FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Yiwei Tang,Junyan Fu,Yicong Wang,Haixin Guo,Xinhua Qi
Hydrogenation of levulinic acid to γ-valerolactone is one of the important reactions for conversion of biomass into renewable fuels and chemicals. Ni-Zn non-noble bimetallic catalysts supported on ordered mesoporous carbon (Ni-Zn@OMC) were prepared by one-pot solvent evaporation induced self-assembly (EISA) method and used for hydrogenation of levulinic acid to γ-valerolactone (GVL) in water. A GVL yield of 93% was obtained over bimetallic Ni 1 -Zn 1 @OMC catalyst at 180 °C in 90 min reaction time, with a turnover frequency (TOF) of 686.4 h −1 . Compared with Ni@OMC, the incorporation of Zn metal leads to the formation of Ni-Zn alloy and high dispersion of Ni particle on the catalyst surface . NiO sites on the catalysts lowered competitive adsorption between H 2 and levulinic acid on Ni 0 sites, as well as the Ni-Zn alloy is beneficial to the activation of carbonyl group in levulinic acid, and they synergistically promote the hydrogenation of levulinic acid to 4-hydroxyvaleric acid (4-HVA). Zn content in the catalyst influences both the activity of Lewis acid sites and the ratio of Lewis acid to Brønsted acid sites, and the active sites of Ni δ– Zn δ+ can facilitates the weakening and cleavage of C-O in 4-HVA, both of them are beneficial to the dehydration of 4-HVA to GVL.
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Haibiao Yu,Xiu Jia,Peng Wang,Ying Xiong,Weijun Shan,Congge Zhang,Zhimeng Song
A series of x wt%Al-SBA-15 catalysts prepared by modified wetness impregnation was investigated for γ-valerolactone (GVL) decarboxylation to butene . It was found that the impregnation of Al species not only remained the ordered mesoporous structure of parent SBA-15, but also created large amounts of Brønsted and Lewis acid sites on the surface of catalyst. The considerable amount of solid acid sites and the suitable Brønsted/Lewis acid ratio endowed 2.23 wt%Al-SBA-15 catalyst an excellent catalytic performance. Under the optimized conditions, the GVL conversion and butene yield can reach 99.8% and 96.6% at 320 °C, respectively. Mechanism studies indicated that the decarboxylation of γ-protonated PEA controlled speed of the whole reaction. Moreover, the catalytic activity of regenerated 2.23 wt%Al-SBA-15 catalyst was satisfactory after eight cycle tests, and the butene yield could still reach 92.2%.
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高影响因子
RSC Advances
·
2021
·Vol. 12
·期 1
·602-610
·
IF 3.361
Yingxin Liu,Kai Liu,Meihua Zhang,Kaiyue Zhang,Jiao Ma,Shuwen Xiao,Zuojun Wei,Shuguang Deng
Highly active and thermally stable Cu–Re bimetallic catalysts supported on TiO2 with 2.0 wt% loading of Cu were prepared via an incipient wetness impregnation method and were applied for liquid phase selective hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) in H2. The effect of the molar ratios of Cu : Re on the physico-chemical properties and the catalytic performance of the Cu–Re/TiO2 catalysts was investigated. Moreover, the influence of various reaction parameters on the hydrogenation of LA to GVL was studied. The results showed that the Cu–Re/TiO2 catalyst with a 1 : 1 molar ratio of Cu to Re (Cu–Re(1 : 1)/TiO2) exhibited the highest performance for the reaction. Complete conversion of LA with a 100% yield of GVL was achieved in 1,4-dioxane solvent under the reaction conditions of 180 °C, 4.0 MPa H2 for 4 h, and the catalyst could be reused at least 6 times with only a slight loss of activity. Combined with the characterization results, the high performance of the catalyst was mainly attributed to the well-dispersed Cu–Re nanoparticles with a very fine average size (ca. 0.69 nm) and the co-presence of Cu–Re bimetal and ReOx on the catalyst surface.
