RSC Advances
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2019
·Vol. 9
·期 19
·10569-10577
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IF 3.049
Jianru Ma,Wenzhi Li,Shengnan Guan,Qiying Liu,Qingqing Li,Chaofeng Zhu,Tao Yang,Ajibola Temitope Ogunbiyi,Longlong Ma
Sulfonated graphene (SG) was prepared and employed to convert corn stalk and xylose into furfural. Transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR) were used to characterize SG. The effects of reaction time, temperature, substrate loading, catalyst dosage and solvents on the reaction were researched and optimized. SG exhibited high catalytic activity in the conversion of xylose and corn stalk to furfural. A fairly high furfural yield of 96% was achieved at 150 °C from xylose and a 71.9% furfural yield was obtained when using a 10.7 ratio (mass ratio: xylose to SG) at 140 °C. While a 48% furfural yield was obtained from corn stalk (based on the starting combined moles of xylan and glucan in corn stalk; yield was >100%, if based on only xylan) using a substrate loading (corn stalk to catalyst mass ratio) of 2.14 and a 19% 5-hydroxymethylfurfural (5-HMF) yield was obtained. What's more, a 43.9% yield of furfural was obtained in only 20 min. In addition, the reusability of SG was also investigated and shown to have good stability for xylose dehydration.
研究领域:
生物化学
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材料科学
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2019
·
IF 4.084
Tingwei Zhang,Yijuan Lu,Wenzhi Li,Mingxue Su,Tao Yang,Ajibola Ogunbiyi,Yongcan Jin
In order to efficiently produce γ-valerolactone (GVL) from furfural , a Zr-graphitic carbon nitride/H-β composite (Zr CN/H-β) had been simply prepared via an impregnation-calcination protocol. The morphology and structure, elemental information, and total acid and base properties of the Zr CN/H-β and related catalysts (H-β, CN/H-β, and Zr/H-β) were determined by SEM, TEM , X-ray photoelectron spectroscopy (XPS), and temperature-programmed desorption (TPD-NH 3 , CO 2 ) characterizations. The effects of reaction temperature and time, and the furfural dosage on GVL production as well as the recyclability of Zr CN/H-β were investigated. With a catalyst/furfural dosage of 0.1/0.22 g, the Zr CN/H-β produced a remarkable 76.5% of GVL yield at 160 °C in 18 h using isopropanol as the solvent. The results of NH 3 , CO 2 -TPD experiments indicated that the simultaneous introduction of Zr species and carbon nitride onto H-β formed new types of acid and base, which should be responsible for the high efficient conversion of furfural to GVL. Additionally, the recyclability of Zr CN/H-β was reasonable.
研究领域:
化学工程
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催化科学
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Shanhui Zhu,Huan Liu,Sen Wang,Xiaoqing Gao,Pengfei Wang,Jianguo Wang,Weibin Fan
One-step efficient conversion of cellulose into value-added γ-valerolactone (GVL) is of great interest because it not only integrates complex tandem reactions in one-step, but also does not need additional hydrogen sources. To achieve this goal, it is crucial to fabricate high-performance catalyst that can accelerate both hydrolysis of cellulose and further transformation of generated stoichiometric levulinic acid (LA) and formic acid (FA) into GVL. CoNi nanoparticles encapsulated in N-doped thin graphene shell gave GVL yield as high as 55.9 % at 200 °C combined with Ag + -exchanged heteropolyacid (AgPW). This composite catalyst is highly resistant to the corrosion of LA and FA, and hence shows high catalytic stability. LA-adsorption FTIR spectra and DFT calculations indicate that LA and FA can penetrate through shell graphene layers into core CoNi sites via cracks. Compared to H 2 , FA can much more rapidly reduce LA because of its low dissociation energy barrier and high dissociation rate.
研究领域:
化学工程
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催化
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材料科学
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生物化工
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2013
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IF 5.825
Xing Tang,Huawei Chen,Lei Hu,Weiwei Hao,Yong Sun,Xianhai Zeng,Lu Lin,Shijie Liu
A series of low-cost readily-assembled eco-friendly metal hydroxides were examined as catalysts in the synthesis of a novel platform molecule, γ-valerolactone (GVL), from biomass-derived ethyl levulinate (EL) via hydrogen transfer reaction. Among these catalysts, ZrO(OH) 2 · x H 2 O was found to be most active. EL conversion of 93.6% and GVL selectivity of 94.5% were achieved when 2-propanol was used as a hydrogen donor at 473 K with a reaction time of only 1 h. The complete reaction pathway and the probable main by-products for the conversion of EL to GVL were clearly deduced for the first time. The ZrO(OH) 2 · x H 2 O catalyst could be reused at least ten times without any significant loss of catalytic activity. Furthermore, characterizations were carried out on the fresh and spent ZrO(OH) 2 · x H 2 O catalysts with XRD, FT-IR, BET, TGA-DTA. Combined with the results of poisoning experiments, a plausible mechanism for catalytic transfer hydrogenation (CTH) of EL to GVL was proposed to be consisted of a catalytic cycle involving a six member ring transition state.
