ENERGY & FUELS
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2019
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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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高影响因子
GREEN CHEMISTRY
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2019
·Vol. 21
·期 5
·1075-1079
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IF 9.405
Yong Ni,Zhihao Bi,Hui Su,Lifeng Yan
Efficient conversion of furfural to valuable chemicals is attracting attention because it is one of the bulk feedstocks in biomass refinery. Maleic acid (MA) and fumaric acid (FA) are two types of bulk monomers that can be prepared from furfural. Here, a simple method was developed to oxidize furfural to both MA and FA in a green deep eutectic solvent (DES). DES contained oxalic acid and choline chloride (ChCl); oxalic acid worked as both the main content of the solvent and acidic catalyst for the conversion. It was found that the conversion of furfural could reach 100%, while the yield of MA and FA reached 95.7% under a mild reaction temperature of 50 °C, which provided a green and efficient route for the synthesis of valuable monomers from furfural.
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高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2019
·Vol. 94
·期 10
·3093-3101
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IF 2.659
Jiaming Wu,Yuewen Shao,Guojian Jing,Zhanming Zhang,Zhengmao Ye,Xun Hu
Background Graphene oxide (GO) has abundant oxygen-containing functionalities such as hydroxyl groups and carboxyl groups with distinct acidities. This feature makes GO a potential solid acid catalyst for the acid-catalyzed reactions such as the production of ethyl levulinate (EL), a platform chemical, from the acid-treatment of furfuryl alcohol (FA). The structure and functionalities of GO are closely related to its catalytic performance, and thus it is necessary to establish the relationship between the chemical structure and the catalytic properties of GO. To achieve this aim, in this work, the GO catalysts were designed by a facile one-pot synthetic route with no subsequent modification. By controlling the parameters of oxidation process in preparation, multiple functional groups were immobilized onto graphitic substrate, significantly impacting the catalytic activity of GO in the conversion of FA to EL in an ethanol (EtOH) medium. Results The results showed that, the oxidation process significantly influenced the distribution of oxygen-containing functionalities on the surface of GO. The amount of the oxygen-containing functionalities can be adjusted by the oxidation parameters such as oxidizing agent equivalent, reaction time and temperature, while the organosulfate can only be remained at a moderate oxidation temperature. The existence of the synergistic effect between the oxygen-containing functionalities and the organosulfate functionalities promoted the catalytic activity of GO for the acid-catalyzed conversion of FA to EL. Conclusions This work provides a new strategy of design and development of functional graphene-based catalysts for the acid-catalyzed reactions, and lays foundation of the practicability of GO in biomass conversion. © 2019 Society of Chemical Industry
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
Xian Zhang,Miaomiao Han,Guoqiang Liu,Guozhong Wang,Yunxia Zhang,Haimin Zhang,Huijun Zhao
We successfully synthesize Cu 3 P nanosheets and granular Ni 2 P nanocrystals on the surface of commercial carbon fiber cloth (CFC) (Cu 3 P/CFC and Ni 2 P/CFC) respectively by a vapor-phase hydrothermal route. The as-synthesized Ni 2 P/CFC and Cu 3 P/CFC as electrodes all show the bifunctional electrocatalytic performances towards hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER), simultaneously all demonstrating the electrocatalytic activities of the furfural hydrogenation reaction (FHR) and furfural oxidation reaction (FOR) in alkaline media. Comparatively, the Cu 3 P/CFC exhibits higher FHR activity with almost ∼100% selectivity of the furfuryl alcohol (FAL) product and high Faradaic efficiency (FE) of 92.0%–98.0% over the applied potential range of −0.05 to −0.55 V ( vs . RHE), while the Ni 2 P/CFC indicates higher FOR activity with almost ∼100% selectivity of furoic acid (FA) product and FE of 90.0%–98.0% at the applied potential of 1.2–1.7 V ( vs . RHE) in alkaline electrolyte containing 50 mM furfural. The DFT calculations results reveal that the (1–10) dominated Cu 3 P can obtain higher hydrogen coverage but restricted H 2 desorption compared to the (001) dominated Ni 2 P, therefore the adsorbed active hydrogen (H) atoms from water can be effectively used for the FHR process, resulting in high FE and current density. The superior FOR activity of the Ni 2 P/CFC is mainly stemmed from the formed high valence state Ni species during electrocatalysis. Thanks to the superior FHR performance of Cu 3 P/CFC and FOR activity of Ni 2 P/CFC, a two-electrode H-type electrocatalysis system assembled with the Cu 3 P/CFC as cathode and Ni 2 P/CFC as anode can be constructed for simultaneously electrocatalytic production of FAL and FA with almost ∼100% selectivity in 1.0 M KOH electrolyte containing 50 mM furfural in each chamber under the given experimental conditions, demonstrating high FE of 97%–99%.
