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  • RESEARCH ARTICLE
    Huaping Lin, Likai Zhu, Ye Liu, Vasilevich Sergey Vladimirovich, Bilainu Oboirien, Yefeng Zhou
    Frontiers of Chemical Science and Engineering, 2024, 18(11): 125. https://doi.org/10.1007/s11705-024-2476-3

    Currently, the conversion of waste plastics into high-value products via catalytic pyrolysis enables the advancement of plastics’ open-loop recycling. However, enhancing selectivity remains a critical challenge. This study introduces a novel approach to catalytic pyrolysis, utilizing a combination of MCM-41 and modified gallium-based HZSM-5 catalysts, to achieve exceptional selectivity for aromatic liquid-phase products from linear low-density polyethylene. Firstly, to enhance the probability of dehydroaromatization optimization, the type and proportion of metal active sites within the HZSM-5 catalyst are fine-tuned, which would establish equilibrium with acid sites, resulting in a remarkable 15.72% increase in the selectivity of aromatic hydrocarbons. Secondly, to enhance the accessibility of volatiles to active sites, mesoporous MCM-41 with cracking capabilities is introduced. The doping ratio of MCM-41 is meticulously controlled to facilitate the diffusion of cracked volatiles to the active centers of modified gallium-based HZSM-5, enabling efficient reforming reactions. Experimental findings demonstrate that MCM-41 significantly enhances the dehydroaromatization activity of the modified gallium-based HZSM-5 catalyst. Under the influence of MCM-41:Zr2Ga3/HZSM-5 = 1:2 catalyst, the selectivity for aromatic hydrocarbons reaches an impressive 93.11%, with a notable 60.01% selectivity for benzene, toluene, ethylbenzene, and xylene. Lastly, this study proposes a plausible pathway for the generation of high-value aromatic hydrocarbons using the combined catalyst.

  • RESEARCH ARTICLE
    Shuo-Shuo Zhang, Xing-Bao Wang, Wen-Ying Li
    Frontiers of Chemical Science and Engineering, 2024, 18(11): 130. https://doi.org/10.1007/s11705-024-2482-5

    Separating monomeric cycloalkanes from naphtha obtained from direct coal liquefaction not only facilitates the valuable utilization of naphtha but also holds potential for addressing China’s domestic chemical feedstock market demand for these compounds. In extractive distillation processes of naphtha, relative volatility serves as a crucial parameter for extractant selection. However, determining relative volatility through conventional vapor-liquid equilibrium experiments for extractant selection proves challenging due to the complexity of naphtha’s compound composition. To address this challenge, a prediction model for the relative volatility of n-heptane/methylcyclohexane in various extractants has been developed using machine-learning quantitative structure-property relationship methods. The model enables rapid and cost-effective extractant selection. The statistical analysis of the model revealed favorable performance indicators, including a coefficient of determination of 0.88, cross-validation coefficient of 0.94, and root mean square error of 0.02. Factors such as α, EHOMO, ρ, and logPoct/water collectively influence relative volatility. Analysis of standardized coefficients in the multivariate linear regression equation identified density as the primary factor affecting the relative volatility of n-heptane/methylcyclohexane in the different extractants. Extractants with higher densities, devoid of branched chains, exhibited increased relative volatility compared to their counterparts with branched chains. Subsequently, the process of separating cycloalkane monomers from direct coal liquefaction products via extractive distillation was optimized using Aspen Plus software, achieving purities exceeding 0.99 and yields exceeding 0.90 for cyclohexane and methylcyclohexane monomers. Economic, energy consumption, and environmental assessments were conducted. Salicylic acid emerged as the most suitable extractant for purifying cycloalkanes in direct coal liquefaction naphtha due to its superior separation effectiveness, cost efficiency, and environmental benefits. The tower parameters of the simulated separation unit provide valuable insights for the design of actual industrial equipment.

