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Mesoporous zeolites for biofuel upgrading and glycerol conversion

Jian Zhang, Liang Wang, Yanyan Ji, Fang Chen, Feng-Shou Xiao

《化学科学与工程前沿（英文）》 2018年第12卷第1期页码 132-144 doi: 10.1007/s11705-017-1681-8

摘要： With the recent emphasis and development of sustainable chemistry, the conversion of biomass feedstocks into alternative fuels and fine chemicals over various heterogeneous catalysts has received much attention. In particular, owing to their uniform micropores, strong acidity, and stable and rigid frameworks, zeolites as catalysts or co-catalysts have exhibited excellent catalytic performances in many reactions, including hydrodesulfurization, Fischer-Tropsch synthesis, and hydrodeoxygenation. However, the relatively small sizes of the zeolite micropores strongly limit the conversion of bulky biomolecules. To overcome this issue, mesoporous zeolites with pores larger than those of biomolecules have been synthesized. As expected, these mesoporous zeolites have outperformed conventional zeolites with improved activities, better selectivities, and longer catalyst lives for the upgrading of pyrolysis oils, the transformation of lipids into biofuels, and the conversion of glycerol into acrolein and aromatic compounds. This review briefly summarizes recent works on the rational synthesis of mesoporous zeolites and their superior catalytic properties in biomass conversion.

关键词： biomass conversion mesoporous zeolite sustainable chemistry

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Separation of 1,3-propanediol from glycerol-based fermentations of Klebsiella pneumoniae by alcohol precipitation

GAO Sujun, SUN Yaqin, XIU Zhilong

《化学科学与工程前沿（英文）》 2007年第1卷第2期页码 202-207 doi: 10.1007/s11705-007-0037-1

摘要： The separation of 1,3-propanediol from the glycerol-based fermentation broth of plays an important role during the microbial production of 1,3-propanediol. In this paper, the separation of 1,3-propanediol from fermentative broth by a combination of ultrafiltration and alcohol dilution crystallization was investigated. The broth was first filtered by ultrafiltration, and 99% of cells, 89.4% of proteins and 69% of nucleic acids were removed. The obtained broth was further condensed by vac uum distillation, and then alcohol was added. The macromolecular impurities, such as nucleic acids, polysaccharides and proteins, were precipitated, and inorganic and organic salts were crystallized. The optimal volume ratio of alcohol added to the condensed fermentation broth was determined to be 2:1. As a result, proteins, nucleic acids and electric conductivity decreased by 97.4%, 89.7% and 95.8%, respectively, compared with the fermentative broth. The influences of pH and water content in condensed broth on alcohol precipitation and dilution crystallization were also investigated. The experimen tal results indicated that alcohol precipitation and dilution crystallization was feasible and effective for the separation of 1,3-propanediol from actual fermentation broth.

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Thermodynamic analysis of steam reforming of glycerol for hydrogen production at atmospheric pressure

Ammaru Ismaila, Xueli Chen, Xin Gao, Xiaolei Fan

《化学科学与工程前沿（英文）》 2021年第15卷第1期页码 60-71 doi: 10.1007/s11705-020-1975-0

摘要： Thermodynamic chemical equilibrium analysis of steam reforming of glycerol (SRG) for selective hydrogen production was performed based on the Gibbs free energy minimisation method. The ideal SRG reaction (C H O +3H O→3CO +7H ) and a comprehensive set of side reactions during SRG are considered for the formation of a wide range of products. Specifically, this work focused on the analysis of formation of H CO , CO and CH in the gas phase and determination of the carbon free region in SRG under the conditions at atmospheric pressure, 600K–1100K and 1.013 × 10 –1.013 × 10 Pa with the steam-to-glycerol feed ratios (SGFR) of 1:5–10. The reaction conditions which favoured SRG for H production with minimum coke formation were identifies as: atmospheric pressure, temperatures of 900K–1050K and SGFR of 10:1. The influence of using the inert carrier gas (i.e., N ) in SRG was studied as well at atmospheric pressure. Although the presence of N in the stream decreased the partial pressure of reactants, it was beneficial to improve the equilibrium yield of H . Under both conditions of SRG (with/without inert gas), the CH production is minimised, and carbon formation was thermodynamically unfavoured at steam rich conditions of SGFR>5:1.

