Molecular Catalysis
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2017
·
IF 0
Hao Chen,Houhang Ruan,Xilei Lu,Jie Fu,Timothy Langrish,Xiuyang Lu
Catalytic transfer hydrogenation of furfural to furfuryl alcohol is considered to be a very important industrial process. In this work, non-noble Cu supported on MgO-Al 2 O 3 catalysts have been prepared by co-precipitation and have shown excellent catalytic performance for conversion of furfural to furfuryl alcohol in near-critical iso-propanol. The effects of the Cu state (reduction degree and dispersion) and loading in Cu/MgO-Al 2 O 3 , acidity of catalysts have been investigated by X-ray diffraction (XRD), coupled plasma optical emission spectrometry (ICP-OES), N 2 adsorption and desorption (N 2 -BET) and temperature-programmed desorption of ammonia (NH 3 -TPD), which have led to high activity for producing furfuryl alcohol. The results have shown that the selectivity of furfuryl alcohol has been influenced by the Cu state, Lewis acidity, reaction temperature and reaction time. The mechanisms, Lewis acid- and metal mediated hydrogenation, have shown that a desirable balance of Cu loading and Lewis acidity of catalyst has influenced the activity significantly. Almost 100% furfural conversion, with 89.3% furfuryl alcohol yield has been obtained. Cycling tests have shown that the prepared catalysts have been stable, where recycling the catalysts at least four times has not shown any reduction in activity.
研究领域:
化学工程
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催化材料
✓ 已验证
DOI
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yue Wang,Xiangyan He,Qi Zhang,Ling Luo,Tianping Lv,Xiuwu Wang,Junhua Zhang
Construction of highly efficient catalysts is crucial for the catalytic transfer hydrogenation (CTH) of bio-based carbonyls to valuable chemicals and fuels. Herein, we successfully synthesized a series of uniformly dispersed Zr(OH) 4 -Fe 3 O 4 nanoparticles with the regulation of sodium dodecyl benzene sulfonate (SDBS), which exhibited exceptional activity for the CTH of furfural (FAL) into furfuryl alcohol (FOL). Systematic characterizations revealed that SDBS effectively modified the interaction between Fe 3 O 4 and Zr(OH) 4 , thereby enhancing Lewis acidity by facilitating the construction of electron-deficient zirconium sites. Meanwhile, the presence of oxygen vacancies and surface hydroxyl groups in Zr(OH) 4 -Fe 3 O 4 -SDBS facilitated the adsorption and activation of both substrate and hydrogen donor. Thanks to these synergistic effects, a complete conversion of FAL with an impressive selectivity towards FOL was achieved, with a remarkable turn-over frequency value reaching as high as 42.5 h −1 . Encouragingly, Zr(OH) 4 -Fe 3 O 4 -SDBS also demonstrated its universality in the CTH of carbonyl compounds by exhibiting remarkable separation capability while maintaining its activity and structure after being reused for 11 cycles without significant changes.
研究领域:
化学工程
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材料科学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
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IF 7.4
Xiaoxian Li,Min Lin,Rui Li,Mingde Yang,Yulong Wu
Algal bio-oil obtained from hydrothermal liquefaction of algae contains a large amount of water and long-chain fatty acids. High acidity and corrosiveness seriously restrict the application of algal bio-oil. The aqueous-phase catalytic upgrading was a promising approach to solve this problem, and the hydrogen donor was one of the most important parameters to the conversion of the algal bio-oil and the quality of the products. Catalytic transfer hydrogenation (CTH) reaction was an efficient, economical and green method for hydrogenation reaction, which can directly transfer hydrogen from the hydrogen donor to the reaction substrate. In this work, the CTH reaction of algal bio-oil model compound palmitic acid was investigated to deal with the problem of high oxygen content in the algal bio-oil. Several common hydrogen donors, included methanol, ethanol, formic acid, and isopropanol, as well as different reaction conditions were experimented to study the CTH process of palmitic acid. The results showed that, with the reaction conditions of 350 °C and 10 h, formic acid achieved the best oxygen removal, carbon retention and energy efficiency, the C 16 selectivity reached the highest at 33.3 % as the formic acid addition ratio was 1:2, and the C 15 selectivity reached the highest at 48.3 % as the formic acid addition ratio was 1:3. In general, the best ratio of formic acid added was 1:3, which showed the highest yield of C 15 and above alkanes of 79.6 %. This result indicates that the catalytic transfer hydrogenation reaction of formic acid has practical value in improving the combustion performance of algal bio-oil.