  • RESEARCH ARTICLE
    Huiyu Fu, Jiewen Wu, Changhai Liang, Xiao Chen
    Frontiers of Chemical Science and Engineering, 2024, 18(11): 126. https://doi.org/10.1007/s11705-024-2477-2

    With the advantages of low raw material cost and 100% atom utilization, the synthesis of high value-added chemical product cyclic carbonates by the cycloaddition of CO2 to epoxides has become one of the most prospective approaches to achieve the industrial utilization of CO2. In the reported catalytic systems, the complexity of the catalyst synthesis process, high cost, separation difficulties, and low CO2 capture limit the catalytic efficiency and its large-scale application. In this paper, Ag nanoparticles loaded on polyethyleneimine (PEI)-modified UiO-66-NH2 (Ag/PEI@UiO-66-NH2) are successfully synthesized by in situ immersion reduction. The Ag nanoparticles and the amino groups on the surfaces of PEI@UiO-66-NH2 contribute to the adsorption of CO2 and polarization of C–O bonds in epoxides, thereby boosting the conversion capability for the CO2 cycloaddition reaction. At the amount of propylene oxide of 0.25 mol and the catalyst dosage of 1% of the substrate, the yield and selectivity of propylene carbonate are up to 99%. In addition, the stability and recyclability of Ag/PEI@UiO-66-NH2 catalyst are attained. The Ag/PEI@UiO-66-NH2 catalyst also demonstrates a wide range of activity and distinctive selectivity toward cyclo-carbonates in the cycloaddition of CO2 to epoxides. This work provides a guide to designing a highly efficient catalyst for in situ capture and high-value utilization of CO2 in industrial applications.

  • RESEARCH ARTICLE
    Muhammad Kashif, Faizan Ahmad, Weitao Cao, Wenke Zhao, Ehab Mostafa, Yaning Zhang
    Frontiers of Chemical Science and Engineering, 2024, 18(10): 115. https://doi.org/10.1007/s11705-024-2466-5

    Eucalyptus species are extensively cultivated trees commonly used for timber production, firewood, paper manufacturing, and essential nutrient extraction, while lacking consumption of the leaves increases soil acidity. The objective of this study was to recover bio-oil through microwave pyrolysis of eucalyptus camaldulensis leaves. The effects of microwave power (450, 550, 650, 750, and 850 W), pyrolysis temperature (500, 550, 600, 650, and 700 °C), and silicon carbide amount (10, 25, 40, 55, and 70 g) on the products yields and bio-oil constituents were investigated. The yields of bio-oil, gas, and residue varied within the ranges of 19.8–39.25, 33.75–46.7, and 26.0–33.5 wt %, respectively. The optimal bio-oil yield of 39.25 wt % was achieved at 650 W, 600 °C, and 40 g. The oxygenated derivatives, aromatic compounds, aliphatic hydrocarbons, and phenols constituted 40.24–74.25, 3.25–23.19, 0.3–9.77, and 1.58–7.75 area % of the bio-oils, respectively. Acetic acid (8.17–38.18 area %) was identified as a major bio-oil constituent, and hydrocarbons with carbon numbers C1 and C2 were found to be abundant. The experimental results demonstrate the potential of microwave pyrolysis as an eco-friendly and efficient way for converting eucalyptus waste into valuable bio-oil, contributing to the sustainable utilization of biomass resources.

  • RESEARCH ARTICLE
    Xiaoling Xian, Biying Li, Shiyong Feng, Jiale Huang, Xinyuan Fu, Ting Wu, Xiaoqing Lin
    Frontiers of Chemical Science and Engineering, 2024, 18(8): 85. https://doi.org/10.1007/s11705-024-2438-9

    In the present study, a sustainable pretreatment methodology combining liquid hot water and deep eutectic solvent is proposed for the efficient fractionation of hemicellulose, cellulose, and lignin from sugarcane bagasse, thereby facilitating the comprehensive utilization of both C5 and C6 sugars. The application of this combined pretreatment strategy to sugarcane bagasse led to notable enhancements in enzymatic saccharification and subsequent fermentation. Experiment results demonstrate that liquid hot water-deep eutectic solvent pretreatment yielded 85.05 ± 0.66 g·L–1 of total fermentable sugar (glucose: 60.96 ± 0.21 g·L–1, xylose: 24.09 ± 0.87 g·L–1) through enzymatic saccharification of sugarcane bagasse. Furthermore, fermentation of the pretreated sugarcane bagasse hydrolysate yielded 34.33 ± 3.15 g·L–1 of bioethanol. These findings confirm the effectiveness of liquid hot water-deep eutectic solvent pretreatment in separating lignocellulosic components, thus presenting a sustainable and promising pretreatment method for maximizing the valuable utilization of biomass resources.

