Biomass Conversion and Biorefinery
·
2021
·Vol. 13
·期 4
·2933-2946
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IF 4.987
Zhao Sibo,Wang Zihua,Chang Chun,Li Pan,Xu Guizhuan,Pang Shusheng
A two-stage alcoholysis was developed for improved conversion of furfural residue (FR) into levulinic acid (LA) and methyl levulinate (ML). Mixed acids including 0.01 M of H 2 SO 4 and Al 2 (SO 4 ) 3 and methanol/water (50/50 v/v%) were identified as the suitable catalyst and reaction medium. The optimum alcoholysis conditions were 198 °C and 1.5 h for the 1st stage and then 163 °C and 1.3 h for the 2nd stage, and the maximum total yield of LA and ML can reach 25.64%. The reaction kinetics and possible conversion pathways for ML and LA production were proposed. On the basis, HCOOH/H 2 O 2 pretreatment was screened for the pretreatment of FR, which increased the cellulose content of FR from 40.01 to 71.91%. The maximum total yield of LA and ML from pretreated FR was 44.96% under the optimum conditions of 195 °C and 1.9 h for the 1st stage and then 166 °C and 1.1 h for the 2nd stage, which was 16.09% higher than that of isothermal alcoholysis. The reusability tests showed that the Al 2 (SO 4 ) 3 was stable and can be reused at least 5 times. This study developed a new method for high-value utilization of FR and cleaner production of LA and ML.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2020
·
IF 4.244
Xiaoyun Li,Xuebin Lu,Shuangxi Nie,Min Liang,Zhihao Yu,Bingyu Duan,Jiaxin Yang,Rui Xu,Lefu Lu,Chuanling Si
A feasible approach to convert glucose and cellulose to levulinic acid applying phosphotungstic acid as catalyst in deep eutectic solvent was proposed. In our study, phosphotungstic acid was considered to be an effective catalyst for levulinic acid production. A considerable yield of levulinic acid (98.9 %) from glucose was achieved using 30 g/L phosphotungstic acid as catalyst at 468 K for 80 min. The peak levulinic acid yield from cellulose was 88.6 % for 120 min at the present temperature and phosphotungstic acid concentration. The reaction system exhibits efficient performance for the conversion of glucose and cellulose, which was due to the combation of phosphotungstic acid and deep eutectic solvent enhanced the levulinic acid production. Additionally, the kinetic study of levulinic acid formation from cellulose was investigated to supply a further insight on the whole biorefining process. The kinetic model agreed with the experiment data well. The activation energy for levulinic acid formation was 47.2 kJ/mol, which obtained from a modified Arrhenius equation.
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Russian Journal of Physical Chemistry A
·
2020
·Vol. 93
·期 13
·2620-2627
·
IF 0.719
Yanyan Xu,Lu Tianliang,Bu Ningning,Luo Qianqian,Qing Yashi,Lin Li
Abstract Catalytic conversion of biomass based platform chemicals to value added chemicals has attracted much attention recently. In this work, Ni-based catalysts were developed for the conversion of levulinic acid to γ-valerolactone. By investigation of reduction behavior of NiO, it was found that a relatively low reduction temperature (300°C) can provide the reduction of NiO to Ni 0 . The high reduction temperature (500°C) generally applied in literature is not necessary. The effect of supports was also studied, and hierarchical AlPO 4 -5 (AlPO 4 -5-meso) supported Ni showed the best catalytic performance due to the proper pore size of AlPO 4 -5-meso, which contains both micropores and mesopores. The effect of Ni loading was also investigated, 10 wt % of Ni is enough for this reaction, which is lower than the reported amount of Ni loading. By using Ni/AlPO 4 -5-meso with 10 wt % Ni as catalyst, 84% γ-valerolactone yield and 100% levulinic acid conversion can be obtained after reaction for 10 h at 180°C.
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Molecular Catalysis
·
2019
·
IF 2.938
Zhi-Xin Li,Xian-Yong Wei,Guang-Hui Liu,Xing-Long Meng,Zheng Yang,Shuo Niu,Di Zhang,Hua-Shuai Gao,Zhi-Hao Ma,Zhi-Min Zong
Highly selective hydrogenation of furfural and levulinic acid (LA) was studied over Ni 0.09 Zn/NC 600 derived from zeolitic imidazolate frameworks. The existence of active Ni 3 ZnC 0.7 particles in Ni 0.09 Zn/NC 600 was confirmed by multiple characterizations. As a result, over Ni 0.09 Zn/NC 600 , 99.7% of furfural conversion (FC) and 100% of furan-2-ylmethanol selectivity (FMS) were achieved in isopropanol (IP) at 170 °C for 2 h, while FC and (tetrahydrofuran-2-yl)methanol (THFM) selectivity are 97.5% and 86.4% in water at 150 °C for 1 h. Over the same catalyst, LA was completely converted to γ-valerolactone in water at 95 °C for 0.5 h. The catalyst is still highly active after 6 cycles of recycling with 92.8% of FC and 100% of FMS in IP at 170 °C for 1.5 h and 90.1% of LA conversion and 100% of γ-valerolactone selectivity in water at 80 °C for 0.5 h.
