Sustainable Energy & Fuels
·
2023
·Vol. 7
·期 11
·2645-2652
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IF 5.6
Rulu Huang,Yuan Cheng,Huai Liu,Lincai Peng,Junhua Zhang
It is incredibly challenging to design a catalyst with high activity for catalytic transfer hydrogenation (CTH) of levulinic acid (LvA) into gamma-valerolactone (GVL). In our previous work, we have designed a mesoporous acid-base bifunctional hybrid (Zr-FDCA) with high contents of Lewis acid (LA) and Lewis base (LB) sites from zirconium and 2,5-furandicarboxylic acid (FDCA) by using acetic acid as the modulator, which exhibited an outstanding performance in CTH of furfural into furfuryl alcohol. However, the catalytic performance was not satisfactory in CTH of LvA into GVL. Herein, we modified a Zr-FDCA hybrid with the introduction of phosphotungstic acid (HPWO). Comprehensive characterization revealed that HPWO could significantly affect the acidity, which afforded acid catalytic activity and introduced a Brønsted acid (BA) site. The synergistic effect between LA and BA sites resulted in the outstanding catalytic activity in CTH of LvA into GVL; a GVL yield of 95.4% with a high formation rate of GVL (12.72 mmol g−1 h−1) was obtained over Zr-FDCA-HPWO. Simultaneously, it also showed an ideal cycle stability and could be used for at least five consecutive runs with no significant loss in the catalytic activity.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Yunfei Zhang,Yi Shen
Converting levulinic acid (LA) to fuel precursors such as gama-valerolactone (GVL) and valeric acid (VA) via an efficient and low-cost method is of great significance. Herein, a series of free-standing electrodes consisting of metallic metals supported by carbon felts (CFs) were fabricated via a facile electro-deposition process. The resulting M/CFs (M = Pb, Cd, Co, Ni, Cu and Bi) electrodes were evaluated for electrocatalytic hydrogenation (ECH) of LA. The electrocatalytic activity of the electrodes was extensively studied by various electrochemical methods including cyclic voltammetry , linear sweep voltammetry and chronoamperometry measurements. The products of the ECH processes were analyzed by gas chromatography-mass spectrometry. Of all the prepared samples, the Pb/CFs and Cd/CFs electrodes showed superior performance for ECH of LA. The selectivity of VA reached up to 91.7% when the Pb/CFs was used and the conversion of LA reached to 57.2% using the Cd/CFs electrode, rendering them as one of the best electrodes for ECH reported in the literature. The effects of applied potentials on the ECH process were investigated. To further optimize the ECH performance of the Pb/CFs electrodes, several key parameters including deposition time , pH value of the electrolyte and reaction time were studied. When the electrodeposition time was 600 s and the concentration of sulfuric acid in the electrolyte was 0.5 M, the complete transformation of 0.2 M of LA was achieved after 6 h. This study may afford an alternative way to the conversion of LA to GVL or VA.
研究领域:
化学工程
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电化学
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催化材料
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DOI
高影响因子
CATALYSIS SURVEYS FROM ASIA
·
2018
·Vol. 22
·期 3
·129-135
·
IF 3.081
Zhang Di,Zhao Yun-Peng,Fan Xing,Liu Zhong-Qiu,Wang Rui-Yu,Wei Xian-Yong
A series of Ni/HZSM-5 catalysts with different Ni-loadings and Si/Al ratios were prepared by incipient wetness impregnation and employed for catalytic hydrogenation of levulinic acid (LA) to gamma-valerolactone (GVL). Their physicochemical properties were characterized by X-ray diffraction, nitrogen adsorption–desorption, X-ray photoelectron spectrometer, temperature-programmed desorption of ammonia,transmission electron microscopy, temperature-programmed reduction of hydrogen, and pyridine-adsorbed infrared spectroscopy. The diffraction peaks assigned to Ni phase were not observed, implying that nickel particles were small and had a high dispersion on the supports. The catalysts with a strong acidity and the appropriate ratio of Brönsted (B) acid sites to Lewis (L) acid sites (B/L = 4.9) show an excellent activity and selectivity for the hydrogenation of LA to GVL. High conversion of LA and selectivity towards GVL were achieved over 5 wt% Ni/HZSM-5-50. The maximum GVL yield of 100% over 5 wt% Ni/HZSM-5-50 was obtained under the optimized reaction conditions of 210 °C, 2 h, and 3 MPa initial hydrogen pressure.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Yafeng Fan,Lianhua Li,Gaixiu Yang,Yongming Sun,Linsong He,Peiwen Wu,Chun Ho Lam,Bing Song
Gamma-valerolactone (GVL) assisted NaOH/water pretreatment for hybrid pennisetum delignification was first investigated. Contrary to the hypothesized results, the addition of GVL significantly suppressed the delignification and hemicellulose removal by mild alkaline pretreatment (37 °C for 24 h). An addition of GVL to GVL/NaOH molar ratio of 1/1 resulted in lignin removal at ∼23% compared with that at ∼75% without GVL. This suppression effect was further confirmed by scanning electron microscopy and Fourier-transform infrared spectroscopy. The extracted lignin was further characterized by two-dimensional heteronuclear single quantum coherence nuclear magnetic resonance spectroscopy, suggesting that the addition of GVL suppressed the decomposition of large lignin molecules by NaOH/water and the release of hemicellulose, resulting in extracted lignin with lower molecular weights and less hemicellulose. The decrease in the partial alkalinity (PA) of alkaline solutions caused by GVL addition was likely the main reason for the suppressed delignification, suggested by the good correlation between PA and delignification in both GVL/NaOH/water and NaOH/water (R2 = 0.967). This study suggested that solvent-assisted alkaline pretreatment can also result in an unwanted suppression effect, and the changes in PA could be referred to as an indicator while selecting organic solvents.
