Catalysts
·
2015
·Vol. 6
·期 1
·6
·
IF 2
Jie Fu,Dong Sheng,Xiuyang Lu
Four types of nickel catalysts supported on aluminum oxide (Ni/Al2O3) with different nickel loadings were synthesized using the co-precipitation method and were used for the hydrogenation of levulinic acid (LA) to prepare γ-valerolactone (GVL). The synthesized Ni/Al2O3catalysts exhibited excellent catalytic activity in dioxane, and the activity of the catalysts was excellent even after being used four times in dioxane. The catalytic activity in dioxane as a solvent was found to be superior to the activity in water. Nitrogen physisorption, X-ray diffraction, and transmission electron microscopy were employed to characterize the fresh and used catalysts. The effects of the nickel loading, temperature, hydrogen pressure, and substrate/catalyst ratio on the catalytic activity were investigated.Keywords:nickel supported on aluminum oxide;γ-valerolactone;levulinic acid;hydrogenation;dioxane
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
BIOCHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 4.446
Xi Cheng,Qingge Feng,Dachao Ma,Feifan Xing,Xu Zeng,Xiaoxiao Huang,Jiayang Teng,Lin Feng
A CH 3 -SBA-15-SO 3 H catalyst was synthesized for the conversion of glucose to levulinic acid. The performance of the catalyst was demonstrated by comparative experiments using γ-valerolactone solution system versus pure water system. Significantly, the conversion efficiency was almost five times higher for γ-valerolactone solution than that of the pure water. The side reactions of the γ-valerolactone solution system were probably less than that of water system. In order to provide a better understanding of the catalytic reaction and guide the engineering design, the kinetics of levulinic acid production from glucose over CH 3 -SBA-15-SO 3 H catalyst in γ-valerolactone solution were investigated. The kinetic model was established based on four differential equations, and the model results were fitted well to the experimental results. Notably, the activation energies of the production of 5-HMF and levulinic acid were 76.55 kJ/mol and 62.66 kJ/mol, respectively, which were obviously smaller than those previously reported, this may be attributed to the synergistic effect of the solid acid and the high concentration of γ-valerolactone solution.
研究领域:
化学工程
·
催化反应动力学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2026
·Vol. 40
·期 33
·18274-18283
·
IF 6
Wu Kai,Chu Chenyang,Wang Haiyong,Cao Qi,Li Mingfan,Zheng Yijie,Zhang Huiyan
Sustainable aviation fuels (SAFs) are mainly composed
of cycloalkanes,
paraffins, and aromatics, representing an inevitable alternative to
conventional fossil fuels. Alcohols and phenolic compounds act as
critical precursors to produce branched alkanes and cycloalkanes,
the major constituents of sustainable aviation fuel. Biomass is primarily
composed of C 6 sugar, and aromatic structures, which can
be employed for the production of phenolics and alcohols. However,
the direct thermal conversion of biomass results in poor selectivity
toward phenolic and alcoholic products. Based on the structural characteristics
of three typical biomass feedstocks, γ-valerolactone (GVL) pretreatment
of biomass coupled with thermal conversion to produce phenolics and
alcohols was proposed. The results showed that GVL pretreatment could
effectively decompose corncob, poplar, and pine into cellulose-rich
fractions (C 6 -based structures) and lignin-rich fractions
(aromatic structures). The highest ethanol yield of 24.4 wt % was
obtained by the catalytic hydrogenolysis of the corncob-based cellulose-rich
fraction over the Ni@C catalyst. The highest relative content (54.1%)
of phenols from fast pyrolysis of lignin-rich fractions extracted
from poplar was achieved. This work demonstrates an advanced process
to achieve a directional conversion of biomass to precursor production
of SAFs.