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Biomass Conversion and Biorefinery
·
2023
·
IF 4
Zhao Shiqiang,Gui Gang,Zhang Weihong,Chen Wei,Zhao Sibo,Xu Guizhuan,Chang Chun
Levulinic acid (LA) is an important biobased platform chemical, which can be produced from carbohydrates via acid hydrolysis. However, the LA concentaration is usually low via the batch process, which is not conducive to its subsequent separation and purification. In this study, we improved the LA production by using novel fed-batch hydrolysis. Compared with the batch process, the LA yield of the one-time feeding process and two-time feeding process increased to 38.66% and 40.60% from 27.80%, the LA concentration increased to 49.83 g/L and 52.33 g/L from 35.83 g/L, respectively. The feasibility of using the waste solid residue generated during the LA production as filler was further investigated. The polyurethane foam was prepared with the incorporation of solid residue, and the compressive strength of the biobased polyurethane foam composites increased by 32.08% with the addition of 5% solid residue. The characterization of the biobased polyurethane foam indicated the solid residue can be used for polyurethane foam enhancement. This study provided a novel method for the efficient and clean production of LA and high-value utilization of the waste produced in the process.
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FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Wansi Lin,Lincai Peng,Huai Liu,Junhua Zhang
Zirconium-derived catalyst with abundant Lewis acid-base pairs has earned it a place of prominence for the catalytic upgrade of bio-based carbonyls to valuable chemicals and fuels through catalytic transfer hydrogenation (CTH) reaction. However, the low catalytic efficiency of Zr-based catalysts urgently needs to be improved to meet the criterion for their industrial deployment. In this contribution, tungstophosphoric acid (HPW) was demonstrated as an effective modifier to the electronic structure of the pristine polyacrylonitrile and lignin-supported Zr nanofiber (Zr-Lig@PAN) to boost the CTH of levulinic acid (LA) into γ-valerolactone (GVL). Especially, an impressive GVL formation rate of 32.5 mmol·g −1 ·h −1 was implemented over Zr/HPW 0.75g -Lig@PAN, significantly prevailing over the previous reported Zr-based catalysts for the CTH of LA or its ester to GVL. Mechanistic investigations well demonstrated that the superior electron-accept ability of HPW allowed the construction of electron-deficient Zr sites, which is beneficial to the adsorption and activation of LA and isopropanol, thus boosting the CTH reaction. These findings open up a new avenue to design efficient Zr-based catalysts for the CTH reaction by elaborately tuning the electronic structure of the catalyst in the presence of a second metal.
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PROCESS BIOCHEMISTRY
·
2018
·
IF 2.616
Chen Liang,Yangdong Hu,Yan Wang,Lianying Wu,Weitao Zhang
Levulinic acid (LA) is an important platform chemical, the production of which by using biomass resources such as corncob is of great significance to the sustainable development. Traditional hydrolysis processes yield low concentrations of levulinic acid with large amounts of acid being consumed. In this paper, a new fed-batch process for hydrolyzing corncob residues with sulfuric acid being utilized as the catalysis to produce levulinic acid at high concentrations is proposed. The mass concentration of the levulinic acid increased with growing the times of feeding and a 107.93 g/L of the levulinic acid can be reached at the 7th hydrolysis. However, the yield of levulinic acid reduces gradually during the fed-batch process. To explore the phenomenon, the reaction mechanism of cellulose acid hydrolysis was experimentally studied. It can be deduced that the reduction of the levulinic acid yield was caused by the polymerization of the soluble humin analogues and the 5-hydroxymethyl furfural (5-HMF) as well as the glucose.
