Reaction Kinetics Mechanisms and Catalysis
·
2022
·Vol. 135
·期 3
·1541-1552
·
IF 1.843
Zhang Zhenwei,Ma Xiaoshi,Yue Chuanjun,Wei Xuejiao,Liu Baoliang
Furfuryl ethyl ether (FEE), an important gasoline additive, is synthesized by a one-step reductive etherification of furfural (FF) by Nb 2 O 5 nanowires loaded with Pd as catalysts. Compared with other materials, the catalyst had a suitable synergistic effect between the reductive sites Pd 0 and the acidic sites of Nb 2 O 5 nanowires, effectively improving the yield of FEE. In ethanol, at 453 K and under 1 MPa H 2 pressure, the catalyst 1.0 wt% Pd/Nb 2 O 5 showed excellent catalytic performance in the reductive etherification reaction, and the yield of FEE reached 87.7%, higher than Pd/C whose yield was 81%. This result showed a feasible way to simplify the FEE preparation process, thus reducing production costs.
研究领域:
催化化学
·
绿色化学
·
纳米材料化学
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能源化工
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有机合成
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DOI
高影响因子
ACS Catalysis
·
2017
·
IF 10.614
Chengtao Wang,Zhiqiang Liu,Liang Wang,Xue Dong,Jian Zhang,Guoxiong Wang,Shichao Han,Xiangju Meng,Anmin Zheng,Feng-Shou Xiao
The metal-catalyzed selective hydrogenation of biomass-derived molecules is in great demand but is challenging due to the complex reaction pathways. Herein, we report a persuasive example for achieving selective hydrogenation of furfural over Pd catalysts by controllable sorption of molecules in zeolite micropores. The key to this success is fixation of Pd nanoparticles inside of silicalite-1 zeolite with controllable wettability (Pd@S-1-OH) by functionalizing silanol groups into the zeolite framework. In the hydrogenation of furfural as a model reaction, the Pd@S-1-OH catalyst with appropriate hydrophilicity exhibits extraordinary selectivity for the formation of furan, giving furan selectivity as high as >99.9% with a complete conversion of furfural, outperforming the conventional Pd nanoparticles supported on zeolite crystals (Pd/S-1) and S-1 zeolite fixed Pd catalysts without an artificially functionalized silanol group (Pd@S-1). The extraordinary performance of Pd@S-1-OH is reasonably attributed to the controllable diffusion of molecules within the hydrophilic zeolite micropores, which favors the adsorption of furfural and a series of byproducts but promotes the desorption of furan. Very importantly, Pd@S-1-OH is stable and gives the furan productivity of ∼583.3 g gPd–1 day–1 in a continuous test.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Jilei Xu,Lin Li,Guangyi Li,Aiqin Wang,Yu Cong,Xiaodong Wang,Ning Li
For the first time, proline-based ionic liquids were reported as effective catalysts for the aldol condensation of angelica lactone with furfural, two platform compounds which were obtained by the hydrolysis–dehydration reactions of cellulose and hemicellulose. Among the investigated catalysts, a renewable ionic liquid that was prepared with biomass-derived choline and l-proline (denoted as ChPro) demonstrated the highest activity. Over the ChPro catalyst, 86% carbon yield of C10 oxygenate was obtained under mild conditions (353 K, 1 h). After being hydrogenated over the Pd/C catalyst and hydrodeoxygenated under the promotion of the Pd–Cu/SiO2, the aldol condensation product of angelica lactone with furfural was transmuted into C8–C10 alkanes within the carbon chain range of jet fuel and diesel. Compared with the Cu/SiO2 and Pd/SiO2, the bimetallic Pd–Cu/SiO2 demonstrated higher activity and/or selectivity to C8–C10 alkanes for the hydrodeoxygenation of hydrogenated aldol condensation product. According to the characterizations of X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, and CO Fourier transform infrared, the excellent catalytic performance of Pd–Cu/SiO2 can be comprehended by the Pd–Cu alloy particles formed during the preparation of this catalyst.