研究领域:
化学工程
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Changzhou Chen,Xialin Ji,Yongzhi Xiong,Jianchun Jiang
Exploring an advanced catalytic strategy for the high value utilization of lignin derived chemicals into value-added aromatics has attracted tremendous sights for green manufacturing. In this paper, a series of bifunctional 3D rod-shaped mesoporous NiCe metal–organic framework catalysts coupling with hydrogen-donner solvent were reported for the hydrodeoxygenation of vanillin to obtain 2-methoxy-4-methylphenol. Under the optimal conditions, 3Ni-Ce/C catalyst realized the highest conversion of vanillin (>95.0 %) and selectivity of 81.4 % in the absence of additional hydrogen pressure. The characterization results indicated that the interaction of metallic Ni and CeO 2 promoted the generation of Ni-CeO 2-x interface and oxygen vacancies (Ov), which could efficiently adsorb and activate aldehyde group of vanillin to obtain reactive intermediates. And then metallic Ni sites activated the hydrogen-donner solvent to form adsorbed H atoms, which then spilled over to the adjacent Ov to stabilized reactive intermediates. Whereafter, bifunctional 3D rod-shaped mesoporous NiCe metal–organic framework catalysts achieved the hydrodeoxygenation upgrading of vanillin to obtain 2-methoxy-4-methylphenol. Density functional theory (DFT) calculations further revealed that the synergistic effect of Ni-CeO 2 and oxygen vacancies promoted the activation and dissociation of aldehyde group bond in vanillin, enhanced the ability of protonation hydrogenolysis. Additionally, 3Ni-Ce/C catalyst displayed robust activity for no less than four recycles, which provided a feasible method for the build of simultaneous utilization of lignin derivates to value-added fuels and chemicals.
研究领域:
化学工程
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材料科学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2020
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IF 5.006
Mo Qiu,Tianmeng Guo,Ran Xi,Danni Li,Xinhua Qi
In this paper, the as-prepared metal-organic frameworks material UiO-66 and other Zr-MOFs were directly used as catalytic transfer hydrogenation (CTH) catalysts to catalyze furfural (FF) to furfuryl alcohol (FAL) with 2-propanol (IPA) acted as both solvent and hydrogen donor. The results showed that the as-prepared UiO-66 had satisfactory catalytic activity and selectivity in yielding FAL (97 %) from the CTH of FF at 140 °C within 5 h. Moreover, the as-prepared UiO-66 exhibited relatively stable catalytic activity over five cycles and easy regeneration. Interestingly, UiO-66 was also applicable for the CTH of the other aldehydes such as 5-hydroxymethyfurfural, 5-methylfurfural, 4-methoxybenzaldehyde, and n-hexanal to the corresponding alcohols, affording high product yields up to 98 %. This work provides a green, simple and sustainable process for the catalytic production of FAL from biomass-based furfural, which has certain significance for the sustainable utilization of biomass.