  • RESEARCH ARTICLE
    Pengzhi Bei, Antony Rajendran, Jie Feng, Wen-Ying Li
    Frontiers of Chemical Science and Engineering, 2024, 18(10): 111. https://doi.org/10.1007/s11705-024-2462-9

    The traditional separation of bicyclic and tricyclic aromatics from coal tar involves complicated multi-steps and consumes significantly more energy. Previous work accomplished the separation between anthracene-phenanthrene isomers using electrostatic interaction, but for the separation between bicyclic and tricyclic aromatics, electrostatic interactions are difficult to produce a recognizable effect. Naphthalene-based solvents, named as naphthaleneacetamide, naphthaleneethanol, naphthalenemethanol, naphthol, naphthylacetic acid, naphthylacetonitrile, and naphthylamine, respectively, were used for the efficient separation of naphthalene and phenanthrene via dispersion interaction. Results showed that the pre-studied structural parameters are the key factors in selecting an efficient solvent. And the substituents on the intermolecular interactions involved in the separation processes had an important impact, which were evaluated. Naphthalenemethanol exhibited a superior performance with a purity of 96.3 wt % naphthalene products because its electron-donating substituent enables the selective recognition of naphthalene via the dispersion interaction. The used naphthalene-based solvents can be regenerated and recycled via back extraction with a purity of over 90 wt % naphthalene products, suggesting solvent structural stability during the regeneration processes. Notably, the naphthalene-based solvents also demonstrated better separation performance for polycyclic aromatics from coal tar with a purity of over 80 wt % for bicyclic aromatics. This study would enhance the utilization of coal tar as a valuable source of polycyclic aromatics besides broadening the knowledge for applying non-bonded interaction in the separation of polycyclic aromatics technologies.

  • RESEARCH ARTICLE
    Ecrin Ekici, Güray Yildiz, Magdalena Joka Yildiz, Monika Kalinowska, Erol Şeker, Jiawei Wang
    Frontiers of Chemical Science and Engineering, 2024, 18(6): 70. https://doi.org/10.1007/s11705-024-2429-x

    Under optimal process conditions, pyrolysis of polyolefins can yield ca. 90 wt % of liquid product, i.e., combination of light oil fraction and heavier wax. In this work, the experimental findings reported in a selected group of publications concerning the non-catalytic pyrolysis of polyolefins were collected, reviewed, and compared with the ones obtained in a continuously operated bench-scale pyrolysis reactor. Optimized process parameters were used for the pyrolysis of waste and virgin counterparts of high-density polyethylene, low-density polyethylene, polypropylene and a defined mixture of those (i.e., 25:25:50 wt %, respectively). To mitigate temperature drops and enhance heat transfer, an increased feed intake is employed to create a hot melt plastic pool. With 1.5 g·min–1 feed intake, 1.1 L·min–1 nitrogen flow rate, and a moderate pyrolysis temperature of 450 °C, the formation of light hydrocarbons was favored, while wax formation was limited for polypropylene-rich mixtures. Pyrolysis of virgin plastics yielded more liquid (maximum 73.3 wt %) than that of waste plastics (maximum 66 wt %). Blending polyethylenes with polypropylene favored the production of liquids and increased the formation of gasoline-range hydrocarbons. Gas products were mainly composed of C3 hydrocarbons, and no hydrogen production was detected due to moderate pyrolysis temperature.

  • RESEARCH ARTICLE
    Sichen Fan, Yifan Liu, Yaning Zhang, Wenke Zhao, Chunbao Xu
    Frontiers of Chemical Science and Engineering, 2024, 18(7): 81. https://doi.org/10.1007/s11705-024-2436-y

    Microwave-assisted pyrolysis is an effective method for recycling plastic wastes into oils that can be used for aviation fuels. In this study, energy and economic analyses of aviation oil production from microwave-assisted pyrolysis of polystyrene were performed. The total energy efficiency, recovered energy efficiency, unitary cost, unitary energy economic cost, relative cost difference, and energy economic factor were detailed. And the effects of microwave power, pyrolysis temperature, microwave absorbent loading, and microwave absorbent type on these parameters were covered. It was found that pyrolysis temperature has the most significant effect on the unitary cost and unitary energy economic cost of aviation oil, and-microwave absorbent type has a significant influence on energy economic factor during the whole microwave-assisted pyrolysis process. The optimum reaction conditions at the tonnage system for pyrolysis of 1 t polystyrene were microwave power of 650 W, pyrolysis temperature of 460 °C, and silicon carbide (microwave absorbent) at a loading of 2 t (twice than feedstock loading). At these optimal conditions, the total energy efficiency, recovered energy efficiency, unitary cost, unitary energy economic cost, relative cost difference, and energy economic factor were 62.78%, 96.51%, 3.21 × 104 yuan·t–1, 779 yuan·GJ–1, 1.49, and 71.02%, respectively.