RENEWABLE ENERGY
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2022
·
IF 8.634
Rulu Huang,Huai Liu,Junhua Zhang,Yuan Cheng,Liang He,Lincai Peng
Design catalytic materials with high Lewis acid/base sites for catalytic transfer hydrogenation (CTH) of levulinic acid (LvA) to γ-valerolactone (GVL) is highly demanded but challenging. Herein, we report a concept of metal ion-polymer hybridization to design a tea polyphenol (TP) and HfCl 4 co-doped polyacrylonitrile (PAN) nanofiber (Hf@PAN-TP) via electrospinning technique . Comprehensive characterization revealed the well coordination between hafnium ions and phenolic hydroxyl groups of TP on PAN fiber, which promoted the formation of Lewis acid and Lewis base sites. As expected, a satisfactory GVL yield of 99.1% with 100% of LvA conversion was obtained using isopropanol as a hydrogen donor at 170 °C in 5 h, and the catalytic activity remained unchanged for five cycles. The kinetic study revealed the lower activation energy for CTH of LvA to GVL (33.5 kJ/mol), demonstrating the outstanding GVL formation rate of 3383.9 μmol/g . h. Based on the systematical combine of catalyst characterization and catalytic behavior, the structure-function relationship and reaction mechanism were proposed. More gratifyingly, Hf@PAN-TP was applicable for catalytic reduction of various carbonyl compounds, demonstrating a great potential for upgrading biomass-derived aldehydes/ketones.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Jiaxin Tang,Jingke Liu,Xinhui Chen,Quanyuan Qiu,Wanqi Peng,Xinyuan Fu,Chenxi Shi,Xiaoqing Lin
Efficient separation of levulinic acid (LA) from biomass hydrolysates remains a major challenge, particularly at high LA concentrations where conventional fixed-bed adsorption suffers from increased competitive adsorption, long cycle times, and high solvent consumption. This study developed a four-zone continuous chromatographic separation process using the hyper-cross-linked resin SY-01 for the recovery of high-concentration LA from simulated biomass hydrolysates. Adsorption equilibrium, competitive adsorption, and kinetic behaviors were first investigated, followed by optimization of fixed-bed adsorption and construction of a continuous chromatographic system. The separation performances of the two operating modes were then quantitatively compared under identical conditions. SY-01 exhibited high adsorption capacity and rapid adsorption kinetics toward LA, while the continuous system achieved stable operation with a peak LA concentration of 321.15 g/L (3.21-fold enrichment). Compared with conventional fixed-bed adsorption, continuous operation reduced cycle time by 86.8%, ethanol consumption by 65.7%, and water consumption by 40.0%, while substantially increasing process throughput. These results demonstrate that integrating SY-01 with four-zone continuous chromatography provides an efficient, economical, and environmentally friendly strategy for industrial recovery of high-concentration levulinic acid.
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LWT-FOOD SCIENCE AND TECHNOLOGY
·
2026
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IF 7.1
Guohua Teng,Min Zhou,Initizar Anwar,Yang Liu,Fuyi Li,Yanxu Chang,Yidan Wang,Yuefei Wang,Fei Tian
Flavonoids in Scutellaria Radix ( SR ) exhibit significant pharmacological activities, yet conventional extraction methods often suffer from low efficiency and poor selectivity. Here, a green and effective strategy was developed using deep eutectic solvent (DES)-functionalized magnetic nanoparticles for selective flavonoid enrichment. Forty-eight DESs were screened, and levulinic acid/L-proline (2:1) was identified as the optimal system. The selected DES was employed to synthesize Fe 3 O 4 @SiO 2 @DES, which demonstrated high specificity and adsorption performance in magnetic solid-phase extraction. Under optimized conditions, adsorption efficiencies for four representative flavonoids ranged from 0.770 ± 0.01 to 0.983 ± 0.002, with desorption recoveries of 0.551 ± 0.003 to 0.919 ± 0.019. The method showed excellent linearity (R 2 ≥ 0.9998) and low limits of detection and quantification (0.01-0.35 μg mL −1 and 0.03-0.98 μg mL −1 , respectively). Moreover, the adsorbent retained high adsorption efficiency after six reuse cycles, demonstrating stability and reusability. This work provides a sustainable and selective approach for flavonoid enrichment from SR and highlights the potential of DES-functionalized magnetic nanomaterials as an eco-friendly alternative to conventional organic solvent-based extraction.