研究领域:
化学工程
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催化
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绿色化学
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可再生能源
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高影响因子
E-POLYMERS
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2019
·Vol. 19
·期 1
·323-329
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IF 1.491
XianRong Shen,DengZhou Xia,YiXin Xiang,JianGang Gao
In this paper, γ-valerolactone (GVL), a bio-based polar solvent, was applied as green solvent for iron(III)-catalyzed AGET ATRP without any external ligand. GVL is a fully degradable, non-toxic green solvent and has complex ability to iron halide complexes through –OCO- group. GVL as the solvent and the ligand for AGET ATRP of MMA in a controlled manner, as proved by kinetic study, the low PDI values and the increase in polymer molecular weight versus monomer conversion. Chain re-initiation experiments and 1 HNMR characterization were conducted to further confirm the living feature. Graphical
研究领域:
材料科学
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化学工程
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高影响因子
BIORESOURCE TECHNOLOGY
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2015
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IF 4.494
Zhiping Xu,Wenzhi Li,Zhijie Du,Hao Wu,Hasan Jameel,Hou-min Chang,Longlong Ma
A novel solid acid catalyst was prepared by the copolymerization of p-toluenesulfonic acid and paraformaldehyde and then characterized by FT-IR, TG/DTG, HRTEM and N 2 -BET. Furfural was successfully produced by the dehydration of xylose and xylan using the novel catalyst in γ-valerolactone. This investigation focused on effects of various reaction conditions including solvent, acid catalyst, reaction temperature, residence time, water concentration, xylose loading and catalyst dosage on the dehydration of xylose to furfural. It was found that the solid catalyst displayed extremely high activity for furfural production. 80.4% furfural yield with 98.8% xylose conversion was achieved at 170 °C for 10 min. The catalyst could be recycled at least five times without significant loss of activity. Furthermore, 83.5% furfural yield and 19.5% HMF yield were obtained from raw corn stalk under more severe conditions (190 °C for 100 min).
研究领域:
化学工程
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生物质能
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PubMed
高影响因子
ChemPlusChem
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2015
·Vol. 81
·期 1
·135-142
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IF 3.026
Hu Li,Zhen Fang,Song Yang
Graphical Attractive separation : Acid–base bifunctional NiZr nanocatalysts with strong magnetism show high activity and reusability in the transformation of biomass derivatives, including EL, fructose, glucose, cellobiose, and carboxymethyl cellulose, into γ -valerolactone (GVL) with 95.2 % yield and 98 % selectivity (see figure). A series of mixed oxide nanoparticles were prepared by a coprecipitation method and characterized by many techniques. Nickel–zirconium oxide catalysts and their partially reduced magnetic counterparts were highly efficient in the direct transformation of biomass derivatives, including ethyl levulinate, fructose, glucose, cellobiose, and carboxymethyl cellulose, into γ-valerolactone (GVL) without the use of an external hydrogen source, producing a maximum GVL yield of 95.2 % at 200 °C for 3 h with hydrogen-reduced magnetic Zr 5 Ni 5 nanoparticles (<20 nm). The acid–base bifunctionality of these nanocatalysts plays a synergic role in the synthesis of GVL in alcohols, whereas appropriate control of the nickel/zirconium molar ratio is able to improve the selectivity towards GVL (≈98 %), along with high formation rates (up to 54.9 mmol g −1 h −1 ). Moreover, the magnetic Zr 5 Ni 5 nanoparticles were conveniently recovered by means of a magnet for five cycles with almost constant activity.
研究领域:
化学工程
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催化材料科学
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PubMed
高影响因子
CATALYSIS TODAY
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2016
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IF 4.312
Kun Jiang,Dong Sheng,Zihao Zhang,Jie Fu,Zhaoyin Hou,Xiuyang Lu
Mixed MgO–Al 2 O 3 (with different Mg/Al ratio) supported nickel catalysts were prepared via co-precipitation method and used for hydrogenation of levulinic acid to γ-valerolactone under mild condition. Characterization results indicated that mixed MgO–Al 2 O 3 supported Ni catalysts possessed bigger surface area than that of Ni/MgO and Ni/Al 2 O 3 , and Ni dispersed highly on the surface of mixed MgO–Al 2 O 3 support. It was found that mixed MgO–Al 2 O 3 supported Ni catalysts were more active and selective for the hydrogenation of levulinic acid to γ-valerolactone than that of Ni/MgO and Ni/Al 2 O 3 , and the best yield of γ-valerolactone at 160 °C, 1 h and 3 MPa H 2 reached 99.7% over Ni/MgAlO 2.5 , and Ni/Mg 2 Al 2 O 5 could be recycled without obvious loss of its initial activity.
