INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Guangyue Xu,Chuang Li,Tianyu Deng,Chenguang Wang,Ying Zhang,Yao Fu
The conversion of levulinic acid (LA) to γ-valerolactone (GVL) is one of the most important reactions from biomass-derived platform chemicals to value-added chemicals. In this work, bimetallic PdRu/TiO2 catalyst compared to monometallic Ru/TiO2 was designed for the conversion of LA to GVL at ambient H2 pressure. The highly dispersed Pd affected the reaction by two antagonistic effects: (I) increasing the reaction rate by promoting the activation of H2; (II) decreasing the reaction rate by lowering the activation ability of carbonyl group over Ru. The kinetic analysis refined by H2 concentration showed much lower apparent activation energy over 0.2Pd1Ru/TiO2 than that over Ru/TiO2. Finally, the catalysts were evaluated by both GVL productivity and catalyst cost to show increasing benefit of Pd addition at lower H2 pressure. This study offers both theoretical foundation and application instructions for high efficiency conversion of LA to GVL under mild conditions, especially ambient H2 pressure.
研究领域:
催化化学
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生物质能
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Shuolin Zhou,Xianxiang Liu,Jinhua Lai,Min Zheng,WenZhu Liu,Qiong Xu,Dulin Yin
A novel inorganic-organic hybrid nanocatalyst has been prepared by initially functionalizing titanate nanotubes with 3-amino-propyltrimethoxysilane and subsequently introducing sulfonic acid groups with 1,4-butane-sultone. The as-prepared hybrid catalyst was characterized by FT-IR, XRD, TEM, SEM-EDX, TG-DTG, and N 2 adsorption isotherm techniques, and its catalytic performance was evaluated by esterification of levulinic acid with n -butyl alcohol under solvent-free conditions. The experimental design and study were carried out by response surface methodology (RSM) to test the effects of reaction conditions on the catalytic process. Up to 82.7% yield of n -butyl levulinate was obtained under the optimal reaction conditions. Furthermore, the catalyst showed an excellent reusability without the loss of reactivity after several runs.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2019
·
IF 4.191
Xiaoyun Li,Rui Xu,Qingling Liu,Min Liang,Jiaxin Yang,Shuangchun Lu,Guangbi Li,Lefu Lu,Chuanling Si
A one-step process was proposed for valorization of corn stover into furfural and levulinic acid catalyzed by SAPO-18 zeolites. With the aim to produce furfural and levulinic acid, the Brønsted to Lewis acid site ratios of SAPO-18 were modified. The influence of reaction temperature, time and the ratios of Brønsted to Lewis acid site on the valorization of corn stover were investigated. At the fixed catalyst concentration of 20 g/L, a furfural yield of 95.1% was observed at 205 °C for 40 min using SAPO-18 with Brønsted to Lewis acid site ratio of 0.11, and a levulinic acid yield of 70.2% achieved at 190 °C for 80 min using SAPO-18 with Brønsted to Lewis acid site ratio of 0.17. The Brønsted to Lewis acid site ratios of SAPO-18 were adjusted by altering the framework Si/Al ratio of SAPO-18. The SAPO-18 with lower Brønsted to Lewis acid site ratios showed higher activity for furfural production from corn stover and that with higher ratios exhibit superior catalytic effect for levulinic acid formation. The kinetic models considering the effect of Brønsted to Lewis acid site ratios agreed with the experiment values well, which provided detailed insights on the conversion of hemicellulose and cellulose fraction of corn stover into furfural and levulinic acid.