✓ 已验证
产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
·
2022
·
IF 4.05
Li Keying,Zhu Hengji,Zhao Yu,Yan Jingwei,Zhang Jiajian,Lin Xiuhua,Fan Liwei,Lu Zexiang
The solvent has an important impact on liquefaction conversion from biomass to efficiently obtain fuels and chemicals. In this paper, the catalytic liquefaction of woody biomass was studied using fir sawdust as raw material and concentrated sulfuric acid as catalyst in GVL/1-octanol mixed solvent with mechanical stirring and oil bath heating. The influence of GVL on liquefaction yield was discussed, and the liquefaction productions were characterized by some analysis methods to analyze the liquefaction mechanism. The results show that adding GVL benefits to improving liquefaction yield and generating high value-added monophenol because of the enhancement of the surface wettability of biomass and the inhibition of polymerization of mononuclear aromatics with other degradation products. The maximum liquefaction yield of 76.07% was obtained under the suitable conditions of fir sawdust 10 g, temperature 150 ℃, reaction time 60 min, mass ratio of sawdust/solvent 1:6, catalyst concentration 0.6 mol·L −1 , and mass ratio of GVL/1-octanol 4:6. The mechanism study reveals that aromatics originated by lignin degradation as well as small molecule ketones from cellulose and hemicellulose degradation. GVL/1-octanol as an eco-friendly solvent system exhibits a promising prospect of application in woody biomass conversion. Graphical abstract
研究领域:
生物化学
·
可再生能源
·
绿色化学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 56
·35415-35424
·
IF 3.361
Mingrui Li,Yixuan Liu,Xialing Lin,Jinyu Tan,Song Yang,Hu Li
γ-Valerolactone (GVL) is an attractive biomass-derived platform molecule that plays an important role in the production of biofuels and biopolymers. The synthesis of GVL from renewable biomass and its derivatives has great application prospects but also presents challenges due to the multiple conversion steps involved. Here, a HfCl4-mediated acid–base bifunctional catalytic system was developed, which was demonstrated to be efficient for upgrading furfural (FF) to GVL in a single pot with unprecedented performance. The Lewis acidity of Hf4+ and moderate basicity of HfO(OH)2·xH2O, and strong Brønsted acidity of HCl in situ generated from HfCl4 hydrolysis were found to play a synergistic role in the cascade reaction processes, mainly contributing to the pronounced catalytic activity. The effects of the key reaction parameters, such as the catalyst dosage, reaction time, and temperature, on GVL production were optimized by response surface methodology. It is worth mentioning that the recovered catalyst after thermal treatment could be directly used for the hydrogen transfer processes, like FF-to-furfuryl alcohol conversion. This catalytic strategy opens a new avenue for the selective conversion of biomass feedstocks involving multiple steps and complex processes.
研究领域:
化学工程
·
可再生资源与环境科学
✓ 已验证
DOI
高影响因子
ACS Omega
·
2017
·
IF 0
Tingting Yang,Hu Li,Jian He,Yanxiu Liu,Wenfeng Zhao,Zhongwei Wang,Xiaoxiao Ji,Song Yang
γ-Valerolactone (GVL) is one of the versatile platform molecules and biofuel additives derived from the lignocellulosic biomass. Herein, the efficient synthesis of GVL from biobased ethyl levulinate (EL) using alcohol as both H-donor and solvent without an external hydrogen source has been achieved over porous Ti/Zr microspheres. The catalysts (TixZry) with different Ti/Zr molar ratios were synthesized using hexadecylamine (HDA) as a structure-directing agent via a sol–gel process combined with solvothermal treatment and characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, thermal gravimetric analysis, NH3/CO2-TPD, N2 adsorption–desorption, and pyridine-IR. A high GVL yield of 90.1% at 100% EL conversion was obtained at 180 °C for 6 h over Ti2Zr8 in 2-propanol. The microspheric and porous structure, enhanced surface areas, and acid/base contents by the proper introduction of Ti species into Zr oxide were demonstrated to be responsible for the pronounced performance. The microspheric Ti2Zr8 porous catalyst could be reused at least six times with no decrease in catalytic activity.