研究领域:
生物化学
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可再生能源
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植物学
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Zhang Shun,Xu Wenhao,Du Rongcheng,Yan Lei,Liu Xuehui,Xu Shimei,Wang Yu-Zhong
Recycling strategies for mixed plastics and textile blends currently aim for recycling only one of the components. Here, we demonstrate a water coupling strategy to co-hydrolyze polyester/cotton textile blends into polymer monomers and platform chemicals in gamma-valerolactone. The blends display a proclivity for achieving an augmented 5-hydroxymethylfurfural yield relative to the degradation of cotton alone. Controlled experiments and preliminary mechanistic studies underscore that the primary driver behind this heightened conversion rate lies in the internal water circulation. The swelling and dissolving effect of gamma-valerolactone on polyester enables a fast hydrolysis of polyester at much lower concentration of acid than the one in the traditional hydrolysis methods, effectively mitigating the excessive degradation of cotton-derived product and undesirable product formation. In addition, the system is also applicable to different kinds of blends and PET mixed plastics. This strategy develops an attractive path for managing end-of-life textiles in a sustainable and efficient way.
研究领域:
材料科学
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化学工程
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可持续性
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纺织工程
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环境科学
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产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2019
·Vol. 149
·期 10
·2749-2757
·
IF 2.372
Lai Jinhua,Zhou Shuolin,Liu Xianxiang,Yang Yongjun,Lei Jing,Xu Qiong,Yin Dulin
Abstract The transformation of biomass-derived intermediates into value-added chemicals and liquid fuels is of great importance in sustainable chemistry. In this study, graphene oxide supported ZrO 2 (ZrO 2 /GO) was found to be an active heterogeneous catalyst for the transfer hydrogenation of ethyl levulinate to γ-valerolactone (GVL) with iso -propanol as the hydrogen donor. Several important reaction parameters such as the hydrogen donor, the reaction temperature and the catalyst loading were studied in detail with the aim to get a high yield of GVL. It was found that the structure of alcohols had a great effect towards the activity of the ZrO 2 /GO catalyst and the selectivity of GVL. Iso -propanol was the best hydrogen donor for the transfer hydrogenation of ethyl levulinate to GVL. The highest GVL yield reached 91.7% with an ethyl levulinate conversion of 96.2% under optimal reaction conditions. More importantly, the ZrO 2 /GO catalyst demonstrated a high stability without the loss of its catalytic activity during the recycling experiments, which should be due to the strong interaction between GO and ZrO 2 . Graphical Abstract The graphene oxide supported ZrO 2 (ZrO 2 /GO) catalyst showed high activity for the transfer hydrogenation of ethyl levulinate to GVL with a high yield up to 91.7%.
研究领域:
催化化学
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可再生资源化学
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DOI
高影响因子
BIORESOURCE TECHNOLOGY
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2020
·
IF 7.539
Peiwen Wu,Lianhua Li,Yongming Sun,Bing Song,Yun Yu,Huping Liu
This study is the first to integrate gamma-valerolactone/water (GVL/water) pretreatment with anaerobic digestion (AD) for biogas production and lignin nanoparticles (LNPs) synthesis. The hydrothermal treatment was conducted at 135 to 180 °C with GVL at 0 to 90%. After pretreatment, the compositions of hybrid pennisetum were changed with the removal of lignin, hemicellulose, and cellulose to different extent. Subsequent anaerobic digestion achieved a maximal specific methane yield of 228.00 ± 4.37 mL/g VS, compared with that at 165.11 ± 1.99 mL/g VS for the control. The highest actual methane yield (150 mL/g RM) was achieved by pretreatment with GVL/water (50/50) at 150 °C for 90 min. LNPs at 200 to 2000 nm were synthesized from the liquid waste with a yield at ~4 mg/mL. The mass balance of this integrated method was discussed. In general, the maximal valorisation of hybrid pennisetum was achieved based on a catalyst-free of GVL/water pretreatment.