研究领域:
生物质化学
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催化化学
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可再生能源
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 150
·期 12
·3505-3513
·
IF 2.482
Zhang Huifa,Geng Tong,Zhang Huixian,Cao Fahai
Abstract 5-Hydroxymethylfurfural (HMF) is mainly produced by dehydration of hexasaccharides which were limited by the source availability and low yield of the process. Accounting to this, the current study was thus designed to first identify the mesoporous niobium phosphate was a tailored catalyst and further to develop a suitable reaction system for hydroxymethylation of furfural to HMF. The mesoporous niobium phosphate was prepared by a two-step sol–gel hydrothermal method used to catalyze this hydroxymethylation reaction either in a pure water solvent or in an aqueous organic solvent system. Detailed investigation on reaction activity and HMF selectivity was carried out by varying reaction conditions. A highest HMF yield of 51.1% was obtained with a 79.2% furfural conversion under the aqueous dimethyl sulfoxide (DMSO) at 90 °C for 20 h over the current catalyst. Moreover, the mesoporous niobium phosphate could be recovered and reused at least for 6 runs without obvious loss in catalytic activity. Grpahic Abstract Mesoporous niobium phosphate was synthesized by a two-step sol–gel hydrothermal method and firstly investigated for the catalytic hydroxymethylation of furfural to HMF. The results suggest that mesoporous niobium phosphate shows a superior activity and selectivity. The highest yield of 51.1% of HMF was obtained with a 79.2% furfural conversion. The excellent catalytic performance could be attributed to attributed to the strong acid sites and larger porous structure in the catalyst.
研究领域:
化学工程
·
催化剂科学
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产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
·
2019
·Vol. 10
·期 2
·277-287
·
IF 2.326
Shi Ning,Liu Qiying,Cen Hu,Ju Rongmei,He Xiong,Ma Longlong
Humins are undesired solids formed during the hydrothermal degradation of carbohydrates. In order to reveal the mechanism of formation of humins, we studied the degradation behavior of 11 model compounds including carbohydrates and furfural derivatives, within water and various pure organic solvents as reaction media. All the studied carbohydrates could generate solid humins in both water and studied organic solvents except ethanol, while the furfural derivatives could generate solid humins in only water. The results could be explained by regarding the formed α-carbonyl aldehydes and α,β-unsaturated aldehydes as primary precursors for formation of humins. Furfural derivatives could generate chain α-carbonyl aldehydes (for example, 6-hydroxy-2,5-dioxohexanal from 5-hydroxymethylfurfural and 2-oxopentanedial from furfural) through hydrolytic ring opening reaction; thus, water is essential for these furfural derivatives to generate humins. As for carbohydrates, they could generate α-carbonyl aldehydes and α,β-unsaturated aldehydes through simple step of β-elimination in all solvents; thus, they could form humins in both water and studied organic solvents except ethanol. Ethanol could react with α-carbonyl aldehydes by acetalization; thus, the condensation between α-carbonyl aldehydes was suppressed in ethanol, leading to few humins formation from carbohydrates. Based on the above analysis, we proposed that the formed α-carbonyl aldehydes and α,β-unsaturated aldehydes should be the primary precursor of humins.
研究领域:
生物化学
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能源化学
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产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
·
2021
·Vol. 13
·期 9
·8115-8121
·
IF 4.987
Ren Dezhang,Jiang Xuelei,Zhang Nahui,Duo Jia,Norinaga Koyo,Huo Zhibao
Production of pyridine derivatives from bio-based feedstocks instead of fossil fuels is a promising strategy. The development of effective heterogeneous catalysts and mild reaction systems for pyridinization of renewable biomass derivatives remains a huge challenge. In this article, a direct and environment-friendly method was reported to produce 3-hydroxypyridine from bio-based furfural in water over a Raney Fe catalyst. Raney Fe exhibited an efficient catalytic performance for activation of the aldehyde group of furfural and afforded an 18.2% yield of 3-hydroxypyridine at 120 °C with ammonia as N source. The polymerization of furfural on the catalyst in hot water was the main cause of deactivation, which was verified by the scanning electron microscope (SEM), X-ray diffraction (XRD), and N 2 adsorption and desorption analysis. A possible mechanism for this reaction was also proposed. This study provides a new way for academia and industry to realize the synthesis of nitrogen-containing chemicals from biomass and its derivatives.