研究领域:
催化化学
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生物质能源
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绿色化学
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材料化学
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有机合成
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Yun Tian,Jie Qu,Kejia Wu,Mengqiao Gao,Jinxing Long,Qiang Zeng,Wei Qi,Xuehui Li
Conversion of lignin to value-added chemicals with endogenous hydrogen is of great significance but highly challengeable. In this work, an external hydrogen-free strategy has been proposed for aqueous transfer hydrogenolysis of lignin launched by the chemo-splitting of water using a series of Ni-Co bimetallic catalysts. With Ni 0.2 Co 0.1 -MgAl-LDO, 82.7 % of lignin conversion was achieved, affording a 20.8 % yield of monophenols, and 62.0 % of which was identified as 4-ethylphenol (yield of 12.9 %). Further investigations demonstrated that the lignin hydrogenolysis was triggered by the water splitting, and enhanced by the tandem demethoxylation and subsequent aqueous reforming reaction. Intensive characterizations using TEM, XPS and XAFS, etc, illustrated that the formation of highly dispersed Ni-Co alloy nanoparticles exhibited a strong metal-support interaction with MgAl-LDO. The electronic transfer effect between Ni and Co components and the strong basic sites are responsible for its excellent catalytic performance of Ni 0.2 Co 0.1 -MgAl-LDO on the lignin hydrogenolysis. Therefore, this work provides novel insight into the catalytic transfer hydrogenolysis of lignin.
研究领域:
催化化学
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生物质转化
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绿色能源
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有机反应工程
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材料化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2025
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IF 6.2
Hui Li,Peng Liu,Fei Ge,Wenlin Xu,Minghao Zhou
The catalytic transfer hydrodeoxygenation (CTHDO) technology of lignin-derived bio-oil is a very promising bio-oil conversion technology. However, the preparation of highly active and stable catalysts remains a major challenge. Carbon-coated metal nanoparticle catalysts can effectively solve the problems of catalyst deactivation and high-temperature metal leaching. In this work, a series of MOF-derived carbon-coated Co-based catalysts were designed via a simple solvothermal method using terephthalic acid as organic ligands, which were applied for the CTHDO reaction of guaiacol using isopropanol as H-donor. Among them, Co/C-2-500 had the best catalytic performance for the conversion of lignin-derived phenol to cyclohexanol. Under the optimal conditions of 180 °C, 0.5 MPa N 2 , and 3 h, the conversion rate of guaiacol can reach 100 %, and the yield of cyclohexanol can reach 96.8 %. Mechanism research showed that the phenol generated from the demethoxylation of guaiacol was a key intermediate, which further underwent the hydrogenation of aromatic ring to form cyclohexanol. Based on the various characterizations, it can be considered that the high catalytic activity was due to the synergistic effect of the metallic Co 0 active sites and the acid sites. This research could provide some insights for the catalytic transfer hydrodeoxygenation of lignin and its derivatives.
研究领域:
催化化学
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生物质转化
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化学工程
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纳米材料
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有机化学
✓ 已验证
产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
·
2022
·Vol. 13
·期 15
·13771-13783
·
IF 4.05
Li Xiaohua,Liu Tieyi,Shao Shanshan,Yan Jinlong,Zhang Hongchang,Cai Yixi
The catalytic transfer hydrogenation of biomass-derived furfural, butyraldehyde, and acetone was carried out over an inexpensive copper-based hydrotalcite-like catalyst using methanol as both hydrogen donor and solvent. X-ray photoelectron spectroscopy (XPS) characterization was conducted to analyze copper valence state on the catalyst. The bivalent copper ion was reduced to monovalent and zero valent copper during the reaction. The transfer hydrogenation of furfural, butyraldehyde, and acetone was obviously promoted at higher temperature and longer duration. With regard to hydroprocessing, the yield of corresponding alcohol was greatly increased to 95.69 mol% (furfuryl alcohol), 97 mol% (butanol and methyl butanol), and 82.17 mol% (isopropanol) at 200 ℃ for 2.5 h, respectively, which indicated the superior catalytic transfer hydrogenation activity of copper-based catalyst. The reactions of different reactant were compared in this study. The highest yields of three target products were obtained at same time, which was mainly ascribed to the reduction rate of copper species. This study put forward a green, efficient hydrogenation reaction of biomass-derived oxygenated chemicals using an inexpensive copper-based catalyst and methanol system without any external hydrogen supply.
研究领域:
催化化学
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生物质转化
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绿色化学
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可再生能源
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多相催化
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）