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2017
·
IF 4.339
Lujie Liu,Hui Lou,Min Chen
Nano-Pt and Nano-Pd particles were introduced to modified multiwalled carbon nanotubes via co-impregnation method for hydrogenation of furfural in liquid phase using ethanol as a solvent. Different transition metal (Cr, Mn, Fe, Co, Ni) was used as promoters using Pt/MWNT and Pd/MWNT catalysts and various supports were also compared to further investigate the hydrogenation process of furfural. Among the catalysts investigated, Pt–Fe/MWNT (Pt: 0.5 wt%) showed highest conversion and selectivity to furfuryl alcohol (yield of 87.4%), while Pd–Ni/MWNT (Pd: 0.5 wt%) catalysts exhibited the best catalytic performance (83.3% yield of tetrahydrofurfuryl alcohol) under the optimized conditions of 30 bar hydrogen and 5 h, at 100 and 130 °C, respectively. Synergistic effect of bimetallic catalysts has been utilized to improve catalytic activity and stability. The extremely active for the selective hydrogenation of furfural over Pt–Fe/MWNT and Pd–Ni/MWNT catalyst might be attributed to active crystal planes exposed over Pt and Pd promoted by Fe and Ni. Catalysts have shown stable activity and selectivity after 5 cycles using Pt–Fe/MWNT and Pd–Ni/MWNT catalysts. Moreover, we suggest that acid sites of conventional supports might have an impact on furfural conversion.
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高影响因子
CATALYSIS LETTERS
·
2017
·Vol. 147
·期 4
·953-963
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IF 2.799
Wu Chunyan,Yuan Wenwen,Huang Yi,Xia Yongmei,Yang Huamei,Wang Haijun,Liu Xiang
Abstract A novel heterogeneous catalyst was prepared by immobilizing bifunctional acidic ionic liquid of metal Al substituted (BAIL-Al) onto the surface of magnetic γ-Al 2 O 3 , and characterized by FT-IR, TG, XRD, BET, XPS, VSM, SEM and TEM. The catalytic activity of the prepared solid catalyst was investigated for the conversion of xylose to furfural. On the basis, the effects of temperature, time, amount of catalyst and solvent were studied on the yield of furfural. A furfural yield of 67.5% with 97.3% xylose conversion was obtained from xylose using Fe 3 O 4 @Al 2 O 3 -(BAIL-Al) as the catalyst in DMSO at 140 °C for 3 h. The immobilized catalyst has the features of easily separation and recycling as well as good thermal stability. Thus, the immobilized catalyst can be efficiently and easily recycled at least five times without apparent loss of activity in xylose conversion and furfural yield. Graphical Abstract A novel heterogeneous catalyst was prepared by immobilized bifunctional acidic ionic liquid (BAIL-Al) onto the surface of magnetic γ-Al 2 O 3 , possessing unique physicochemical properties and excellent catalytic activity for xylose transformation have been developed.
