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
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绿色化学
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材料科学
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产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2020
·Vol. 4
·期 4
·2018-2025
·
IF 5.503
Songyan Jia,Jiao Ma,Dongping Wang,Kangjun Wang,Qiang Zheng,Chunshan Song,Xinwen Guo
Levulinic acid (LA) is a promising renewable platform compound derived from biomass for the manufacture of various valuable chemicals, among which levulinate esters have been demonstrated to be good fuel additives. Many previous studies have focused on the production of short-chain levulinates for biofuels such as methyl and ethyl levulinates, but these esters suffer from some essential issues including a high oxygen content, low energy density (or heating value) and water solubility. Long-chain levulinate esters have similar structures to biodiesel. The long carbon chain may provide a higher carbon content and strong hydrophobicity, therefore improving the energy density and water insolubility. In this work, the synthesis of a long-chain levulinate ester, n-hexyl levulinate (HL), has been fast and efficiently achieved by the catalytic esterification of LA and 1-hexanol at low temperature. Tungsten hexachloride (WCl6) showed the most superior activity among the tested metal salt catalysts under mild conditions. A HL yield of ∼85% with almost complete LA conversion could be obtained at 50 °C after only 30 min. Other hexanols that have larger steric hindrances, such as 2-ethyl-1-butanol, 2-hexanol, 3-hexanol and cyclohexanol, could also promote efficient esterification with LA over the WCl6 catalyst, resulting in excellent product yields of ∼82–91%. The strategy applies to the efficient synthesis of longer chain levulinate esters such as n-octyl levulinate (OL) as well. The WCl6 catalyst was reusable several times in a consecutive batch reaction mode. The method reported herein offers a strategy for the efficient production of liquid fuels from LA, potentially bridging raw biomass feedstocks and terminal utilization of biobased products.
研究领域:
化学工程
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可再生资源利用
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产品关联
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2022
·Vol. 36
·期 5
·e6646
·
IF 4.072
Yanyun Wang,Yuming Zhou,Jiehua Bao,Jiajia Wang,Yiwei Zhang,Xiaoli Sheng,Yuzhong Huang
Pt nanocatalysts have received enthusiastic attention in the field of clean energy technologies due to their high catalytic activity and selectivity. The growth size and dispersion of Pt particles play significant effects on the reaction activity, especially in high temperature catalytic reactions where catalysts are prone to deactivation due to agglomeration and sintering of Pt particles. Herein, the Pt nanoparticles were effectively stabilized on AIPO-18 molecular sieve by a biomolecule-mediated green synthesis method. Based on the biocompatibility and electrostatic synergy of carboxymethyl chitosan (CMC), a high degree of Pt nanoclusters dispersion in AIPO-18 zeolites was achieved. The hydroconversion of levulinic acid (LA)was carried out at 160°C and 2 MPa hydrogen pressure, and the LA conversion of Pt/AIPO-18 (5CMC) reached 95.2% and the selectivity of γ-valerolactone (GVL) was 97.9% after 2 h. Pt/AIPO-18 (5CMC) exhibited satisfactory results that superior to the initial reactivity of Pt/AIPO-18 (0CMC) after five runs.