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ChemSusChem
·
2023
·Vol. 16
·期 21
·e202300754
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IF 8.4
Jing Guo,Feng Li,Yuting Chu,Peng Zou,Chuang Li
Graphical The 10 % Ni@CeOx catalyst exhibits excellent catalytic efficiency in the reduction amination of levulinic acid to prepare 1,5-dimethyl-2-pyrrolidone. 1,5-dimethyl-2-pyrrolidone (MNMP), as a highly efficient green solvent, can be obtained from biomass-derived levulinic acid and its esters with 100 % conversion and 96.8 % yield over a 10 % Ni@CeOx catalyst at 140 °C, 2 MPa H 2 , 8 h, and with water as the solvent. Structure-property correlation investigations were performed with diverse characterization methods, including BET, XRD, XPS, TEM, HAADF-STEM, H 2 -TPR, NH 3 -TPD, CO 2 -TPD and FT-IR, and the results revealed that the excellent catalytic performance of the 10 % Ni@CeOx catalyst was mainly resulted from the strong interaction between Ni and CeOx, which formed more catalytic active sites and contributed to higher reductive amination efficiency. Besides, the 10 % Ni@CeOx catalyst had a chemisorption effect on LA. This was also the key to the excellent catalytic activity of the 10 % Ni@CeOx catalyst. The 10 % Ni@CeOx catalyst exhibited great stability throughout 6 reaction runs and excellent catalytic efficiency in the kilogram scale preparation of MNMP. This work provides a low-cost, efficient, and environmentally friendly heterogeneous catalytic system for the production of MNMP.
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CARBOHYDRATE RESEARCH
·
2022
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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.
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Materials
·
2022
·Vol. 15
·期 21
·7464
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IF 3.748
Ying Yang,Suoying Zhang,Lin Gu,Shijie Hao
Herein, we report a stable catalyst with Ru single atoms anchored on a one-dimensional carbon fiber@graphitic carbon nitride hierarchy, by assembling wet wipes composed of fiber-derived carbon fiber (CF), melamine-derived graphitic carbon nitride (g-C3N4) and RuCl3 before NaBH4 reduction. The atomically dispersed Ru species (3.0 wt%) are tightly attached via N-coordination provided by exterior g-C3N4 nanosheets, and further stabilized by the interior mesoporous CF. The obtained CF@g-C3N4–Ru SAs catalyst can be cycled six times without notable leaching of Ru or loss of GVL yield in the acidic media. This catalyst is more stable than Ru nanoparticles supported on CF@g-C3N4, as well as Ru single atoms anchored on CF and g-C3N4, and proves to be one of the most efficient metal catalysts for aqueous LA hydrogenation to γ-valerolactone (GVL). The isolated Ru atoms by strong N-coordination, and their enhanced electron/mass transfer afforded by the one-dimensional hierarchy, can be responsible for the excellent durability of CF@g-C3N4–Ru SAs under harsh reaction conditions.Keywords:Ru single atom;one-dimensional hierarchy;levulinic acid;γ-valerolactone;stability
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BIORESOURCE TECHNOLOGY
·
2022
·
IF 11.889
Shanta Dutta,Qiaozhi Zhang,Yang Cao,Chunfei Wu,Konstantinos Moustakas,Shicheng Zhang,Ka-Hing Wong,Daniel C.W. Tsang
Lignocellulosic paper waste constitutes a major waste stream globally, which should be valorised for chemical production. However, paper properties ( e.g. , feedstock composition, cellulosic crystallinity, and thermal stability/degradability) vary with raw materials and pulping processes. This study investigated levulinic acid (LA), hydroxymethylfurfural (HMF), and furfural production by H 2 SO 4 and FeCl 3 catalysed conversion of nine types of paper wastes in a green solvent system (1:1 γ‐valerolactone/water). At 160–180 °C for 1–20 min, ∼23–27 wt% LA yield was achieved from sanitary papers, tracing/parchment paper, and paper food box mainly containing crystalline cellulose, while a lower LA yield (∼10–20 wt%) was obtained from other paper wastes with high contents of ash and lignin. A higher selectivity towards HMF (∼12 mol%) was achieved in the presence of FeCl 3 . A furfural yield of ∼ 4–7.5 wt% was also obtained from the hemicellulose content. This study elucidates crucial factors and desirable characteristics of paper waste for catalytic valorisation.