研究领域:
化学工程
·
生物质能
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2019
·
IF 5.162
Shuqi Fang,Zhibing Cui,Yuting Zhu,Chenguang Wang,Jing Bai,Xinghua Zhang,Ying Xu,Qiying Liu,Lungang Chen,Qi Zhang,Longlong Ma
Herein, we reported in situ synthesis of biomass-derived Ni/C catalyst by self-reduction with pomelo peel. Compared with the conventional method, which includes carbonization , activation, impregnation and reduction, the entire preparation process was simplified to two steps, which was more straightforward. This synthesis method was green as Ni/C can be prepared without any additional chemical and the self-reduction process was realized in N 2 , which can avoid using H 2 thus averting some problems such as storage, transportation and safety of H 2 . Meanwhile, the size and dispersion of Ni particles can be controlled by changing carbonization temperature. The synthesis mechanism of Ni/C catalyst with self-reduction was investigated, which was mainly attributed to the carbon and reducing gas produced during the carbonization process. For the catalytic performance of GVL synthesis, a high yield (94.5%) can be obtained and it exhibited good stability up to 5 cycles without obvious loss of catalytic activity .
研究领域:
催化
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绿色化学
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材料科学
·
生物质转化
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 13
·6258-6265
·
IF 3.3
Guojun Lan,Zhenqing Li,Xiaojia Han,Liping Zhang,Yiyang Qiu,Xiucheng Sun,Zaizhe Cheng,Ying Li
The electron cloud density of the ruthenium nanoparticles plays a key role in catalyzing the hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). Herein, the effects of interactions between the carbon support and ruthenium nanoparticles (Ru NPs) were systematically investigated by tailoring the surface of nanodiamonds (NDs). The binding energy of the Ru NPs increases first then decreases along with the increasing of the annealing temperature during the preparation of the carbon supports. The nanodiamonds annealed at 900 °C transferred more electrons to Ru NPs, which increased the electron density of the Ru NPs in the Ru/ND-900 catalyst. The Ru/ND-900 catalyst with high electron density exhibits an efficient activity for the hydrogenation of levulinic acid. Moreover, the Ru/ND-900 catalyst also exhibits much more stability than the Ru/ND catalyst for the hydrogenation of LA in the aqueous phase.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 21
·10455-10462
·
IF 3.3
Mengting Chen,Qifeng Zhong,Jiao Ma,Zhiyang Zhang,Yingxin Liu,Zuojun Wei,Shuguang Deng
Hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is a key reaction in the conversion of biomass to renewable fuels and value-added chemicals. Developing low-cost, highly efficient and reusable non-noble metal-based heterogeneous catalysts is vital but challenging. Herein, non-noble Ni–Mn/SiO2 catalysts with a low Ni loading (2.0 wt%) were designed for the selective hydrogenation of LA to GVL. The results showed that the optimal Ni–Mn/SiO2 (Ni/Mn = 2) catalyst with well-dispersed and small-sized metal nanoparticles (2.21 nm) and moderate acid sites exhibited excellent activity and selectivity and achieved a 100% yield of GVL in a 1,4-dioxane solvent under mild reaction conditions (e.g., 0.8 mol% Ni, 140 °C and 2.0 MPa H2) for 5.5 h and a 100% GVL yield at 180 °C for 2 h with a turnover frequency (TOF) of 190.2 h−1, which is better than most non-noble metal catalysts reported. Furthermore, the catalyst exhibited excellent reusability and could be recycled at least five times with only slight activity loss. This work provides new insights for the rational design of highly efficient and stable non-noble metal catalysts for the conversion of LA to GVL.
研究领域:
催化化学
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可再生能源
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2023
·
IF 11.4
Xiaofen Xu,Beiling Liang,Ying Zhu,Jiashuo Chen,Tao Gan,Huayu Hu,Yanjuan Zhang,Zuqiang Huang,Yuben Qin
This study aimed to produce bio-based levulinic acid (LA) via direct and efficient conversion of cellulose catalyzed by a sustainable solid acid. A carbon foam (CF)-supported aluminotungstic acid (HAlW/CF) catalyst with Brønsted–Lewis dual-acidic sites was creatively engineered by a hydrothermal impregnation method. The activity of the HAlW/CF catalyst was determined via the hydrolysis and conversion of cellulose to prepare LA in aqueous system. The cooperative effect of Brønsted and Lewis acids in HAlW/CF resulted in high cellulose conversion (89.4%) and LA yield (60.9%) at 180 °C for 4 h, which were greater than the combined catalytic efficiencies of single HAlW and CF under the same conditions. The HAlW/CF catalyst in block form exhibited superior catalytic activity, facile separation from reaction system, and favorable reusability. This work offers novel perspectives for the development of recyclable dual-acidic catalysts to achieve one-pot catalytic conversion of biomass to value-added chemicals.