研究领域:
催化
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材料科学
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绿色化学
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能源技术
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产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
·
2022
·
IF 4.05
Zhou Shuolin,Long Min,Wu Lu,Lei Min,Bai JunZhuo,Huang Keying,Liu XianXiang,Yin Dulin
Covalently bonded sulfamic acid on the titanate nanotubes (TNTs-N(SO 3 H)-(CH 2 ) 2 -NHSO 3 H) was designed and successfully fabricated by the post-synthesis modification method. The as-prepared catalyst was characterized by a variety of characterization techniques such as FT-IR, TEM, XRD, XPS, and TG-DTG. The catalytic activity of TNTs-N(SO 3 H)-(CH 2 ) 2 -NHSO 3 H was evaluated for the synthesis of n-butyl levulinate (BL) from levulinic acid (LA). It was found that the tube-like structure of the TNTs still maintained during the modification process, and Brønsted and Lewis acid sites can be efficiently immobilized on the TNTs. The effects of reaction factors such as reaction time, reaction temperature, and catalyst dosage on the esterification of LA were systematically studied. Under the optimal reaction conditions, a relatively high yield of BL (95.3%) was achieved for esterification of levulinic acid owing to the strong Brønsted acidic sites. Furthermore, the hybrid catalyst TNTs-N(SO 3 H)-(CH 2 ) 2 -NHSO 3 H was used at least five times without significant decrease in activity, and no leaching of the active species in hot filtration test was observed. Graphical abstract
研究领域:
化学工程
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催化材料科学
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产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Ni Wei,Xin Xu,Jiushun Qin,Wei Lai,Ruoyan Li,Chenhuan Lai,Qiang Yong
Development of green pretreatment strategies with excellent lignin removal ability is particularly important for masson pine biorefinery. γ-Valerolactone (GVL), as a green and recyclable solvent, has unique solvent characteristics to extract lignin. In this study, three acid catalysts, including sulfuric acid (H 2 SO 4 ), hydrochloric acid (HCl) and p -toluenesulfonic acid (TsOH), were used to catalyze γ-valerolactone (GVL) pretreatment of masson pine. Among them, the TsOH-catalyzed GVL pretreatment achieved the highest lignin removal ratio and the best cellulose enzymatic hydrolysis yield. Under the optimized pretreatment conditions (150 ℃, 150 mM TsOH, GVL/H 2 O (4:1, w/w), 1 h), the lignin removal ratio reached 89.0 %, achieving a 72 h glucose yield of 87.1 % from the pretreated residues. The solvent lignins from pretreatment liquid was separated and characterized by NMR analysis. Meanwhile, the hexoses in pretreatment liquid were further converted into levulinic acid (LA) using the TsOH-catalyzed bi-phase reaction systems. This study gives insights into developing a biorefining process for the effective utilization of masson pine.
研究领域:
生物化学
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生物质能工程
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2026
·
IF 10.6
Zhenbang Liu,Shenghui Zhou,Jiangang Wang,Jinghua Wang,Hongyou Cui
The efficient conversion of cellulose into levulinic acid (LA) is a challenge due to the recalcitrant crystalline structure of cellulose and the facile formation of humin during the conversion process. Herein, we report a highly efficient and green catalytic system, which is composed of LiCl·3H2O (molten salt hydrate, MSH) and a bifunctional NbP/HZSM-5 catalyst, achieving a LA yield of 85.8% from microcrystalline cellulose (MCC) under mild conditions. Mechanistic investigation indicates that MSH not only helps disrupt the cellulose crystallinity but also serves as a co-catalyst to promote catalytic activity of NbP/HZSM-5. Their synergistic effect markedly lowers the activation energy of the 5-hydroxymethyl furfural (HMF)-to-LA reaction. Moreover, MSH can activate the produced LA and formic acid (FA) as an autocatalytic proton shuttle to form a self-accelerating cycle, which drastically reduces the dependence on external acid inputs. In addition, the catalytic system demonstrates excellent recyclability, still maintaining an 82.1% LA yield after four cycles. This research not only offers an efficient route for LA production from cellulose but also exemplifies a green chemistry-advancing strategy by integrating benign solvents, recyclable catalysts, and atom-efficient autocatalysis which align with the core principles of green chemistry.
