INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
·
IF 7.139
Yunfei Zhang,Yi Shen
Converting levulinic acid (LA) to fuel precursors such as gama-valerolactone (GVL) and valeric acid (VA) via an efficient and low-cost method is of great significance. Herein, a series of free-standing electrodes consisting of metallic metals supported by carbon felts (CFs) were fabricated via a facile electro-deposition process. The resulting M/CFs (M = Pb, Cd, Co, Ni, Cu and Bi) electrodes were evaluated for electrocatalytic hydrogenation (ECH) of LA. The electrocatalytic activity of the electrodes was extensively studied by various electrochemical methods including cyclic voltammetry , linear sweep voltammetry and chronoamperometry measurements. The products of the ECH processes were analyzed by gas chromatography-mass spectrometry. Of all the prepared samples, the Pb/CFs and Cd/CFs electrodes showed superior performance for ECH of LA. The selectivity of VA reached up to 91.7% when the Pb/CFs was used and the conversion of LA reached to 57.2% using the Cd/CFs electrode, rendering them as one of the best electrodes for ECH reported in the literature. The effects of applied potentials on the ECH process were investigated. To further optimize the ECH performance of the Pb/CFs electrodes, several key parameters including deposition time , pH value of the electrolyte and reaction time were studied. When the electrodeposition time was 600 s and the concentration of sulfuric acid in the electrolyte was 0.5 M, the complete transformation of 0.2 M of LA was achieved after 6 h. This study may afford an alternative way to the conversion of LA to GVL or VA.
研究领域:
化学工程
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电化学
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催化材料
✓ 已验证
DOI
高影响因子
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
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催化科学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2021
·
IF 3.171
Lihua Qian,Guojun Lan,Xiaoyan Liu,Zhenqing Li,Ying Li
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) by using water as solvent is a crucial process in the production of fine chemicals from biomass. An ultrathin carbon layer coating CoRu bimetallic catalyst supported on silica (CoRu@C/SiO 2 ) is prepared by using tannis-ligated cobalt-ruthenium complex on silica as precursors, and applied for catalyzed synthesis of GVL from LA. Because of the synergistic effect between cobalt and ruthenium, the addition of small amounts of Ru to Co catalysts can increase the catalytic activity in the aqueous hydrogenation of LA. The ultrathin carbon layer covered on the CoRu bimetallic catalyst can greatly reduce the leaching of active metals. The CoRu@C/SiO 2 catalyst achieves high stability and is reused up to 5 runs without significant loss of performance in aqueous hydrogenation of levulinic acid.
研究领域:
催化化学
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生物质能
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材料科学
✓ 已验证
DOI
高影响因子
CARBOHYDRATE RESEARCH
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2022
·
IF 2.975
Huifang Ren,Xiao-Yang Yue,Wen-Sheng Dong
We propose a new approach for the synergistically catalytic conversion of cellulose to levulinic acid (LA) in water by SO 3 H-functionalized ionic liquid (SFIL) and lanthanide chloride (LnCl 3 ). Compared with using 1-methyl-3-(3-sulfopropyl)imidazolium chloride ([MIMPS]Cl) only, the LA yield using [MIMPS]Cl and ErCl 3 increased by 14.4% and 13.6% at 50 mol% of IL and 30 mol% of IL, respectively. Moreover, the combined [MIMPS]Cl and ErCl 3 system can tolerate high concentrations of substrates and maintain high activity at eleven runs. We also investigated the effects of the cation structure of ionic liquids (alkyl chain length, hydroxyl groups on the side chains, and aromatic properties) on LA production. The observations can provide useful information for designing efficient ionic liquid catalysts for biomass utilization.
研究领域:
化学工程
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生物质能
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
NANOTECHNOLOGY
·
2022
·Vol. 33
·期 35
·355401
·
IF 3.953
Qianqian Ding,Yuan Wang,Liang Ma
Transforming levulinic acid (LA) to γ-valerolactone (GVL) is a significant route for converting biomass into valuable chemicals. The development of an efficient and robust heterogeneous catalyst for this reaction has aroused great interest. In this work, nitrogen-doped graphene (NG) supported nickel (Ni) based heterogeneous catalyst with excellent activities was successfully synthesized. The Ni/NG catalyst shows outstanding performance for hydrogenation of LA to GVL at a relatively low temperature of 140 °C, which is superior to most of reported heterogeneous catalysts. Further investigations indicate Ni nanoparticles are the active sites and the NG also plays an indispensable role. The catalytic performance is highly depended on the crystallinity, particles sizes and electronic structure of Ni in Ni/NG catalyst, which can be optimized by nitrogen doping. This work affords a new route for designing robust and excellent heterogeneous catalysts by doping method to optimize the support.