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Shanhui Zhu,Huan Liu,Sen Wang,Xiaoqing Gao,Pengfei Wang,Jianguo Wang,Weibin Fan
One-step efficient conversion of cellulose into value-added γ-valerolactone (GVL) is of great interest because it not only integrates complex tandem reactions in one-step, but also does not need additional hydrogen sources. To achieve this goal, it is crucial to fabricate high-performance catalyst that can accelerate both hydrolysis of cellulose and further transformation of generated stoichiometric levulinic acid (LA) and formic acid (FA) into GVL. CoNi nanoparticles encapsulated in N-doped thin graphene shell gave GVL yield as high as 55.9 % at 200 °C combined with Ag + -exchanged heteropolyacid (AgPW). This composite catalyst is highly resistant to the corrosion of LA and FA, and hence shows high catalytic stability. LA-adsorption FTIR spectra and DFT calculations indicate that LA and FA can penetrate through shell graphene layers into core CoNi sites via cracks. Compared to H 2 , FA can much more rapidly reduce LA because of its low dissociation energy barrier and high dissociation rate.
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高影响因子
GREEN CHEMISTRY
·
2017
·Vol. 19
·期 16
·3869-3879
·
IF 9.125
Shurong Wang,Yuan Zhao,Haizhou Lin,Jingping Chen,Lingjun Zhu,Zhongyang Luo
For the purpose of building a green reaction system to produce furfural (FF), the conversion of two important pentoses from hemicellulose, namely xylose and arabinose, was investigated in an aqueous reaction system including a Lewis acidic ionic liquid as a catalyst and renewable γ-valerolactone (GVL) as a co-solvent. The results showed that the introduction of GVL greatly improved the reactivity of pentose and inhibited the secondary decomposition reaction of FF compared to a pure-water reaction system. NMR analysis suggested that the composition of pentose conformers was greatly altered towards a reactive distribution. The highest FF yields were 79.76% (from xylose) and 58.70% (from arabinose), which were obtained at 140 °C. The influence of reaction parameters on pentose conversion was also studied. A comparison between different reaction conditions suggested that arabinose had less reactivity than xylose, leading to its lower conversion rate and FF yield. Furthermore, xylan and real biomass materials were tested in the proposed reaction system, and decent FF yields of up to 69.66% (from xylan) and 47.96% (from corn stalk) were obtained.
研究领域:
生物化学
·
绿色化学
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DOI
高影响因子
Molecular Catalysis
·
2020
·
IF 3.687
Na Ji,Zhenyu Liu,Xinyong Diao,Jinrong Bao,Zhihao Yu,Chunfeng Song,Qingling Liu,Degang Ma,Xuebin Lu
GVL (γ-valerolactone) is identified as an important biomass platform molecule due to its wide application. In this work, a series of novel supported Ni catalysts with different supports and Ni loading were synthesized via metal-organic chemical vapor deposition (MOCVD) method for the hydrogenation of EL (ethyl levulinate) to GVL. Fourier transform infrared spectroscopy (FT-IR), X-ray powder diffraction (XRD), nitrogen adsorption/desorption, inductively coupled plasma optical emission spectroscopy (ICP-OES) and transmission electron microscopy (TEM) were used to characterize the as-synthesized catalysts. The results showed that the 2 wt.% Ni/AC(MOCVD) presented superior catalytic activity when compared with the catalyst prepared by impregnation method. This behavior is explained in terms of the smaller Ni nanoparticles (4.28 nm) and higher dispersion on 2 wt.% Ni/AC(MOCVD). Among the catalysts, the 2 wt.% Ni/AC catalyst exhibited the best catalytic performance with 99.7 % EL conversion and 79.8 % GVL yield under 1 MPa initial H 2 pressure (measured at room temperature) at 250 °C for 2 h. In addition, the reaction conditions were optimized and the stability of the catalyst were also investigated. The insights gained from this study in the design of high dispersed Ni particles with smaller particle size via MOCVD method will facilitate the metal-catalyzed hydrogenation of EL to GVL.
研究领域:
化学工程
·
生物质能源
·
催化科学
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DOI
高影响因子
ACS Catalysis
·
2016
·
IF 9.307
Shanhui Zhu,Yanfeng Xue,Jing Guo,Youliang Cen,Jianguo Wang,Weibin Fan
The high-yield synthesis of the biofuel γ-valerolactone (GVL) is a challenging task, which currently stems from the depolymerization of cellulose to levulinic acid, followed by its hydrogenation. We have developed a novel integrated process for the production of GVL from hemicellulose without using liquid acids and external hydrogen. The hemicellulose feed underwent hydrolysis and consecutive dehydration to produce furfural over ZSM-5 catalyst. Subsequently, the formed furfural with 2-propanol performed tandem conversion to GVL over Au/ZrO2 catalyst combined with ZSM-5. This process gave a high yield of GVL under mild conditions: up to 61.5% based on hemicellulose. The outstanding performance was mainly ascribed to the strong interface interaction of Au with ZrO2 species, large amounts of medium-strength acid sites over ZSM-5, and efficient synergy between active metal and acid sites.