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DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
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2025
·
IF 2.8
Xiang Sun,Huilin Hu,Ning Kang,Zhenbiao Song,Shulai Lu,Songyang Huang,Shicheng Zhao
The research on ester-based lubricants for acrylonitrile–butadiene–styrene (ABS) resins has not yet received enough attention, and the structure–property relationship remains unknown. In this paper, 1,11-undecanediol levulinate (LAUD) and its ketalized derivative (K-LAUD) were successfully prepared as two ester-based lubricants for ABS, and the influence of the end-group structure on the lubrication properties was thoroughly evaluated. Both ABS/LAUD and ABS/K-LAUD were prepared by extrusion. Compared with ABS/LAUD, ABS/K-LAUD exhibited significantly lower glass transition temperature ( T g ), complex viscosity, and surface roughness. The tensile test results suggested that the elongation at break of ABS/K-LAUD increased by 23.3% compared to ABS/LAUD. This revealed that K-LAUD with ketal end-groups displayed enhanced lubrication properties in ABS. The lubrication mechanism was further proposed with molecular dynamic simulations. This could be primarily attributed to the unique ketal structure of K-LAUD, which offered abundant nucleophilic sites and a stronger binding energy with the polymer matrix. Furthermore, the presence of the 1,3-dioxane ring remarkably enlarged the free volume of the matrix and facilitated the molecular chain disentanglement, thus resulting in improved mobility and diffusivity of molecular chains. This work filled the research gap of structure–property relationships of ester-based lubricants for ABS and provided an academic foundation for the design of ester-based lubricants.
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DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Baoting Yi,Huimei Wang,Keyin Liu,Xiaohui Wang,Fangong Kong,Junli Ren
Catalytic biomass conversion is a crucial pathway for high-value utilization of renewable resources, yet current catalysts face limitations such as insufficient acid sites, poor product selectivity, and low cycling stability. This study developed a magnetic tin-based solid acid catalyst (Fe 3 O 4 @PDA-Sn) using 5-sulfoisophthalic acid sodium salt as a ligand and dopamine hydrochloride-coated Fe 3 O 4 for targeted catalytic conversion of sugarcane bagasse. Results demonstrated that the catalyst achieved a furfural yield of 86.2% and a levulinic acid yield of 32.5% at 170°C for 90 min, with FT-IR, NMR, and XRD confirming its differential deconstruction capability toward cellulose and hemicellulose. Mechanistic analysis demonstrated that the coordinated interaction between Brønsted and Lewis acid sites played a crucial role in steering the reaction toward specific pathways: hemicellulose hydrolysis products underwent dehydration to furfural (enriched in the organic phase), while cellulose was selectively cleaved to form levulinic acid. The catalyst maintained stable performance over 5 cycles without regeneration, with 97.3% magnetic recovery efficiency, offering a novel "facile magnetic separation–excellent cycling performance" strategy for hierarchical biomass conversion. This work provides critical insights into the design of multifunctional biorefinery catalysts for sustainable biomass valorization.
研究领域:
催化
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生物质转化
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绿色化学
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可再生能源
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材料科学
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产品关联
DOI
高影响因子
KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2019
·Vol. 36
·期 5
·740-752
·
IF 2.476
Gong Chen,Wei Junnan,Tang Xing,Zeng Xianhai,Sun Yong,Lin Lu
Biomass-derived levulinic acid (LA) and its esters are currently envisaged as versatile, renewable platform chemicals. In this study, cellulosic pulp derived from the cooking of lignocellulosic biomass with active oxygen and solid alkali was employed as raw material for the formation of LA or ethyl levulinate (EL). This pretreatment process is highly effective for the delignification and deconstruction of lignocellulose matrix, making a facile degradation of the resulting cellulosic pulp to LA or EL. At this point, the acid-catalyzed hydrolysis or ethanolysis of cellulosic pulp was optimized by response surface methodology (RSM), offering desirable LA yield of 65.3% or EL yield of 62.7%, which is significantly higher than those obtained from raw biomass. More importantly, coking behavior on the inwall of the reactor was eliminated during the hydrolysis or ethanolysis of cellulosic pulp, which is one of the top challenges for the acid-catalyzed conversion of biomass in an industrial scale.