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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
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Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 134
·期 2
·777-792
·
IF 2.081
Liu Yingxin,Zhang Kaiyue,Zhang Liang,Wang Yun,Wei Zuojun
The selective reductive amination of levulinic acid (LA) into pyrrolidone derivatives is regarded as one of the most promising reactions in the fields of biomass conversion into high value-added chemicals. Herein, we report a one-pot synthesis of N -substituted-5-methyl-2-pyrrolidones by reductive amination of LA/ester with nitriles over several commercial catalysts. Among the catalysts texted, Pd/C was found to be the most efficient for the reductive amination of LA/ester with various nitriles to give high yields of pyrrolidones (up to 92%) under mild reaction conditions (80 °C, 1.6 MPa H 2 , tetrahydrofuran solvent). And the catalyst showed good reusability.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Yaowei Lu,Yongxing Wang,Qinghu Tang,Qiue Cao,Wenhao Fang
The synergistic effect in a bimetallic oxide usually plays a vital role in determining the behavior of supported-metal catalysts. We show the unique synergy in a Sn x Mn 1 O y oxide, which can boost the hydrogenation catalysis of supported Pt nanoparticles for selective conversion of levulinic acid (LA) to γ-valerolactone (GVL). On a series of Pt/Sn x Mn 1 O y catalysts with a similar Pt loading ( ca. 0.44 wt%) and a controlled Pt size ( ca. 2.7 nm), the intrinsic TOF presents a volcano-like dependence on Pt 0 sites and Lewis acidity, which is determined by the variable synergistic effect between MnO y and SnO y . The optimal Pt/Sn 0.8 Mn 1 O y catalyst exhibits a high i TOF of 2709 h −1 and achieves 100% selectivity to GVL at 99% conversion of LA at 120 ℃ and 2 MPa of H 2 . DFT calculations demonstrate that the incorporation of Sn can provide a lower energy barrier for the crucial elementary reactions.
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ENERGY & FUELS
·
2019
·
IF 3.021
Mingxue Su,Wenzhi Li,Qiaozhi Ma,Song Li,Tao Yang,Xiaomeng Dou
A water-tolerant, basic, and hierarchical MFI zeolite catalyst was synthesized and applied in the aldol condensation reaction between biomass-derived furfural and levulinic acid. The results showed that the addition of poly(diallyl dimethylammonium chloride) significantly affected the textural and acid–base properties of hierarchical zeolite, which subsequently influenced the catalytic performance of hierarchical zeolite. In the aqueous phase, potassium-modified, hierarchical MFI zeolite (K/H-MFI-n) was more active for aldol condensation between furfural and levulinic acid than the potassium-modified, conventional MFI zeolite (K/MFI). This was ascribed to higher basic sites density and improved diffusion limitation of K/H-MFI-n. A 70.6% yield of aldol condensation product was achieved with a complete conversion of furfural at 100 °C for 9 h by K/H-MFI-0.6. However, only 27.4% yield of aldol condensation product with 55.1% furfural conversion was obtained by K/MFI at the same condition. Two major isomeric aldol products, β-furfurylidenelevulinic acid and δ-furfurylidenelevulinic acid (β-FDLA and δ-FDLA), were obtained after acidification. K/H-MFI-n displayed an enhanced selectivity (54.9%) to δ-FDLA, owing to the stronger basicity of K/H-MFI-n. However, K/MFI showed a preferred selectivity to β-FDLA (42.7%), owing to the dominant Lewis acidity. Recyclability research showed that the catalytic performance of potassium-modified, hierarchical MFI zeolite was acceptable after five runs.
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NEW JOURNAL OF CHEMISTRY
·
2015
·Vol. 39
·期 10
·8158-8164
·
IF 3.086
Dongshun Deng,Guoqiang Han,Yaotai Jiang
Efficient and reversible absorption of SO2 in six new deep eutectic solvents (DESs) composed of levulinic acid (LA) and quaternary ammonium salts (choline chloride, CC; choline acetyl chloride, CAC; tetraethylammonium chloride, TEAC; tetraethylammonium bromide, TEAB; tetrabutylammonium chloride, TBAC; tetrabutylammonium bromide, TBAB) was systematically investigated. The molar ratio of LA to quaternary ammonium salt was fixed at 3 : 1. The results showed that all DESs possessed satisfactory performance for SO2 absorption, with the maximum absorption capacity of 0.625 g SO2 per g DES of LA–TEAC at 293.15 K under ambient pressure. The absorbed SO2 was easily released by bubbling N2 at 323.15 K and the regenerated DES was recycled five times without obvious loss of absorption performance. The solubility of SO2 in DES of LA–CC at T = 293.15, 303.15, 313.15, and 323.15 K under subatmospheric pressures was also determined. The relative thermodynamic parameters, i.e., absorption enthalpy, absorption entropy, and absorption Gibbs free energy, were further calculated, giving results with small negative values. The influence of water content on the SO2 absorption was also investigated. According to NMR and FTIR analyses, the absorption of SO2 in DES was a physical process. Moreover, all the DESs exhibited high selectivity for SO2/CO2. The present DESs are promising absorbents for SO2 because of their high absorption capacity and good reversibility.
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