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高影响因子
RSC Advances
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2017
·Vol. 7
·期 48
·29916-29924
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IF 3.108
Yuanshuai Zhu,Wenzhi Li,Yijuan Lu,Tingwei Zhang,Hasan Jameel,Hou-min Chang,Longlong Ma
A resorcinol-formaldehyde resin carbon (RFC) catalyst with a well-developed, ordered, mesoporous framework was prepared using a soft template method at room temperature. The carbon was sulfonated in water using sulfanilic acid under mild atmospheric conditions. The sulfonated RFC (S-RFC) was characterized by N2 adsorption–desorption, elemental analysis, TEM, XPS, and FT-IR. It was determined that S-RFC is an efficient solid acid catalyst for furfural production from xylose and corn stover in γ-valerolactone (GVL). The effects of reaction time, reaction temperature, catalyst loading, substrate dosage and water concentration were investigated. 80% furfural yield and 100% xylose conversion were obtained from xylose at 170 °C in 15 min with 0.5 g catalyst. Comparatively, 68.6% furfural yield was achieved from corn stover at 200 °C in 100 min when using 0.6 g catalyst. Since there was no discernable decrease in furfural yield after multiple conversions utilizing the same catalyst, the recyclability of the catalyst is considered good.
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高影响因子
BIORESOURCE TECHNOLOGY
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2024
·
IF 9.7
Huanhuan Zhang,Liutao Hou,Weihong Zhang,Yucheng Lin,Xueli Liu,Shiqiang Zhao,Chun Chang
The purpose of this study is to design and investigate two coupling processes for acid-catalyzed hydrolysis of corncob, achieving the simultaneous preparation of biomass-based furfural and levulinic acid (LA). Meanwhile, high concentration and yield of LA were obtained through a situ feeding strategy of pretreated furfural residue with high solids loading (20%, w/v). In Scenario A, 2-methyltetrahydrofuran was selected as the solvent for the LA extraction process compared with the neutralization process in Scenario B. Techno-economic assessment results show that Scenario A is technically feasible and cost-competitive, with an internal rate of return of 21.92%, a net present value of 121 million US dollars, a carbon efficiency of 72%, an environmental factor of 4.38, and a process mass intensity of 32.19. This study will provide new insights for fully utilizing lignocellulosic biomass to prepare renewable energy resources, comprehensively evaluating the economic feasibility, and promoting green and low-carbon development.
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PubMed
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
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2024
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IF 5.6
Jiarong Qiu,Yi Liu,Jingwen Zhang,Ben Zhou,Qiyue Yang,Liangqing Zhang,Jianfeng Chen,Bingshu Wang,Lu Lin,Xianhai Zeng
A series of zirconium phosphate (ZrP) loaded H-beta-25 zeolite (i.e., ZrP@HB) multifunctional composite catalysts were synthesized by a simple co-precipitation method, and the one-pot upgrading for the transfer hydrogenation of furfural to γ-valerolactone (GVL) was systematically investigated through various characterizations and catalytic evaluation experiments. Comparative characterization analysis of the ZrP@HB-X(Y) catalysts showed that the ZrP@HB-4(4) catalyst has uniform distribution of elements, exhibiting a large specific surface area and hierarchical mesoporous/microporous structure. Fourier transform infrared spectroscopy of pyridine (Py-FTIR) and NH 3 temperature-programmed desorption characterizations indicated the presence of Lewis and Brønsted acid sites, as well as weak, moderate, and strong acid sites in the ZrP@HB-4(4) catalyst. It was confirmed by X-ray photoelectron spectroscopy and FTIR that the main reason for Lewis and Brønsted acid sites formation is the presence of P-O-Zr, P-O-H, and HB zeolite on the ZrP@HB-4(4) catalyst. The HB zeolite as well as Zr and P ratio, can be easily adjusted to efficiently regulate the acidity strength and Lewis and Brønsted acid sites of the ZrP@HB-X(Y) catalysts. The catalytic experiments demonstrated that the physicochemical properties of the ZrP@HB-4(4) catalyst mentioned above significantly enhance the GVL production. Notably, Lewis and Brønsted acid sites as well as transition metal sites of Zr in the ZrP@HB-4(4) catalyst were identified as the main factors that enhance the yield of the target product. By optimizing the reaction conditions, the yield of GVL could be as high as 88.16%. Reusability experiments demonstrate that the ZrP@HB-4(4) catalyst possesses excellent stability. Using levulinic acid as the substrate, the yield of GVL reached 93.92%, suggesting its potential versatility.