研究领域:
生物化学
·
催化化学
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DOI
高影响因子
ACS Nano
·
2025
·
IF 16
Jingjing Cao,Wenji Zhan,Meng Ren,Yao Wang,Haifei Wang,Ni Zhang,Yuetian Chen,Tianfu Wang,Yanfeng Miao,Yixin Zhao
The application of promising perovskite light-emitting diodes (PeLEDs) faces a significant challenge known as efficiency roll-off, which refers to the decline in external quantum efficiency (EQE) at high current densities. This issue arises mainly from high trap densities in perovskite films and imbalanced carrier injection, which limit improvements in brightness and stability of PeLEDs. Here, we develop a green solvent strategy using γ-valerolactone (GVL) to suppress efficiency roll-off in PeLEDs. This strategy effectively slows down the crystallization kinetics, yielding cubic-phase formamidinium lead triiodide (α-FAPbI3) films with reduced trap states, enhanced charge carrier injection, and suppressed Auger recombination. As a result, we achieve a record radiance of 1411 W sr–1 m–2 for GVL-based PeLEDs. These PeLEDs exhibit a substantially reduced efficiency roll-off, maintaining an EQE above 20% even at a high current density of 900 mA cm–2. Our findings highlight the potential of the green solvent approach for developing high-brightness, high-efficiency PeLEDs for practical applications.
研究领域:
材料科学
·
光电技术
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Chanjuan Yang,Shoukang Xiao,Liyu Chen,Yingwei Li,Kui Shen
γ-Valerolactone (GVL) as an important high-value chemical can be readily produced through the catalytic hydrogenation of renewable levulinic acid (LA). However, high reaction temperatures (70–240 ℃) and H 2 pressures (0.5–6 MPa) are usually required to achieve full LA conversion and desired GVL yield in previous studies. Herein, we report, for the first time, the ambient-condition upgrading of LA to GVL by rationally constructing a series of metallic–acidic Ru x Pt y /MIL-101 catalysts comprising RuPt-alloyed nanoparticles (NPs) and Lewis-acid sites within a chromium-based MOF (namely MIL-101). Benefiting from the favorable synergy between Ru and Pt in their alloyed NPs and abundant Lewis-acid sites in MIL-101, the best Ru 4 Pt 1 /MIL-101 featuring an optimized Ru/Pt molar ratio of 4:1 shows a complete LA conversion with > 99.9 % yield of GVL under unprecedented ambient temperature and pressure, affording a high turnover frequency (TOF) of 1480.5h −1 , which is 15.1 and 10.1 times that of its monometallic Pt/MIL-101 (98.3 h −1 ) and Ru/MIL-101 (146.7 h −1 ) counterparts, respectively. Detailed experiments and density functional theory (DFT) calculations suggest the RuPt-alloyed effect and Lewis-acid sites in Ru 4 Pt 1 /MIL-101 can optimize the adsorption energy of 4-hydroxyvaleric acid (HPA) to remarkably boosting its catalytic performance for this reaction.