研究领域:
生物能源
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环境科学
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生物质转化
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Qingrui Peng,Haijun Wang,Yongmei Xia,Xiang Liu
A multifunctional Zr-containing catalyst (FM-Zr-ARS) was successfully synthesized by a modulated hydrothermal synthesis route. Systematic characterization results supported the presence of robust porous inorganic-organic frameworks stabilized by the strong coordination interaction of Zr 4+ with oxygen-rich functional groups in Alizarin red S (ARS). Moreover, the -O-Zr-O- network in the FM-Zr-ARS structure formed a rich content of acid-base sites. In addition, the inherent sulfonic groups in ARS made the FM-Zr-ARS hybrids possess Brønsted acid sites. Therefore, under the synergistic catalysis of the multiple functional sites, FM-Zr-ARS showed remarkably high catalytic activity for γ-valerolactone (GVL) production from levulinate esters and furfural. Finally, 72.4 % and 97.7 % yields of GVL were obtained in the conversion of furfural and ethyl levulinate, respectively, after 8 h of reaction at 433 K. On the basis of the role of different functional sites, a plausible catalytic mechanism was presented for the conversion of biomass-derived furfural to GVL.
研究领域:
化学工程
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生物质转化
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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
FUEL
·
2016
·
IF 3.611
Zhenhuan Xiao,Huacong Zhou,Jianmin Hao,Hailong Hong,Yinmin Song,Runxia He,Keduan Zhi,Quansheng Liu
As the fast depletion of coal resources, exploring the value-added utilization approaches of low rank coals or their components and, in parallel, promoting the conversion of sustainable resources (such as biomass) into useful chemicals are critical issues facing human society. In this work, we used humic acids (HAs), an abundant material in nature (mainly derived from low rank coals), and the transition metal zirconium (Zr) to prepare a novel Zr-containing hydrogen transfer catalyst. The prepared catalyst was applied into the conversion of biomass-derived ethyl levulinate (EL) into gamma-valerolactone (GVL) via hydrogen transfer reaction. Both the preparation conditions of the catalysts and the reaction parameters during the conversion of EL into GVL were systematically investigated. The catalyst was characterized by SEM, TEM, FTIR, powder XRD, and TG analysis. The results demonstrated that the as-prepared catalyst was highly efficient for the conversion of EL into GVL. Under optimized conditions, EL could be completely converted and the GVL yield could reach up to 88.3%. The catalyst could be used at least 11 times without notable changes in both activity and structures, indicating an excellent stability. As far as we know, this is the first work using HAs to prepare Zr-containing catalyst and its application to the conversion of EL into GVL in biomass utilization.
研究领域:
化学工程
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可再生能源
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催化化学
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 45
·17441-17453
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IF 4.569
Yuewen Shao,Mingzhu Guo,Mengjiao Fan,Kai Sun,Guoming Gao,Chao Li,Félix Mérimé Bkangmo Kontchouo,Lijun Zhang,Shu Zhang,Xun Hu
One-pot conversion of furfural, a biomass-derived platform chemical, to gamma-valerolactone (GVL), a fuel additive and green solvent, involves multiple steps of hydrogenation. Among these reactions, the deep hydrogenation of the furan ring in furfural interrupts GVL formation over Ni or Co-based catalysts. In this study, a method of alloying Ni and Co with Fe over a ZSM-5 support was proposed for tackling excessive activity of the catalyst for hydrogenation. The results indicated that the formation of binary NiFe and CoFe alloys in Ni–Co–Fe/ZSM-5 enhanced the dispersion of metallic species, reduction of metal oxides, formation of more Lewis acidic sites, and the adsorption of the C–O functionality of the furan ring, while lowering the capability for adsorption/activation of H2 and the adsorption of the CC group of the furan ring. These factors together reduced the activity for the hydrogenation of the furan ring in furfural, but enhanced the hydrogenation of the CO in ethyl levulinate (EL). The kinetic study confirmed that the hydrogenation of EL was the rate-determining step. The coordination of the dual alloys, NiFe and CoFe, in the bifunctional Ni–Co–Fe/ZSM-5 catalyst rendered superior activity for selective one-pot conversion of furfural to GVL with a yield of 85.7%.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Xiaoqin Hai,Jiawei Liu,Qin Li,Yongpeng Ma,Ruiyu Fu,Hongbo Li,Yanhui Zhang,Xiaoli Guo,Xin Di
In this work, UiO-66-HCl-based dispersive solid-phase extraction (DSPE) was designed and developed for the enrichment of pyrethroid pesticide residues in water and food matrices before high performance liquid chromatography analysis. For the first time, gamma-valerolactone (GVL), a biodegradable, food-grade green solvent, was used as the eluent in DSPE process, realizing a significant progress in economic and ecological benefit. The stable and highly porous UiO-66-HCl was synthesized as the adsorbent by hydrothermal synthesis and hydrochloric acid etching. The prepared material was characterized by FT-IR, SEM, XRD, TGA and N 2 adsorption–desorption analyses, and the important parameters affecting the extraction efficiency were optimized. Under the optimized conditions, the method has shown satisfactory limit of detection (4 ∼ 5 μg/L) and desirable recoveries (78.3 %∼105.7 %) as well as excellent precision (RSD < 15.7 %). Moreover, the benefits of the proposed method were assessed via various green chemistry tools, and the extraction mechanism was also briefly investigated to understand the appealing adsroption performance. It was demonstrated that the method can be successfully applied for extraction and analysis of pyrethroid pesticide residues in water and food matrices, showing an excellent application potential for green analysis of trace components.
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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）