研究领域:
催化化学
·
绿色化学
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可再生资源转化
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
·
IF 5.107
Yinhua Yang,Zhihao Si,Di Cai,Xingning Teng,Guozhen Li,Ze Wang,Shufeng Li,Peiyong Qin
A high hydrophobicity of membrane plays a vital role in separating organics from dilute solution by pervaporation, which highly contributes to the increase of organics selectivity. Herein, we chose the high-hydrophobic poly[(3,3,3-trifluoropropyl)methylsiloxane] (PTFPMS) material to prepare the pervaporation membrane using a green method for the first time. Within the PTFPMS membrane, the -Si-O- chains imply the hydrophobic nature, and introducing CF 3 groups further enhances the hydrophobicity. The high-efficiency transport pathways are formed in which water will experience a larger diffusion resistance within PTFPMS membrane compared with the conventional polydimethylsiloxane (PDMS) membrane without CF 3 groups. Moreover, considering the great threat of organic solvent to the environment and operators during membrane preparation, a green approach using water instead of organic solvent was employed. Especially, when separating 1 wt% furfural aqueous solution at 80 ℃, there are 30% of increase in the furfural separation factor (45.6) and an effective increase in furfural flux (328 g m −2 h −1 ) compared with those of PDMS membrane. Overall, the super-hydrophobic PTFPMS membrane highly improves the feasibility of the downstream processes for recovering the biomass derives furfural.
研究领域:
材料科学
·
环境工程
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产品关联
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2014
·
IF 5.039
Huiling Li,Aojie Deng,Junli Ren,Changyu Liu,Qi Lu,Linjie Zhong,Feng Peng,Runcang Sun
Selectively catalytic hydrothermal pretreatment of corncob into xylose and furfural has been developed in this work using solid acid catalyst ( SO 4 2 - /TiO 2 –ZrO 2 /La 3+ ). The effects of corncob-to-water ratio, reaction temperature and residence time on the performance of catalytic hydrothermal pretreatment were investigated. Results showed that the solid residues contained mainly lignin and cellulose, which was indicative of the efficient removal of hemicelluloses from corncob by hydrothermal method. The prepared catalyst with high thermal stability and strong acid sites originated from the acid functional groups was confirmed to contribute to the hydrolysis of polysaccharides into monosaccharides followed by dehydration into furfural. Highest furfural yield (6.18 g/100 g) could be obtained at 180 °C for 120 min with 6.80 g/100 g xylose yield when the corncob/water ratio of was 10:100. Therefore, selectively catalytic hydrothermal pretreatment of lignocellulosic biomass into important platform chemicals by solid acids is considered to be a potential treatment for biodiesel and chemical production.