研究领域:
化学工程
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材料科学
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可再生能源
✓ 已验证
DOI
高影响因子
RSC Advances
·
2021
·Vol. 12
·期 1
·602-610
·
IF 3.361
Yingxin Liu,Kai Liu,Meihua Zhang,Kaiyue Zhang,Jiao Ma,Shuwen Xiao,Zuojun Wei,Shuguang Deng
Highly active and thermally stable Cu–Re bimetallic catalysts supported on TiO2 with 2.0 wt% loading of Cu were prepared via an incipient wetness impregnation method and were applied for liquid phase selective hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) in H2. The effect of the molar ratios of Cu : Re on the physico-chemical properties and the catalytic performance of the Cu–Re/TiO2 catalysts was investigated. Moreover, the influence of various reaction parameters on the hydrogenation of LA to GVL was studied. The results showed that the Cu–Re/TiO2 catalyst with a 1 : 1 molar ratio of Cu to Re (Cu–Re(1 : 1)/TiO2) exhibited the highest performance for the reaction. Complete conversion of LA with a 100% yield of GVL was achieved in 1,4-dioxane solvent under the reaction conditions of 180 °C, 4.0 MPa H2 for 4 h, and the catalyst could be reused at least 6 times with only a slight loss of activity. Combined with the characterization results, the high performance of the catalyst was mainly attributed to the well-dispersed Cu–Re nanoparticles with a very fine average size (ca. 0.69 nm) and the co-presence of Cu–Re bimetal and ReOx on the catalyst surface.
研究领域:
催化化学
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可再生能源
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemCatChem
·
2022
·Vol. 14
·期 13
·e202200311
·
IF 5.497
Yuyao Zeng,Bowei Wang,Fanyong Yan,Wensheng Xu,Guoyi Bai,Yang Li,Xilong Yan,Ligong Chen
Graphical Through a convenient impregnation method, highly-distributed and stable Cu nanoparticles were dispersed on the boron doped γ-Al 2 O 3 support, which catalyzed continuous reductive amination of levulinic acid to corresponding N-substituted pyrrolidinones. The reductive amination of biomass-derived levulinic acid (LA) to value-added N-substituted pyrrolidinones with amine and molecular hydrogen over heterogeneous catalyst represents an atom-economical and scalable route. In this paper, a series of boron doped Cu/Al 2 O 3 catalysts via kneading and impregnation method are developed for the continuous reductive amination of LA. Compared with Cu/Al 2 O 3 , Cu 10 /AlB 3 O catalyst exhibits greatly improved catalytic performance for this reaction at low operation temperature. Structure-property correlation investigations were performed with diverse characterization methods, and the results revealed that the excellent catalytic performance of boron doped Cu/Al 2 O 3 catalysts was mainly attributed to the synergistic effect of its well-dispersed Cu nanoparticles, appropriate surface Cu electronic state and surface acidic sites nearby. Besides, Cu 10 /AlB 3 O shows great stability during the reaction over 200 h. This work provides a low-cost, efficient and environmentally friendly heterogeneous catalytic system for the continuous production of N-substituted pyrrolidinones.
研究领域:
催化化学
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绿色化学
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生物质转化
✓ 已验证
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2020
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IF 4.244
Jing Gu,Jun Zhang,Yazhuo Wang,Denian Li,Hongyu Huang,Haoran Yuan,Yong Chen
A series of magnetic zirconium nanoparticles with varied Zr/Fe molar ratios were synthesized and developed as acid−base bifunctional catalysts in the catalytic transfer hydrogenation (CTH) of biomass-derived furfural (FFR) and levulinic acid (LA) using 2-propanol as both hydrogen donor and solvent. Zirconium constituents coated on nano-sized Fe 3 O 4 endowed the catalysts with abundant acid−base sites, moderate surface areas (94.0‒187.6 m 2 /g) and pore sizes (3.42–9.51 nm), thus giving nearly 100 % yields of furfuryl alcohol (FA) and γ-valerolactone (GVL) after 2 h of reaction. Particularly, competitive activation energy (E a ) for the CTH of FFR into FA over Zr 1 Fe 1 -300 was as low as 50.9 kJ/mol. Moreover, the easily separable nanocatalyst Zr 1 Fe 1 -150 was also applicable to CTH of various alkyl levulinates into GVL in high efficiency and could be reused for multiple cycles without obvious loss of its catalytic performance in the transfer hydrogenation of LA.
