acidity and the density of micropores, which increases the final catalytic conversion. The effect of porous hierarchy on the diffusion of active sites and the final catalytic activity was also studied by comparing the catalytic conversion after selectively designed poisoned acid sites. These poisoned Hier-ZSM-5- x shows much higher catalytic conversion than the poisoned commercial ZSM-5 zeolite, which indicates that the numerous intracrystalline mesopores significantly reduce the diffusion path of the reactant, leading to the faster diffusion inside the zeolite to contact with the acid sites in the micropores predominating in ZSM-5 zeolites. This study can be extended to develop a series of hierarchical single-crystal zeolites with expected catalytic performance.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Yunwu Zheng,Jida Wang,Can Liu,Yi Lu,Xu Lin,Wenbin Li,Zhifeng Zheng
The main objective of the present work is to investigate the influence of nickel to cerium ratio on hydrogen exchanged Zeolite Socony Mobil-5 (HZSM-5) towards the catalytic upgrading of pine derived oxygenated pyrolysis vapours into aromatic hydrocarbon and phenol in pyrolysis oil via ex-situ fixed bed reactor . The presence of CeO 2 could change electron density of Ni, promote the reduction of Ni species, accelerate the transfer of carbon species, and suppress the production of carbon deposits (17.53%–25.11%) compared with the parent HZSM-5 catalyst (28.95%); it also improved the hydrodeoxygenation ability of all xNiyCe/HZSM-5(nickel and cerium bimetal modified HZSM-5) catalysts, resulting increases in noncondensable gas content (from 31.46% to 52.99%–65.53%). Ni to Ce ratio of 1:1 and 1:2 produced highest aromatic hydrocarbon (32.14%) and phenols (55.51%) relative peak areas. The acid center of HZSM-5 and the metal acid center of the Ni:Ce = 1:1 catalyst obviously fine-tuned the formation of coke; and promoted hydrocarbon production. Moreover, high Ni content promoted alkylation of benzene at C6–C9 and increased C10 + PAHs relative peak area; high Ce content promoted the formation of olefin and Increasing the cleavage of C–O bonds and promoted hydrogenation or dehydrogenation , reduced polycyclic aromatic hydrocarbons and coke yield, and increased phenols and alkylphenols selectivity.
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BIOMEDICINE & PHARMACOTHERAPY
·
2021
·
IF 6.53
Liyun Zeng,Qiongyan Zou,Peng Huang,Li Xiong,Yan Cheng,Qitong Chen,Yitong Li,Hongye He,Wenjun Yi,Wu Wei
Secondary hyperparathyroidism (SHPT), the most common complication in the later stage of chronic kidney disease (CKD), seriously affects quality of life and the survival time of patients. At present, the conventional drugs and surgical methods still cannot fully meet the needs of clinical treatment. It is quite significant to develop effective and minimally invasive treatment methods. 5-Aminolevulinic acid-mediated photodynamic therapy (5-ALA-PDT), an alternative treatment relying on light irradiation, photosensitizer, and oxygen to produce a series of cytotoxic effects on tissue, is a promising technique for treating SHPT. We have successfully cultivated SHPT primary cells and organoids, and further proved that the amount of 5-ALA transformed into protoporphyrin IX in a time- and concentration-dependent manner. Also, 5-ALA-PDT exerted a cytotoxic effect on both primary cells and organoids by the cell counting kit (CCK-8) assay. Mechanically, 5-ALA-PDT increased the number of autophagosomes, and autophagy- and apoptosis-related proteins were upregulated markedly by western-blotting. The autophagy inhibitor Chloroquine (CQ) significantly increased the proportion of apoptotic cells, while the autophagy inducer rapamycin decreased the inhibitory ability of 5-ALA-PDT in SHPT primary cells. In brief, 5-ALA-PDT exhibits a phototoxic effect on SHPT primary cells and organoids. Autophagy and apoptosis are involved in the mechanism, and autophagy plays a role in promoting survival and inhibiting apoptosis. Therefore, the use of autophagy inhibitors can increase the sensitivity of SHPT cells and organoids treated with 5-ALA-PDT.
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PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Changhao Yan,Shouteng Zheng,Na Chen,Shouqi Yuan,Yao Chen,Bing Li,Yunlei Zhang
In this work, the novel acid-base bi-functional mesoporous SBA-15 catalysts with four kinds of morphologies were synthesized by Mg incorporated and sulfated zirconia (SZ) grafted. The introduction of Mg to mesoporous SBA-15 materials significantly improves the strength of the base. And the supported SZ group exhibit effective Brønsted/Lewis acid strength. The physical and chemical properties of the prepared materials were systematically analyzed by the characterization tests of SEM, TEM, XRD , N 2 adsorption-desorption of, FT-IR, TGA , XPS, NH 3 /CO 2 -TPD and in-suit PY-IR. The obtained catalysts of SZ@Mg-SBA-15 could be applied to the fructose conversion into 5-hydroxymethylfurfural (5-HMF) with the co-solvent system of iPrOH/DMSO ( v / v = 9:1). 5-HMF was achieved under the optimal reaction condition with the highest yield of 98.6%. The result shows that the reaction of fructose dehydration into 5-HMF could be caused by the combination of Brønsted acid site and basic site. This work developed reaction system could avoid the large use of environmentally dangerous solvents, and provides a new economical and feasible method for the large-scale conversion of fructose biomass.