研究领域:
化学工程
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催化
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生物质转化
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绿色化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Xiaohao Liu,Dali Han,Jinming Xia,Dongxu Yan,Rui Diao,Fenglei Qi,Zhenyu Wang,Lei Yang,Xiang Wu,Peiyong Ma,Ying Zhang
Nanopore-confining strategy is an effective way to inhibit catalyst sintering and improve catalytic performance. However, the expensive material precursors and complex preparation process greatly limit the scale utilization of this particularly structured catalyst. Herein, nanopore-confined catalysts (Ni@PAC) with adjustable active species were successfully prepared by a very simple method exploiting the characteristics of phosphoric acid-activated biochar (PAC). The abundant phosphorous functional groups in PAC confined Ni well in pores and significantly inhibited sintering through the spatial-confined effect of nanopore. Moreover, the evolution and migration of P functional groups can be regulated by changing the reduction temperature, and the modulation of active species of Ni metal or nickel phosphide can be achieved. Using biomass-based levulinic acid hydrogenation as the probe reaction, it was found that the catalytic activity of 20Ni@PAC-600 was one order of magnitude higher than that of the non-phosphated 20Ni/ZAC-600 catalyst, and γ-valerolactone could be selectively prepared at near atmospheric pressure (1 bar). The formation of Ni2P and the spatial-confined effect of nanopore could be the main reasons for the high catalytic activity.
研究领域:
催化化学
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生物质转化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Weimeng Cai,Haojie Du,Erju Wang,Yuting Qiang,Kunhong Hu,Jianhua Guo
The synthesis of value-added chemicals from renewable biomass is becoming increasingly important in the transition to a sustainable and low-carbon energy system. Herein, we demonstrate a solvent-polarity modulation strategy to engineer biomass-derived Cu-MOF using 2,5-furandicarboxylic acid (FDCA) as a renewable ligand, where tailored β/α ratios via Kamlet-Taft parameters balance nucleation-growth kinetics to optimize textural properties. Pyrolyzed Cu-MOF at 500 °C under a nitrogen atmosphere yield the Cu/C catalysts, which were subsequently employed in the selective hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). Among the various solvents used, the Cu-MOF precursor synthesized in a mixed solvent of methanol and N, N-dimethylformamide (DMF) demonstrated the highest catalytic performance, outperforming those synthesized in other solvents. This highlights the significant impact of solvent selection on the structure of Cu-MOF, which in turn affects their hydrogenation activity. Advanced characterization confirming that the uniform Cu dispersion (confirmed by HRTEM mapping) and Cu⁰/Cu⁺ electronic synergy (via Cu Auger analysis) enhanced hydrogenation performance. Additionally, the biomass-derived catalysts exhibited excellent durability. Overall, this research provides a promising approach to develop highly efficient catalysts using renewable ligands and demonstrates the potential of regulating catalyst properties through the strategic selection of solvents, as informed by Kamlet-Taft parameters.