研究领域:
生物化学
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可再生化学
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产品关联
DOI
高影响因子
Catalysts
·
2015
·Vol. 5
·期 4
·1636-1648
·
IF 2
Rui Wang,Xiaolin Xie,Yanxiu Liu,Zhigang Liu,Guofang Xie,Ning Ji,Lizhi Ma,Mingquan Tang
The kiwifruit industry is booming worldwide. As a result, a great deal of kiwifruit waste residue (KWR) containing monosaccharides is produced and discarded. This material shows great potential for the production of platform chemicals. In this study, a series of Nb/Al oxide catalysts were synthesized via a facile and low-cost coprecipitation method, and their structures were characterized using: thermal gravimetric analysis (TGA), XRD, FESEM, TEM, X-ray photoelectron spectroscopy (XPS), NH3-TPD, N2adsorption-desorption, and FTIR-Pyridine adsorption. Experimental results of sugar-to-levulinic acid (LA) conversion revealed that the 20%Nb/Al oxide catalyst provided the highest catalytic performance and durability in terms of LA yield from fructose (74.2%) at 463 K after 10 min and from glucose (47.5%) at 473 K after 15 min. Notably, the 20% Nb/Al oxide catalyst with a 10% dosage is capable of converting kiwifruit waste residue to LA at 473 K after 10 min. In conclusion, the enhanced catalytic performance was obtained due to the high acidity, and large surface areaof Nb/Al oxide catalyst.Keywords:levulinic acid;kiwifruit waste residue (KWR);heterogeneous catalysis;Nb/Al oxide catalyst
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 38
·16526-16536
·
IF 3.288
Xufeng Bai,Ting Ren,Jingbo Mao,Shenmin Li,Jingmei Yin,Jinxia Zhou
Cellulose-derived levulinic acid (LA) can be converted into gamma-valerolactone (GVL), a sustainable platform chemical for the production of bio-based chemicals. However, LA as an organic acid causes severe metal leaching during the heterogeneous hydrogenation of LA to GVL, especially in the presence of water. Various endeavors for preventing metal leaching have focused more on the process and less on the intrinsic nature of catalysts. The aim of this work is to derive a novel metal-leaching-resistant catalyst for the aqueous-phase hydrogenation of LA into GVL by using a nanocomposite containing three components, Ag, ZrO2, and graphene oxide (GO). The AgZrO2GO catalyst without pre-reduction treatment resulted in complete conversion of LA and approximately 100 mol% selectivity to GVL in the aqueous reaction, and metal leaching from the catalyst was completely eliminated. The relationship between the catalytic performance and the distinct physicochemical properties of the catalyst was extensively discussed.
研究领域:
化学工程
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催化材料
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Meng-xing Xu,Yan Xu,Yu-zhen Liu,Dan Zhao,Shun-min Ding,Chao Chen
Acquiring practical catalysts was crucial for promoting the application of advanced chemical transformations. Here, a series of Co-Ni-P catalysts with addition of Y were designed for hydrogenation transformation of biomass-derived levulinic acid (LA) or furfural (FAL) in water. The molar-composition-manipulated catalysts were characterized in Co-Ni phosphide alloy nanostructure with YPO 4 enriched on surface and denoted as (YPO 4 ) x /Co y Ni 2-y P. By comprehensive catalytic measurements, both Co:Ni ratio in phosphide alloy and amount of YPO 4 were testified to be key factors to modulate intrinsic catalytic properties (hydrogen activation and acid catalysis) along Y-Co-Ni-P interface, the attractive and reproducible yield for desired product γ-valerolactone (up to 98 %) or cyclopentanone (up to 93%) could achieve under low H 2 pressure of 0.1–0.5 MPa over the well modulated catalyst (YPO 4 ) 0.2 /Co 1.0 Ni 1.0 P in comparison with high H 2 pressure (beyond 1.0 MPa) required in most of literature systems, indicating that the efficiency and feasibility of these important biomass transformations could be greatly enhanced on the low-cost and robust (YPO 4 ) x /Co y Ni 2-y P catalysts. These findings suggested that the phosphide-alloy engineering technique provided in this work could serve as a novel and practical method for innovating competitive catalysts to boost advanced heterogeneous catalysis applications as well as current aqueous hydrogenation transformations of biomass derivatives.
研究领域:
催化化学
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生物质能
·
绿色化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）