研究领域:
催化化学
·
生物质转化
·
材料科学
✓ 已验证
DOI
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Mingya Liu,Hanli Zheng,Xiaohui Yang,Zewei Hu,Yunxi Hou,Lu Shen,Dongyu Liu,Shitao Yu,Lu Li,Shiwei Liu,Yue Liu
The high efficiency production of renewable resources has been widely used in fuel and synthetic chemistry. In this work, a series of novel, efficient Pd@mSiO 2 -xCeO 2 bifunctional yolk-shell catalysts have been developed and applied to the preparation of γ-valerolactone by the hydrogenation of levulinic acid. The results showed that CeO 2 can effectively improve the catalytic performance of the catalyst, then achieve 100 % conversion of levulinic acid and 97 % selectivity of γ-valerolactone. The characterization results showed that the addition of CeO 2 regulated the acid sites of the catalyst, promoted the reduction of PdO, thus promoting the formation of more Pd 0 . In addition, the kinetic experiment results showed that the activation energy of the reaction effectively decreased with the addition of CeO 2 . Then, the reaction mechanism was studied using Density functional theory (DFT) calculations. Finally, the encapsulation strategy of mesoporous silica shell provided a stable environment for the catalyst and maintains high activity after 5 cycles. The efficient and stable noble metal catalysts developed in this study significantly enhance the yield of biomass-derived γ-valerolactone. Their large-scale application not only supports the green production of biofuels and biodegradable materials but also establishes a material foundation for the generation of renewable energy, thereby contributing to the realization of a low-carbon circular economy.
研究领域:
催化化学
·
绿色化学
·
可再生能源
·
材料科学
·
化学工程
·
理论化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2021
·
IF 9.676
Ziyi Li,Haigang Hao,Jingjing Lu,Chengming Wu,Rui Gao,Jifan Li,Chun-Ling Liu,Wen-Sheng Dong
Here we exquisitely fabricated Cu/ZrO 2 -dp catalysts with plentiful Cu-ZrO 2 interfaces by depositing amorphous ZrO 2 onto Cu nanoparticles for the hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). With the created plentiful Cu-ZrO 2 interfaces, the optimal catalyst 3Cu/ZrO 2 -dp exhibited exceptional catalytic performance under mild reaction conditions, and achieved the highest GVL mass productivity of 266.0 mmol GVL·h −1 ·g −1 Cu, which was 12.5 and 2.3 times of Cu/ZrO 2 catalysts with equivalent Cu loadings prepared by traditional impregnation (3Cu/ZrO 2 -im) or co-precipitation (3Cu/ZrO 2 -cp). As far as we know, this GVL mass productivity stood at the highest level compared with those obtained using non-noble metal catalysts under similar reaction conditions. By systematic investigation with multiple characterizations, density functional theory (DFT) calculations, and kinetic studies, it was found that interfacial active centers were created at Cu-ZrO 2 interfaces, which contained oxygen vacancies (O v ), negatively charged Cu δ− and partially reduced Zr 3+ . The O v favored the adsorption and activation of LA via its ketone group, while negatively charged Cu δ− was able to enhance heterolysis of H 2 , which resulted in the formation of H + -Cu δ− and Zr 3+ -H − active species via hydrogen spillover. Also, plentiful acid sites, which derived from coordinatively unsaturated and defective Zr species, generated at Cu-ZrO 2 interfaces. With the cooperation of interfacial active centers (Cu δ− -O v -Zr 3+ ) and acid sites, the fabricated 3Cu/ZrO 2 -dp with plentiful Cu-ZrO 2 interfaces achieved excellent catalytic performance for the hydrogenation of LA to GVL. Hence, the synergistic catalysis of Cu-ZrO 2 interfaces provided an effective strategy for designing catalysts with a satisfactory performance for the hydrogenation of LA, which also can be expanded to other hydrodeoxygenation reactions.