研究领域:
催化化学
·
绿色化学
·
材料科学
·
可再生能源
·
化学合成
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Fengyi Zhou,Yurun Tian,Hongyuan Zhang,Yijun Yin,Zeyu Wang,Rui Qin,Yu Chen,Zhiyong Li,Tiancheng Mu
The rapid growth of spent lithium-ion batteries (LIBs) raises concerns over the supply chain of critical metals and environmental impacts, emphasizing the urgent need for efficient recycling technologies. Due to their potential to reduce the consumption of energy and avoid the use of corrosive acid, deep eutectic solvents (DESs) have been widely studied to selectively leach and recover valuable metals from spent LIBs. There is general agreement that DESs with high acidity, coordination, reducibility, and low viscosity could efficiently dissolve cathode materials. However, it is hard to design binary DES compositions to fulfill all of these requirements simultaneously. Herein, this study focuses on the design of ternary DESs, leveraging the synergistic effects of their components to achieve strong coordination and low viscosity, enhanced acidity, and reducibility to efficiently extract valuable metals. Specifically, ChCl/CuCl:4Levulinic acid demonstrated exceptional leaching capabilities, recovering over 90% of LiCoO2 within 10 min. Furthermore, to ensure the purity of recovered metal products, ChCl/LiCl:8Levulinic acid was investigated to realize the efficient leaching, recovery, and DES regeneration process. It was verified that ChCl/LiCl/8Levulinic acid has high leaching efficiency and good cycling stability and facilitates a convenient recycling process. Overall, this work demonstrates the potential of tailored ternary DESs for the efficient leaching of cathode materials and proposes a sustainable process to realize metal recovery from spent LIB cathode and DES regeneration.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2020
·Vol. 95
·期 9
·2537-2548
·
IF 2.75
Liquan Zhang,Can Wang,Hairong Zhang,Haijun Guo,Lian Xiong,Hailong Li,Xuefang Chen,Xinde Chen
BACKGROUND Levulinic acid (LA) and furfural are important biomass-based platform compounds. During the preparation of LA and furfural from lignocellulosic biomass, other organic chemicals including sugars, formic acid, acetic acid, and acid-soluble lignin (ASL) will be produced simultaneously. Thus, the purification of LA and furfural is an important process. In this work, a series of glycidyl methacrylate (GMA) modified hyper-cross-linked resins were synthesized and the mechanism of pore formation of the resins was studied. Furthermore, the effect of their textural properties on adsorption performance towards LA and furfural was investigated. RESULTS The hyper-cross-linked resin modified with 50 wt% GMA (PC-4) achieved the best adsorption performance. The adsorption capacities of LA and furfural onto PC-4 were 100.81 and 40.22 mg g −1 , respectively, which were 2423.76% and 249.24% higher than the un-modified resin HQ-8, and 31.0% and 22.7% higher than its precursor PR-4. During desorption process, the average desorption ratio of LA and furfural were 94.96% and 97.86%, respectively. Moreover, PC-4 also showed a good adsorption performance towards formic acid, acetic acid, and ASL, while sugar loss rate was about 5%. CONCLUSION This study not only reported a potential adsorbent, PC-4, for the comprehensive utilization of sugarcane bagasse hydrolysate, but it also studied the relationship between synthesis conditions, resin structures, and its adsorption performance of GMA modified hyper-cross-linked resins, which provides a guidance for new adsorbent design. © 2020 Society of Chemical Industry
研究领域:
化学工程
·
材料科学
·
生物质利用
·
环境科学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2020
·
IF 3.687
Yaowei Lu,Yongxing Wang,Yinghao Wang,Qiue Cao,Xiaoguang Xie,Wenhao Fang
A bifunctional Ru/(AlO)(ZrO) n catalyst was reported for efficient hydrogenation of levulinic acid to γ-valerolactone, an important and environmental-benign upgrading process of bio-platform compound. The optimal Ru/(AlO)(ZrO) 0.1 catalyst showed 100% yield to γ-valerolactone in water at 120 °C under 1 MPa H 2 , one of the best performances among Ru catalysts under mild conditions. And this catalyst also presented good stability and reusability. PXRD, TEM, XPS, CO chemisorption, CO adsorption DRIFT-IR, NH 3 -TPD and pyridine adsorption IR gave insights into the acidic property and surface synergy of the catalysts. Highly active electron-rich Ru 0 sites stabilized by strong metal-support interaction (SMSI) can effectively adsorb and activate molecular H 2 and C O bond in levulinic acid. Varying Zr/Al ratio and calcination temperature can rationally control the acid strength and acid sites distribution of support, and (AlO)(ZrO) 0.1 calcined at 400 °C exhibited the maximal proportion of Lewis acid sites. Ru 0 species and Lewis acid sites synergistically enhanced the conversion of levulinic acid and facilitated the intramolecular dehydration of 4-hydroxypentanoic acid as intermediate to γ-valerolactone ( i.e. , the rate-limiting step).
研究领域:
催化化学
·
绿色化学
·
材料科学
✓ 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）