研究领域:
化学工程
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生物质能源
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Lungang Chen,Yong Liu,Canshuo Gu,Gang Feng,Xinghua Zhang,Jianguo Liu,Qi Zhang,Chenguang Wang,Longlong Ma
Selective production of 2-butanol from levulinic acid (LA) hydrogenolysis over a non-precious catalyst is long desirable. However, the process requires the precious metal Ru, and the yield of 2-butanol was less than 65%. Herein, we prepared Ni-based bimetallic catalysts, among which the NiMn catalyst exhibited the highest efficiency and reached an 84.5% yield of 2-butanol at 100% LA conversion under optimal conditions. The electronic states and surface properties were characterized by various techniques such as X-ray diffraction, X-ray photoelectron spectroscopy, temperature-programmed desorption, temperature-programmed reduction, and scanning electron microscopy/transmission electron microscopy. The high efficiency of the NiMn catalyst was due to the synergy between Ni0 and Mn2+ species, and the modified surface showed a high basicity and a high affinity to adsorb LA and LA-derived molecules with C═O or COOH. The high affinity of the NiMn catalyst was further confirmed by density functional theory calculations.
研究领域:
催化化学
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可再生能源
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2016
·Vol. 18
·期 11
·3370-3377
·
IF 8.506
Wenjing Yang,Haiyang Cheng,Bin Zhang,Yan Li,Tong Liu,Mingli Lan,Yancun Yu,Chao Zhang,Weiwei Lin,Shin-ichiro Fujita,Masahiko Arai,Fengyu Zhao
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) was studied with a homogeneous RuCl2(PPh3)3 catalyst in supercritical CO2 (scCO2). The conversion of LA was observed to increase with CO2 pressure and the possible reasons for this rate acceleration were discussed, including the molecular interactions of CO2 with the reacting and catalytic species as well as the acidity and phase behavior of the reaction mixture. The interaction between CO2 and RuCl2(PPh3)3 was significant, which resulted in the production of an active RuHCl(CO)(PPh3)3 complex and thus enhanced the rate of hydrogenation in the presence of CO2.
研究领域:
化学工程
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Bioresources and Bioprocessing
·
2022
·Vol. 9
·期 1
·1-10
·
IF 4.983
Zhai Siyu,Zhang Lihe,Zhao Xi,Wang Qian,Yan Yin,Li Cui,Zhang Xu
The current energy crisis has prompted the development and utilization of renewable energy and energy storage material. In this study, levulinic acid (LA) and 1,4-butanediol (BDO) were used to synthesize a novel levulinic acid 1,4-butanediol ester (LBE) by both enzymatic and chemical methods. The enzymatic method exhibited excellent performance during the synthesis process, and resulted in 87.33% of LBE yield, while the chemical method caused more by-products and higher energy consumption. What’s more, the thermal properties of the obtained LBE as a phase change material (PCM) were evaluated. Differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) showed that the melting temperature, latent heat of melting, and pyrolysis temperature were 50.51 °C, 156.1 J/g, and 150–160 °C, respectively. Compared with the traditional paraffin, the prepared PCM has a superior phase transition temperature, a higher latent heat of melting, and better thermal stability. The thermal conductivity could be increased to 0.34 W/m/k after adding expanded graphite (EG). In summary, LBE has great potential in the application of energy storage as a low-temperature phase change energy storage material. Graphical Abstract
研究领域:
能源材料
·
生物化学
·
可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Sustainable Energy & Fuels
·
2023
·Vol. 7
·期 11
·2645-2652
·
IF 5.6
Rulu Huang,Yuan Cheng,Huai Liu,Lincai Peng,Junhua Zhang
It is incredibly challenging to design a catalyst with high activity for catalytic transfer hydrogenation (CTH) of levulinic acid (LvA) into gamma-valerolactone (GVL). In our previous work, we have designed a mesoporous acid-base bifunctional hybrid (Zr-FDCA) with high contents of Lewis acid (LA) and Lewis base (LB) sites from zirconium and 2,5-furandicarboxylic acid (FDCA) by using acetic acid as the modulator, which exhibited an outstanding performance in CTH of furfural into furfuryl alcohol. However, the catalytic performance was not satisfactory in CTH of LvA into GVL. Herein, we modified a Zr-FDCA hybrid with the introduction of phosphotungstic acid (HPWO). Comprehensive characterization revealed that HPWO could significantly affect the acidity, which afforded acid catalytic activity and introduced a Brønsted acid (BA) site. The synergistic effect between LA and BA sites resulted in the outstanding catalytic activity in CTH of LvA into GVL; a GVL yield of 95.4% with a high formation rate of GVL (12.72 mmol g−1 h−1) was obtained over Zr-FDCA-HPWO. Simultaneously, it also showed an ideal cycle stability and could be used for at least five consecutive runs with no significant loss in the catalytic activity.
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
危险品化学品经营许可证（带存储）