研究领域:
催化
·
化学工程
·
材料科学
·
物理化学
✓ 已验证
DOI
高影响因子
Catalysts
·
2020
·Vol. 10
·期 9
·1096
·
IF 3.52
Ligang Luo,Xiao Han,Qin Zeng
A series of Ni-Fe/SBA-15 catalysts was prepared and tested for the catalytic hydrogenation of levulinic acid to γ-valerolactone, adopting methanol as the only hydrogen donor, and investigating the synergism between Fe and Ni, both supported on SBA-15, towards this reaction. The characterization of the synthesized catalysts was carried out by XRD (X-ray powder diffraction), TEM (transmission electron microscopy), H2-TPD (hydrogen temperature-programmed desorption), XPS (X-ray photoelectron spectroscopy), and in situ FT-IR (Fourier transform–infrared spectroscopy) techniques. H2-TPD and XPS results have shown that electron transfer occurs from Fe to Ni, which is helpful both for the activation of the C=O bond and for the dissociative activation of H2molecules, also in agreement with the results of the in situ FT-IR spectroscopy. The effect of temperature and reaction time on γ-valerolactone production was also investigated, identifying the best reaction conditions at 200 °C and 180 min, allowing for the complete conversion of levulinic acid and the complete selectivity to γ-valerolactone. Moreover, methanol was identified as an efficient hydrogen donor, if used in combination with the Ni-Fe/SBA-15 catalyst. The obtained results are promising, especially if compared with those obtained with the traditional and more expensive molecular hydrogen and noble-based catalysts.Keywords:biomass ester derivatives;solvothermal processing;levulinic acid;γ-valerolactone;Ni-Fe bimetallic catalysts
研究领域:
化学工程
·
催化反应
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2016
·
IF 4.179
Jian He,Hu Li,Yanxiu Liu,Wenfeng Zhao,Tingting Yang,Wei Xue,Song Yang
A series of mesoporous acid–base bifunctional Zr/B mixed oxides with different molar ratios were prepared by a sol–gel method, and developed for conversion of ethyl levulinate (EL) to γ -valerolactone (GVL) by using alcohol as hydrogen source. The morphological structures and physico-chemical characteristics of the synthesized materials were identified by various techniques. A high GVL yield of 88.5% was achieved from EL in 2-propanol when Zr 1 B 1 was used. And acid–base sites played a synergic role in synthesizing GVL from EL as evident by poisoning experiments. Furthermore, the catalyst could be reused several times without significant loss of its catalytic activity.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
Russian Journal of Physical Chemistry A
·
2020
·Vol. 93
·期 13
·2620-2627
·
IF 0.719
Yanyan Xu,Lu Tianliang,Bu Ningning,Luo Qianqian,Qing Yashi,Lin Li
Abstract Catalytic conversion of biomass based platform chemicals to value added chemicals has attracted much attention recently. In this work, Ni-based catalysts were developed for the conversion of levulinic acid to γ-valerolactone. By investigation of reduction behavior of NiO, it was found that a relatively low reduction temperature (300°C) can provide the reduction of NiO to Ni 0 . The high reduction temperature (500°C) generally applied in literature is not necessary. The effect of supports was also studied, and hierarchical AlPO 4 -5 (AlPO 4 -5-meso) supported Ni showed the best catalytic performance due to the proper pore size of AlPO 4 -5-meso, which contains both micropores and mesopores. The effect of Ni loading was also investigated, 10 wt % of Ni is enough for this reaction, which is lower than the reported amount of Ni loading. By using Ni/AlPO 4 -5-meso with 10 wt % Ni as catalyst, 84% γ-valerolactone yield and 100% levulinic acid conversion can be obtained after reaction for 10 h at 180°C.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL COMMUNICATIONS
·
2013
·Vol. 49
·期 46
·5328-5330
·
IF 6.378
Zhen Yang,Yao-Bing Huang,Qing-Xiang Guo,Yao Fu
A catalytic transfer hydrogenation process was developed for the production of γ-valerolactone (GVL) from ethyl levulinate (EL) and a H-donor at room temperature. Ethyl levulinate was almost quantitatively converted to γ-valerolactone. Further, a two step process for producing GVL from biomass derived platform molecules was also reported.
研究领域:
化学工程
·
可再生能源
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）