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2024
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IF 4.7
Shifang Cheng,Junfang Ding,Yakai Chen,Ganen Pan,Xinya Feng,Xingliang Xu,Jing Xu
Catalytic furfural (FF) into high value-added furfuryl alcohol (FOL) is a very important biomass improvement process and remains a challenging task. Herein, a series of Co-based composite oxide (CoMgAl-LDO) catalysts with highly dispersed Co 3 O 4 -based spinel oxide nanoparticles were synthesized by the topological transformation of Co-based ternary layered hydroxides (CoMgAl-LDH) under calcination conditions and tested for catalytic transfer hydrogenation of FF to FOL using isopropanol (2-PrOH) as hydrogen donor. The CoMgAl-LDO, especially Co 1.5 Mg 1.5 Al 1 -LDO calcinated at 500 °C (Co 1.5 Mg 1.5 Al 1 -LDO-500) offered the outstanding catalytic performance for the catalytic transfer hydrogenation of FF to FOL (99.7 % FF conversion and 95.9 % FOL selectivity), which was attributed to effectively dispersed active sites, abundant acid-base sites and mesoporous structure. Additionally, the Co 1.5 Mg 1.5 Al 1 -LDO-500 catalyst manifested good stability with wider universality to other carbonyl compounds, making the catalytic system extremely economical and practical in various biomass hydrogenation processes.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2025
·
IF 2.5
Chenghu Zhang,Zezhou Xing,Ying Li,Tong Xu,Yinghui Sun,Jie Bai
Utilizing metal alloying strategies to fully exploit the role of precious metals in upgrading biomass chemicals remains both a challenging task and a key sustainable strategy. To improve the hydrogen transfer efficiency of furfural molecules in the catalytic transfer hydrogenation pathway, we report a Pd–Cu alloy composite nanocatalyst supported on mesoporous-structured zirconia through electrospinning technology. The chemical states of Pd and Cu in the catalyst were studied using XRD, HRTEM and XPS characterization methods, proving the presence of the PdCu alloy. A series of synthesized monometallic and bimetallic catalysts were tested for their ability to catalyze the catalytic transfer hydrogenation of furfural. Results showed that the PdCu alloy catalyst exhibited excellent performance similar to that of the monometallic Pd catalyst. 95.6% furfural conversion and 91.5% furfuryl alcohol selectivity were achieved at 170 °C and 2 MPa N2 for 12 h, and the catalytic activity did not decrease significantly after 6 cycles. The excellent catalytic activity was mainly attributed to the alloy and solvent effects, which promoted the improvement in hydrogen transfer efficiency.
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高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Huabin Lian,Riming Hu,Lin Zheng,Daowei Gao,Shuai Wang,Rongyao Wang,Bin Wang,Guozhu Chen
The electrocatalytic reduction of biomass-derived furfural represents a sustainable pathway for the production of furfuryl alcohol and 2-methylfuran, serving respectively as value-added chemicals and biofuels. However, the production of these high-value-added products under mild conditions is hampered by low Faradaic efficiency. In this study, we develop a strategy to establish strong metal-support interactions, enabling Cu/NC (nitrogen-doped carbon) catalysts to efficiently produce value-added products under mild conditions. Specifically, we prepare a cost-effective NC support with highly dispersed ultrafine nano-Cu particles of approximately 1 nm in diameter. Under mild pH conditions, our comparative experiments show that the Faradaic efficiency for value-added products (furfuryl alcohol and 2-methylfuran) is nearly four times higher than that of commercial foam copper. We elucidate the influence of nitrogen-doped supports on the behavior of the supported metal Cu. Comprehensive in-situ infrared reflection absorption spectroscopy characterization and DFT theoretical calculations reveal a positive shift in the d-band center of the Cu 3d orbitals. This shift enhances the adsorption of furfural C1=O1 bonds on the Cu/NC catalyst and improves its capacity to bind active hydrogen, thereby increasing the Faradaic efficiency of the value-added products. Our findings advance theoretical understanding and providing practical insights for electrocatalytic hydrogenation of furfural under mild pH conditions.
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