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CATALYSIS LETTERS
·
2019
·Vol. 150
·期 5
·1373-1388
·
IF 2.372
Ji Qinghua,Yu Xiaojie,Yagoub Abu El-Gasim A.,Li Mo,Fakayode Olugbenga Abiola,Yan Dong,Zhou Cunshan,Chen Li
Abstract The purpose of this study was to efficiently convert the sugary food waste (SFW) to 5-hydroxymethylfurfural (5-HMF) by ultrasound-[Bmim]Cl pretreatment in ionic liquids (ILs)-ion exchange resin system. The effect of ultrasonic pretreatment on SFW and the effect of ultrasonic frequency, ILs, acid resin and catalyst load on SFW conversion were studied. The kinetic curve and the relationship between products and intermediates were studied. In addition, the structure of SFW was also studied by FT-IR and SEM. The results indicated ultrasound-[Bmim]Cl pretreatment can significantly promote the dissolution of cellulose in SFW, and the optimal ultrasonic frequency, solvent and catalyst were 20 + 40 + 60 kHz, [Bmim]Cl and D001-cc resin, respectively; under the best reaction conditions, the maximum 5-HMF yields from the orange and apple wastes were 42.15 and 44.66 mol%, respectively. The kinetic studies showed that the early stage of 100 and 120 °C was mainly the hydrolysis reaction, and late stage was mainly isomerization and dehydration reaction; the early stage of 140 and 160 °C was a rapid hydrolysis and dehydration reaction, and the late stage was mainly the rehydration reaction of 5-HMF. The relationship between the intermediate precursors and 5-HMF showed that the rates of formation and rehydration of 5-HMF increased with the increase in temperature, and the formation reaction was mainly concentrated in zone II. The FT-IR and SEM results of degradation products showed that cellulose in SFW was more easily hydrolyzed at high temperature and long time. Graphic Abstract
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高影响因子
BIORESOURCE TECHNOLOGY
·
2019
·
IF 6.669
Lele Jin,Wenzhi Li,Qiying Liu,Longlong Ma,Chao Hu,Ajibola T. Ogunbiyi,Mingwei Wu,Qi Zhang
In this study, the Mo-promoted Ir/SiO 2 (Ir-MoO x /SiO 2 ) catalysts combined with the zeolite HZSM-5 were used for the direct conversion of microcrystalline cellulose (MCC) to liquid fuel (C 5 /C 6 alkanes) in n-dodecane/H 2 O system. A synergistic effect was formed between the partially reduced MoO x species and the Ir particles, which effectively promoted the catalytic activity of Ir/SiO 2 catalyst. When the Mo/Ir molar ratio was 0.5, a high yield of C 5 /C 6 alkanes (91.7%) was achieved at 210 ℃ for 12 h. In addition, the main component of C 5 /C 6 alkanes was n-hexane, which was proven to be obtained by the hydrogenolysis of the key intermediate, sorbitol, formed from the hydrolysis and hydrogenation of MCC.
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高影响因子
CRYSTENGCOMM
·
2019
·Vol. 21
·期 34
·5095-5105
·
IF 3.382
Xia-Lin Dai,Alexander P. Voronin,Wei Gao,German L. Perlovich,Tong-Bu Lu,Jia-Mei Chen
5-Fluorouracil (5FU) is a BCS class III drug with good aqueous solubility and poor permeability, which severely limits its transdermal permeation through the stratum corneum. Herein, four cocrystals of 5FU with a series of isomeric hydroxybenzoic acids, including salicylic acid (2 : 1), 3-hydroxybenzoic acid (1 : 1) and 4-hydroxybenzoic acid (forms I and II, 1 : 1) were prepared and subjected to membrane permeation. They exhibited significantly improved membrane permeability due to the lipid solubility enhancement caused by cocrystallization. Solid-state DFT computations followed by Bader analysis based on single crystal structures were carried out to quantify the pattern of non-covalent interactions in the cocrystals. The lattice energy values were estimated as a sum of energies of non-covalent intermolecular interactions, which show a negative correlation with the lipid solubility of 1 : 1 cocrystals. This study has important implications for the use of the cocrystallization approach to improve the permeability of transdermal drugs.
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FUEL PROCESSING TECHNOLOGY
·
2019
·
IF 4.507
Lele Jin,Wenzhi Li,Qiying Liu,Longlong Ma,Song Li,Yang Liu,Baikai Zhang,Qi Zhang
The liquid fuel (made of C 5 /C 6 alkanes) was obtained directly from the hydrogenolysis of microcrystalline cellulose (MCC) with Ir-VO x /SiO 2 combined with HZSM-5 as the composite catalyst in a biphasic system (n-dodecane + H 2 O). The performance of the catalyst was investigated by carrying out a series of experiments using various V/Ir molar ratios , catalyst dosages, reaction temperatures, reaction time, hydrogen pressure and substrates. At the optimized conditions, the cellulose was almost completely converted, and at the same time, a high C 5 /C 6 yield of 85.1% was obtained at 210 °C for 24 h and 6 MPa with the V/Ir molar ratio being 0.13. These results not only proved that Ir-VO x /SiO 2 (V/Ir = 0.13) has excellent performance for the hydrogenolysis of MCC to liquid alkanes, but also indicated that vanadium is a good metal promoter for iridium . In addition, it was proven the C5/C6 alkanes were obtained via sorbitol through the combined effect of Ir-VO x /SiO 2 and HZSM-5.
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