研究领域:
生物化学
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可再生资源与环境工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysts
·
2023
·Vol. 13
·期 4
·663
·
IF 3.9
Xu Wu,Heqin Guo,Litao Jia,Yong Xiao,Bo Hou,Debao Li
The base-free oxidation of furfural by non-noble metal systems has been challenging. Although MnO2emerges as a potential catalyst application in base-free conditions, its catalytic efficiency still needs to be improved. The crystalline form of MnO2is an important factor affecting the oxidation ability of furfural. For this reason, four crystalline forms of MnO2(α, β, γ, and δ-MnO2) were selected. Their oxidation performance and surface functional groups were analyzed and compared in detail. Only δ-MnO2exhibited excellent activity, achieving 99.04% furfural conversion and 100% Propo.FA(Only furoic acid was detected by HPLC in the product) under base-free conditions, while the furfural conversion of α, β, and γ-MnO2was below 10%. Characterization by XPS, IR, O2-TPD and other means revealed that δ-MnO2has the most abundant active oxygen species and surface hydroxyl groups, which are responsible for the best performance of δ-MnO2. This work achieves the green and efficient oxidation of furfural to furoic acid over non-noble metal catalysts.Keywords:base-free;MnO2;crystal type;furfural oxidation to furoic acid
研究领域:
催化化学
·
绿色化学
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产品关联
DOI
高影响因子
Green Energy & Environment
·
2018
·
IF 0
Wei Hui,Yan Zhou,Yan Dong,Zhi-Jun Cao,Fei-Qiang He,Min-Zhong Cai,Duan-Jian Tao
Novel superacid SO 4 H-functionalized ionic liquids (SFILs) were designed and prepared in this work. The catalytic activities of SFILs were evaluated in xylan hydrolysis and xylose dehydration to produce furfural. Combined with the results of acid strength of SFILs characterized by solid-state 31 P MAS NMR, it was found that the catalytic performance of SFILs was positively correlated to their acid strength. The superacid SFIL [Ch-SO 4 H][CF 3 SO 3 ] displayed the best catalytic performance with more than 80% yield of furfural, and it was also obviously superior to usual SO 3 H-functionalized acidic ILs, mineral liquid acids, and acidic resin Amberlyst-15 catalysts in catalytic activity under optimized conditions. In addition, the superacid SFIL [Ch-SO 4 H][CF 3 SO 3 ] could be easily separated from reaction system and reused at least five times without obvious decrease.
研究领域:
化学工程
·
催化
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绿色化学
·
可再生能源
✓ 已验证
产品关联
DOI
RSC Advances
·
2018
·Vol. 8
·期 43
·24534-24540
·
IF 2.936
Jin Tan,Haiyong Wang,Longlong Ma,Chenguang Wang,Qiying Liu,Qi Zhang,Minghong He
Several simple and effective solvents combined with Hβ zeolite were tested to selectively convert glucose into furfural and hydroxymethylfurfural in this work. The physicochemical properties of typically different polar aprotic solvents were compared. Tetrahydrofuran was found to be a suitable solvent in the selective conversion of glucose. The effect of reaction parameters, such as temperature, reaction time, water content, glucose dosage and protonic acid addition, on the product distribution were investigated in detail. Furfural and hydroxymethylfurfural could be selectively produced in this system, and the highest yields of furfural and hydroxymethylfurfural were up to 35.2% and 49.7% respectively. Furfural could be stable in a tetrahydrofuran medium when adding 5 wt% water in the absence of extra protonic acid. However, furfural production was extremely suppressed after addition of an acidic inorganic salt, which increased the yield of hydroxymethylfurfural. This investigation indicates a simple and feasible method to selectively produce furfural and hydroxymethylfurfural from renewable cellulosic carbohydrates.
研究领域:
化学工程
·
可再生资源转化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Qian Yao,Lujiang Xu,Zheng Han,Ying Zhang
Furfural, an abundant biomass derived compound, was converted into indoles via thermo-catalytic conversion and ammonization with zeolites. The effect of reaction temperature, catalyst, weight hourly space velocity (WHSV) and ammonia to furfural molar ratio on the product distribution was investigated systematically. They all played important roles on indoles production. The maximal carbon yield of indoles (20.79%) was achieved by using HZSM-5 (Si/Al = 25) catalyst at 650 °C with WHSV as 1.0 h −1 and NH 3 to furfural molar ratio as 2. The HZSM-5 (Si/Al = 25) catalyst was recycled for five times and showed slight deactivation. Three possible aldehyde group of furfural conversion pathways were proposed and one possible reaction pathway from furfural to indoles was verified based on the experimental and quantum calculation results, that is, furfural firstly reacted with ammonia to form furfural-imine, and then furfural-imine underwent a cracking reaction to form furan. Thereafter, furan was converted to pyrrole and finally to indoles.
研究领域:
生物化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）