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ENERGY & FUELS
·
2024
·
IF 5.2
Yifan Wang,Kaifeng Lu,Yuan Zhao,Lingjun Zhu,Shurong Wang
Converting renewable biomass into liquid fuels and value-added chemicals has emerged as a pivotal technology, driving the transformation of the energy landscape. Efficiently transforming the cellulose components of biomass into the crucial liquid fuel precursor levulinic acid holds profound significance. The principal objective of this study is to fabricate a temperature-responsive catalyst based on Al-doped silicotungstic acid, which is intended for converting glucose into levulinic acid. By exploiting the interaction between choline chloride and silicotungstic acid, which exhibits a notable capacity for high proton migration, we successfully synthesized a stable acid catalyst with responsive properties to temperature changes. Through precise adjustments of Al3+ concentration, we engineered a collection of Lewis/Brønsted composite catalysts capable of responding to temperature variations. A comprehensive analysis of the catalyst’s structure and acidity was conducted using various techniques including FTIR, XRD, TEM, and Py-IR. These methods revealed crucial insights into the crystalline architecture, surface morphology, and distribution of acidic domains, providing a solid foundation for a deeper understanding of the catalytic reaction mechanism. Through the meticulous optimization of key reaction parameters, including Al3+ loading, solvent composition, reaction temperature, and reaction duration, the ChAl2/3HSiW12O40 catalyst achieved its pinnacle of efficiency at 150 °C over an 8 h period. This resulted in the remarkable outcome of complete glucose conversion, yielding an impressive 62.01% of levulinic acid. Additionally, an evaluation of the catalyst’s recyclability was carried out, demonstrating its commendable hydrothermal stability and ability for repetitive usage without any reduction in catalytic efficiency.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Mingya Liu,Hanli Zheng,Xiaohui Yang,Zewei Hu,Yunxi Hou,Lu Shen,Dongyu Liu,Shitao Yu,Lu Li,Shiwei Liu,Yue Liu
The high efficiency production of renewable resources has been widely used in fuel and synthetic chemistry. In this work, a series of novel, efficient Pd@mSiO 2 -xCeO 2 bifunctional yolk-shell catalysts have been developed and applied to the preparation of γ-valerolactone by the hydrogenation of levulinic acid. The results showed that CeO 2 can effectively improve the catalytic performance of the catalyst, then achieve 100 % conversion of levulinic acid and 97 % selectivity of γ-valerolactone. The characterization results showed that the addition of CeO 2 regulated the acid sites of the catalyst, promoted the reduction of PdO, thus promoting the formation of more Pd 0 . In addition, the kinetic experiment results showed that the activation energy of the reaction effectively decreased with the addition of CeO 2 . Then, the reaction mechanism was studied using Density functional theory (DFT) calculations. Finally, the encapsulation strategy of mesoporous silica shell provided a stable environment for the catalyst and maintains high activity after 5 cycles. The efficient and stable noble metal catalysts developed in this study significantly enhance the yield of biomass-derived γ-valerolactone. Their large-scale application not only supports the green production of biofuels and biodegradable materials but also establishes a material foundation for the generation of renewable energy, thereby contributing to the realization of a low-carbon circular economy.
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PubMed
高影响因子
CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2022
·
IF 4.119
Bin Wang,Haifeng Cong,Xingang Li,Hong Li,Xin Gao
The recovery of levulinic acid (LA) and formic acid (FA) from aqueous solutions and actual biomass hydrolysates by using the stepwise adsorption method was investigated for the first time. The carbon molecular sieve was used as the adsorbent for FA and microporous activated carbon was used as the adsorbent for LA according to the steric hindrance effect of the pore channels and the difference in molecular diameter of FA and LA. The adsorption data of LA and FA onto their respective adsorbents were measured and numerically analyzed by adopting batch adsorption experiment and fixed-bed column methods. In the study of static adsorption equilibrium experiment, the Langmuir equation fitted the data of LA adsorption on activated carbon, while the Freundlich equation fitted well the adsorption data of FA adsorption on carbon molecular sieve. In the kinetic study, the LA adsorption on activated carbon and FA adsorption on carbon molecular sieve confirmed the PSO model. Moreover, the effect of various conditions on fixed-bed column adsorption progress was investigated, which indicated that the adsorption property improved with feed flow rate, column length, temperature decreasing and initial concentration increasing. The Yoon-Nelson model was adopted to predict and analyze the whole process of adsorption breakthrough and consistent well with the experimental data. The separation of LA and FA was realized by continuous fractional adsorption.
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RSC Advances
·
2018
·Vol. 8
·期 71
·40989-40995
·
IF 2.936
Ruifeng Wang,Lungang Chen,Xinghua Zhang,Qi Zhang,Yuping Li,Chenguang Wang,Longlong Ma
Novel catalytic material with high catalytic activity and hydrothermal stability plays a key role in the efficient conversion of levulinic acid (LA) to γ-valerolactone (GVL) in water. In this study, mixed oxides Al2O3–TiO2, Al2O3–MoO3 and Al2O3–Co3O4 were synthesized by co-precipitation using aqueous solution of NaOH as precipitant. Ru catalysts supported on mixed oxides were prepared by impregnation method and their catalytic performances were tested in the hydrogenation of LA to GVL on a fixed bed reactor. The physicochemical properties of the catalysts were characterized by XRD, H2-TPR, NH3-TPD, and BET techniques. The TiO2 component significantly affected the acidity of the catalyst, and thus its catalytic activity for the GVL yield was affected. The desired product GVL with a yield of about 97% was obtained over the Ru/Al2O3–TiO2 catalyst under mild conditions (WHSV = 1.8 h−1, T = 80 °C). Moreover, the catalyst Ru/Al2O3–TiO2 exhibited excellent thermal stability in the test period of time.
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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.
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