研究领域:
化学工程
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催化化学
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高影响因子
ENERGY & FUELS
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2017
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IF 3.091
Haizhou Lin,Jingping Chen,Yuan Zhao,Shurong Wang
To obtain an efficient and green reaction system for the production of furfural (FF), this study investigated the use of a SO3H-functionalized ionic liquid as a catalyst for the conversion of xylose in a solvent of renewable γ-valerolactone (GVL). A high FF yield of 78.12% was obtained in this reaction system catalyzed by 1-propylsulfonic-3-methylimidazolium chloride at 140 °C. The GVL remarkably enhanced the reaction rate and increased the xylose conversion and FF yield because the solvent effect of GVL could improve the catalytic activity of the acidic protons and suppress the side reactions. In addition, the ionic liquids showed satisfactory catalytic performance in the conversion of xylose to FF due to functionalization by introducing a SO3H group. The conversion of other C5 carbohydrates (arabinose and xylan) was also tested in this system, and moderate FF yields were achieved.
研究领域:
生物化学
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绿色化学
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高影响因子
CATALYSIS TODAY
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2017
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IF 4.636
Zhijie Wu,Min Zhang,Yirong Yao,Jingtuo Wang,Danhong Wang,Minghui Zhang,Yongfeng Li
1,3-propanediol (1,3-PDO) and γ-valerolactone (GVL) were simultaneously obtained via the hydrogenolysis of glycerol in levulinic acid (LA) using Ru/C catalysts. Ru/C catalyst exhibited a high LA conversion (∼99%) and a high GVL selectivity (∼99%) for the hydrogenation of LA; while a low conversion (∼11%) and little selectivity of 1,3-PDO for the hydrogenolysis of glycerol. LA promoted the hydrogenolysis of glycerol over Ru/C catalyst, in which LA catalyzed dehydration of glycerol into acetol (precursor of 1,2-propanediol (1,2-PDO)), and glycerol acetalization with the hydrogenated GVL into cyclic acetals, resulting in the formation of 1,3-PDO. A reaction scheme involves the formation of cyclic acetal ethers between GVL and glycerol was proposed to explain the product distributions in the one-pot synthesis of 1,3-PDO and GVL. 64.5% conversion of glycerol and 35.8% selectivity of 1,3-PDO together with 99.1% conversion of LA and 85.8% selectivity of GVL were obtained during one-pot converting glycerol and LA with 3.0 MPa H 2 at 200 °C for 6 h. We reported an effective strategy for the preparation of 1,3-PDO by selective hydrogenolysis of dioxan originated from glycerol with aldehydes or ketones.
研究领域:
生物化学
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催化化学
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高影响因子
ChemSusChem
·
2017
·Vol. 10
·期 8
·1720-1732
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IF 7.226
Zuojun Wei,Jiongtao Lou,Chuanmin Su,Dechao Guo,Yingxin Liu,Shuguang Deng
Graphical Stability through doping : The embedding of Ru nanoparticles in N-doped mesoporous carbon effectively improve the dispersion and decrease the average size of the Ru nanoparticles, improve the adsorption of levulinic acid, and increase the interaction between Ru and the support. The strategy prevents the Ru nanoparticles from migration, aggregation, and leaching, and consequently increases the reusability of the catalyst. To achieve a higher activity and reusability of a Ru-based catalyst, Ru nanoparticles were embedded in N-doped mesoporous carbon through a hard-template method. The catalyst showed excellent catalytic performance (314 h −1 turnover frequency) and recyclability (reusable five times with 3 % activity loss) for the hydrogenolysis of levulinic acid to γ-valerolactone. Compared with the mesoporous carbon without N-doping and conventional activated carbon, the introduction of N-dopant effectively improved the dispersion of Ru nanoparticles, decreased the average size of Ru nanoparticles to as small as 1.32 nm, and improved the adsorption of levulinic acid, which contributed to the increase in the activity of the catalyst. Additionally, the embedding method increased the interaction between Ru nanoparticles and carbon support in contrast with the conventional impregnation method, thus preventing the Ru nanoparticles from migration, aggregation, and leaching from the carbon surface and therefore increasing the reusability of the catalyst.
研究领域:
催化
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化学工程
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材料科学
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PubMed
高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
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2022
·Vol. 48
·期 3
·1181-1198
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IF 3.134
Zhang Zhongze,Liu Zonghui,Gu Zhiyuan,Wen Zhe,Xue Bing
The catalytic transfer hydrogenation (CTH) reaction of ethyl levulinate (EL) with alcohol to γ-valerolactone (GVL) has been investigated over a series of Zr-based catalysts, including ZrO 2 , ZrP, Zrβ, ZrP/Hβ and ZrO 2 /HZSM-5. It is found that the simplest ZrO 2 was the most efficient for GVL production, giving an EL conversion as high as 97% and GVL selectivity of 91% after 7 h at 170 °C using 2-propanol as the hydrogen donor and solvent. The effects of reaction temperature, time and solvent on catalytic performance were investigated. Moreover, the kinetic behavior of CTH reaction of EL was also studied over ZrO 2 catalyst. The as-prepared ZrO 2 gives an Ea value of 32.9 kJ/mol, which is much lower than other catalysts in the literatures. Furthermore, those catalysts have been, respectively, characterized by XRD, IR, BET and NH 3 -TPD techniques to reveal the physical properties and structures of these materials. Correlating the catalyst performance with its physical and chemical properties uncovers that the higher pore diameter, lower total acidity and higher Lewis acid sites of catalyst surface would be the key to the catalyst performance. Graphical abstract
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危险品化学品经营许可证（带存储）