关键词： steam reforming of glycerol H₂ N₂ carbon deposition thermodynamic analysis Gibbs free energy minimisation

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Thermodynamic analysis of liquid phase in situ hydrogenation of glycerol for 1,3-propanediol synthesis

Kun OUYANG, Yu HUANG, Haoyi CHEN, Tao LI, Fahai CAO, Dingye FANG

《化学科学与工程前沿（英文）》 2011年第5卷第1期页码 67-73 doi: 10.1007/s11705-010-0541-6

摘要： Based on the combination of the glycerol aqueous-phase reforming (APR) and catalytic hydrogenation of glycerol, a novel reaction system of liquid phase in situ hydrogenation of glycerol for the synthesis of 1,3-propanediol is proposed, in which hydrogen is produced from glycerol aqueous-phase reforming in the same reactor. In this new system, the glycerol is the raw material of the aqueous-phase reforming reaction; the hydrogen generated from the APR of glycerol can be quickly transformed to the in situ hydrogenation of glycerol to produce 1,3-propanediol, which can improve the selectivity of hydrogen for the APR process of glycerol. Moreover, thermodynamic calculation of the coupling processes was carried out, and standard molar enthalpies and equilibrium constants of foregoing reactions were obtained. The above calculation results indicate that the combination process is feasible for 1,3-propanediol synthesis.

关键词： glycerol aqueous-phase reforming 1 3-propanediol in-situ reduction

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甘油诱导的鼠李糖脂增强伯克霍尔德菌属C3中二苯并噻吩的生物降解 Article

Camila A. Ortega Ramirez, Abraham Kwan, Qing X. Li

《工程（英文）》 2020年第6卷第5期页码 533-540 doi: 10.1016/j.eng.2020.01.006

摘要：

在高度城市化的地区，人为活动造成的污染损害了土地的完整性，减少了农业耕作的土壤利用率。二苯并噻吩（DBT）是一种城市地区常见的杂环芳香烃，常被用作污染物微生物转化研究的模型化合物。人体接触的可能性及其健康风险使DBT成为一种令人担忧的化学品，因此，需要对DBT进行环境管理。利用甘油刺激伯克霍尔德菌属C3（Burkholderia sp. C3），降解其中的DBT，内容涉及以下方面：①DBT的生物降解动力学；②细菌生长；③鼠李糖脂（RL）的生物合成；④RL分泌。在甘油与DBT最佳摩尔比的情况下，实验第1天，DBT的生物降解速率常数与单独使用DBT培养基相比提高了18倍，DBT的生物降解率提高了25％~30%。这种增长变化与细菌生长加快和RL生物合成反应的增强有关。蛋白质组学研究揭示了参与RL生物合成作用的上级和主要阶段的酶类。在增添了甘油和DBT的培养基中鉴定出了鼠李糖脂的同系物：Rha-C10-C10、Rha-Rha-C10-C10、Rha-Rha-C10-C12和Rha-Rha-C12-C12，然而，在不含甘油或添加了RL抑制剂的培养物中只鉴定出Rha-C12-C12。研究表明，甘油通过促进RL的合成和细菌的生长来促进DBT的生物降解。根据这些结果，值得进一步研究甘油对环境生物的刺激作用，以促进生物修复技术的发展和提高农业土壤的有效性。

关键词：生物降解生物修复生物表面活性剂生物转化甘油微生物代谢鼠李糖脂

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Adsorption of 1,3-propanediol from synthetic mixture using polymeric resin as adsorbents

W. LUERRUK, A. SHOTIPRUK, V. TANTAYAKOM, P. PRASITCHOKE, C. MUANGNAPOH

《化学科学与工程前沿（英文）》 2009年第3卷第1期页码 52-57 doi: 10.1007/s11705-009-0087-7

摘要： The aim of this work was to separate 1,3-PDO from a synthetic mixture using polymeric resins, Amberlite XAD-7 and XAD-16 resins. The equilibrium adsorption of 1,3-PDO onto two polymeric resins were investigated in binary and tertiary systems. Experimental results of binary component adsorption equilibrium indicated that the adsorption capacity ( ) of 1,3-PDO at 160 g/L onto XAD-7 and XAD-16 was 835.96 and 584.61 mg 1,3-PDO/g dry resin, respectively. The adsorption isotherms were closely predicted by the Langmuir-Freundlich model among the two isotherm model tested. The value of n of 1,3-PDO adsorbed on XAD-7 are much higher than those on XAD-16. This result suggested that XAD-7 resin has a higher affinity for the 1,3-PDO adsorption than XAD-16 resin. Moreover, the value of adsorption capacity of 1,3-PDO in the binary and tertiary component were compared at the same conditions. In the tertiary system, although the selectivity of 1,3-PDO from XAD-7 was approximately six times higher than XAD-16, the adsorption capacity of 1,3-PDO at 160 g/L onto XAD-16 was higher than XAD-7. Interestingly, the reusability of XAD-7 and XAD-16 resins in the three cycle times shows a slight loss of adsorption capacity. Furthermore, the investigation about desorption by an ethanol/water mixture at 50% ( / ) indicated that the desorption yield of 1,3-PDO from XAD-7 was lower than XAD-16 resin for both the binary and tertiary component. This was due to the more favorable adsorption characteristics of XAD-7 resin than XAD-16 resin.

关键词： adsorption 1 3-propanediol glycerol polymeric resin adsorption isotherm