研究领域:
催化
·
绿色化学
·
可再生能源
·
材料科学
·
化学工程
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高影响因子
BIOMASS & BIOENERGY
·
2025
·
IF 5.8
Zonghui Liu,Xueting Zhu,Chao Cai,Jiayi Zheng,Bing Yan,Liangmin Ning,Dan Yang,Bing Xue
Developing conversion routes from lignocellulosic platform compounds to high-value chemicals is fundamental to advancing sustainable resource utilization in the bioeconomy. In this study, we designed a series of SBA-15-supported bifunctional catalysts with precisely tunable Lewis acid sites (LAS), Brønsted acid sites (BAS), and basic sites through strategic incorporation of hafnium species and heteropolyacids (HPAs), demonstrating their exceptional performance in the multi-step tandem conversion of furfural (FUR) to γ-valerolactone (GVL). HfO 2 was used LAS and basic sites to catalyze the transfer hydrogenation reaction of FUR and levulinate ester using 2-propanol as the H-donor. Complementary to this, HPA could catalyze the hydrolytic ring-opening of furans. The amount of LAS, BAS, and basic sites was adjusted by changing the ratio of HPA to HfO 2 and the types of HPA (phosphotungstic acid (HPW), phosphomolybdic acid (HPMo), silicotungstic acid (HSiW) and silicomolybdic acid (HSiMo)). The ratio of HPA to HfO 2 and types of HPA have a great influence on the catalytic performance, among which HPW/Hf-SBA-15_0.37 (W/Hf = 0.37) was identified as the best catalyst and presented the highest GVL selectivity (73.5 %) under optimized reaction conditions. The poison experiment (addition of benzoic acid, pyridine, or 2,6-lutidine to the reaction) indicated that both acidic and basic sites play important role in the FUR to GVL reaction. Moreover, by correlating the catalyst performance with the BAS/LAS ratio of catalysts, it can be found that the balance between the BAS and LAS is also the key to higher GVL selectivity.
研究领域:
催化
·
绿色化学
·
生物经济
·
材料科学
·
化学工程
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Tinghao Han,Zhongdi Liu,Lincai Peng,Weipeng Song,Huai Liu,Wenlong Jia,Rui Zhang
The efficient production of γ-valerolactone (GVL) with high yield directly from xylose is of particular interest but remains a great challenge due to the long reaction path. We herein developed a facile catalytic system to directly convert xylose to GVL with a record-high yield of 54.3 %, employing β-zeolite supported Zr-based catalyst in 1,4-dioxane/isopropanol co-solvent. Using Zr(NO 3 ) 4 ·5 H 2 O as the Zr sources resulting in well-retained β-zeolite structure, larger surface area and pore volume and better dispersion of Zr species, as well as balanced acidic sites where higher amount of Brønsted acid sites promoted the ring-opening of furfural alcohol for this cascade reaction. Notably, the introduction of 1,4-dioxane facilitated the in situ formation of furfural (i.e. yield-determining step) by diluting the competitive adsorption behavior between isopropanol and xylose, allowing more xylose molecules to access the active center, thus promoting the sequential production of GVL with unexpectedly high yield. The present work provides a efficient and straightforward preparation of GVL from xylose, paving the pathway towards higher atom economy.
研究领域:
催化
·
绿色化学
·
生物质转化
·
化学工程
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DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2025
·
IF 2.8
Yu-Xiang Jia,Lin Xie,Xiao-Guang Xu,Meng Wang
The nonsolvent induced phase separation (NIPS) method and its variants have garnered significant attention for the fabrication of ion-exchange membranes (IEMs) due to several potential advantages, including ease of scalability, reduced material requirements, and enhancements in operational performance. However, the hazards associated with traditional membrane fabrication solvents poses a considerable limitation to the advancement and application of NIPS. This study explores the use of a green solvent, specifically γ-valerolactone (GVL), for the first time in the preparation of IEMs via the NIPS technique. Initially, fundamental investigations, including thermodynamic and kinetic analyses of the casting solution composed of GVL and chloromethylated polysulfone (CMPS), as well as assessments of membrane morphology and electrochemical properties, are conducted to evaluate the feasibility of IEM production in comparison to the NMP/CMPS system. Additionally, some applied experiments, such as desalination by electrodialysis (ED) and acid recovery via diffusion dialysis (DD), are performed to examine the impacts of casting solution composition on the performances of the resulting membranes. The results from the ED experiments indicate that the membrane produced from a 19 w.% GVL/CMPS solution can achieve a 27% reduction in energy consumption while maintaining a comparable current efficiency to commercial membranes. Furthermore, the DD experiments reveal that this membrane exhibits a H + dialysis coefficient of 42 × 10 − 3 $$ 42\times {10}^{-3} $$ m/h and a separation factor of 256, significantly surpassing the performance metrics of commercial membranes. These findings clearly demonstrate that GVL is a viable green solvent for the preparation of polysulfone IEMs with highly competitive performance characteristics.
研究领域:
材料科学
·
环境工程
·
化学工程
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高影响因子
危险品化学品经营许可证（带存储）