Catalysts
·
2025
·Vol. 15
·期 5
·416
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IF 4
Jie Qin,Guohong Chen,Kaiqi Zheng,Jiajun Wu,Fanan Wang,Xueping Liu,Rengui Weng
2-Methyltetrahydrofuran (2-MTHF), a hydrogenated derivative of levulinic acid (LA), is a biomass-derived platform compound with diverse and significant applications as a biofuel, gasoline additive, green solvent, and pharmaceutical synthesis intermediate. This study investigates the preparation of a Cu1Ni2/Al2O3catalyst through the calcination–reduction of CuNiAl hydrotalcite as a precursor, which was subsequently utilized in the hydrogenation of LA to produce 2-MTHF. The calcination–reduction process applied to CuNiAl hydrotalcite results in a lattice confinement effect. This method not only disperses the active metal sites but also alters the bonding patterns of the active metals, thereby enhancing the activity and stability of the Cu1Ni2/Al2O3catalyst. The results indicate that complete conversion of LA and a 2-MTHF yield of 87.6% can be achieved under optimal conditions of 190 °C, 5 MPa hydrogen, and a reaction time of 5 h, demonstrating an efficient one-step conversion process. Additionally, the catalyst’s recyclability was assessed through multiple reuse tests, with a loss of activity of only 9.2% after six cycle experiments, suggesting its feasibility and reliability for industrial applications.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 13
·6258-6265
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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.
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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.
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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.
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PubMed
高影响因子
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.
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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.
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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 .
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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.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ying Zhu,Furui Hu,Zi Yu,Yongxin Liang,Tao Gan,Huayu Hu,Zuqiang Huang,Yanjuan Zhang
The activation of reaction system for high-efficiency hydrogenation of levulinic acid (LA) into γ-valerolactone (GVL) is significant for sustainable development of biomass. Herein, based on a strategy of tourmaline (TM)-activated aqueous-phase system, a Cu-Ni/ZrO 2 @TM/C catalyst was facilely constructed by a totally solid-phase method. Cu-Ni/ZrO 2 @TM/C exhibited outstanding catalytic performance, benefiting from the spontaneous polarization and far-infrared radiation characteristics of tourmaline and the strong metal–metal and metal–support interactions. Under the optimum reaction conditions of 180 °C, 150 min, and 1.5 MPa H 2 , 100.0 % of LA conversion and 93.0 % of GVL yield were achieved. A variety of tests and theoretical calculations confirm that tourmaline with spontaneously polarized electric field and far-infrared radiation can break intermolecular hydrogen bonds to form small water clusters for activating aqueous-phase environment, facilitating the transport of active species as well as greatly reducing the hydrogenation barrier. The activating water effect of tourmaline, the acid sites and oxygen vacancies of ZrO 2 , and the alloying structure of Cu-Ni bimetal can synergistically benefit the transport of active species for reinforcing water-assisted proton hopping. Moreover, a reasonable tourmaline-activated aqueous-phase system was proposed to explain the enhanced aqueous hydrogenation of LA. This study innovatively illuminates the construction of functional non-precious metal catalysts for efficient aqueous-phase hydrogenation of biomass-derived chemicals.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Rulu Huang,Yue Wang,Feiyi Chen,Huai Liu,Rui Zhang,Wenlong Jia,Lincai Peng,Yong Sun,Junhua Zhang
The sluggish kinetic of the hydrogen transfer reaction pose a significant challenge in developing efficient catalytic transfer hydrogenation (CTH) system for upgrading biomass-derived platform molecules. In this contribution, for the first time, hafnium (Hf) species have been found to coordinate with the hydroxyl groups on halloysite nanotubes surface to construct a single-atom Hf catalyst (Hf@HNTs) with unsaturated-coordinated structure at room temperature. Especially, the Hf(1.7)@HNTs delivered an impressive catalytic performance for the CTH of levulinic acid (LvA) to gamma-valerolactone (GVL) with high turn-over frequency (TOF) of 43.1 h −1 at 160 °C, considerably exceeding that of coordination-saturated HfO 2 and state-of-art Hf-based catalysts. Experimental and density functional theory (DFT) studies revealed that Hf(1.7)@HNTs possessed unsaturated-coordinated and atomically-dispersed Hf-O Lewis acid-base pairs, which favored the adsorption and activation of LvA. Moreover, DFT calculations explicitly demonstrated that the energy barriers for the hydrogen transfer between the LvA and hydrogen donor were significantly reduced on the Hf(1.7)@HNTs than that of HfO 2 .
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高影响因子
CHEMICAL PHYSICS
·
2024
·
IF 2
Ronghua Zhang,Shikun He,Fei Wang,Bo Cai,Junfeng Feng,Hui Pan
Porous bi-functional catalsyts consisting of metals and zeolites are used as solid acid catalysts, characterized by octahedral morphology and good stability. In this work, a series of bifunctional catalysts (xZr-HY) with Lewis and Brønsted acid sites were prepared by a simple impregnation method, and used for the conversion of glucose to levulinic acid and methyl levulinate. The catalysts were characterized using different methods of physical and chemical properties. The analysis results showed that these catalysts existed in tetrahedral form with good pore structure , suitable acid strength and acidity. Using 10Zr-HY as the catalyst, 43.0 % yield of LA and ML could be obtained at 200 ℃ for 2.5 h. In addition, this catalytic system also gave high LA and ML yields from other biomass carbohydrates. Meanwhile, the 10Zr-HY catalyst had good stability and reusability after four cycles. This catalyst has the potential to convert biomass into high value-added platform compounds.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Mengli Zhou,Sichan Li,Haojie Tian,Xinyu Liu,Zhimin Wu,Qiying Liu,Jianchun Jiang
Levlinic acid (LA) and its derived γ-valerolactone (GVL) are the two important biomass derived platform molecules, which showed wide application in the fields of fine chemicals, drug and liquid fuel industrials. Considering the coupling of sequential steps for glucose to LA and GVL, selective production of LA and GVL via glucose one-pot conversion in water is an open challenge. Herein, we used metal chlorides as the acidic catalyst for glucose conversion to LA, obtaining the high yield of 77.8 C-mol% over SnCl 4 . Moreover, using the SnCl 4 and Ru/C as the combined catalyst, glucose or cellulose could be converted to GVL with the high yield of 60.1 or 57.9 C-mol% in the case of in situ hydrogenation by formic acid (the by-products during LA formation) decomposition. The formation of LA was responsible for the cooperative effect of BAS (Bronsted acid sites) and LAS (Lewis acid sites) of SnCl 4 for accelerating glucose isomerization, fructose dehydration followed by 5-hydroxymethyl furfural (HMF) rehydration, while the GVL production is relative to the highly efficient formic acid decomposition to H 2 followed by LA hydrogenation to GVL over Ru/C. This study provided an avenue for facile and highly efficient conversion of biomass and the derivatives to LA and GVL using commercial catalysts.
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高影响因子
危险品化学品经营许可证（带存储）