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学者姓名:李铁森
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The development of sustainable techniques to produce high-performance zeolite is essential to achieve green production in industry.Herein,we report an eco-friendly route to synthesizing hierarchical Beta zeolite from kaolinite and recycled mother liquor.The results reveal that the unutilized species(such as silicon species and Na+)in mother liquor stayed in a stable concentration during eleven recycled experiments.Moreover,the syn-thesized Beta zeolites still have comparable physicochemical properties and catalytic performance in the esteri-fication of levulinic acid with ethanol over the initial zeolite although eleven recycled experiments.Life cycle assessment exhibits that the synthesis of Beta zeolite with recycled mother liquor can reduce global warming potential by 23%and resource depletion-water use by 36%compared to that without recycled mother liquor.This quantitatively demonstrates that the approach proposed in this work is really a sustainable one,extremely increasing the utilization efficiency of raw materials and decreasing the environmental burden.
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GB/T 7714 | Guoxi Xiao , Xiaoling Chen , Tiesen Li et al. Eco-friendly synthesis and environmental impact assessment of hierarchical Beta zeolite from kaolinite and recycled mother liquor [J]. | 绿色化学工程(英文) , 2024 , 5 (4) : 501-510 . |
MLA | Guoxi Xiao et al. "Eco-friendly synthesis and environmental impact assessment of hierarchical Beta zeolite from kaolinite and recycled mother liquor" . | 绿色化学工程(英文) 5 . 4 (2024) : 501-510 . |
APA | Guoxi Xiao , Xiaoling Chen , Tiesen Li , Chan Wang , Qingyan Cui , Yuanyuan Yue . Eco-friendly synthesis and environmental impact assessment of hierarchical Beta zeolite from kaolinite and recycled mother liquor . | 绿色化学工程(英文) , 2024 , 5 (4) , 501-510 . |
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Controllable synthesis of hierarchical zeolites from natural aluminosilicate minerals is considered an efficient and eco-friendly approach for the production of high-performance zeolites, but its synthesis mechanism is still obscure. Herein, we take the synthesis of a single-crystalline hierarchical NaA zeolite using submolten salt depolymerized kaolin (SMS-K) as the sole source of silicon and aluminum via a mesoscale reorganization strategy as an example to elucidate the reorganization process. Comprehensive morphological and structural analyses reveal that sodium-rich voids in SMS-K facilitate concurrent assembly both within the interior and at the interface of the amorphous gel, leading to the formation of numerous nanoparticles with short-range order which assemble into single-crystal nanocube NaA zeolites with intracrystalline mesopores. By harnessing confinement effects, SMS-K modulates the growth of nanoparticle sizes and enhances the intimate interconnection of nanocubes, thereby yielding NaA zeolite aggregates that exhibit hierarchical porosity, encompassing micro-, meso-, and macropores. This study offers the potential for designing and precisely controlling the fabrication of hierarchical zeolites derived from natural minerals.
Keyword :
depolymerized kaolin depolymerized kaolin hierarchical NaA zeolite hierarchical NaA zeolite mesoscale reorganization mechanism mesoscale reorganization mechanism role of sodium and hydroxide ions role of sodium and hydroxide ions single-crystalline single-crystalline
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GB/T 7714 | Chen, Xiaoling , Li, Tiesen , Cui, Qingyan et al. Mesoscale Reorganization of the Depolymerized Aluminosilicate into Single-Crystalline Hierarchical Zeolite [J]. | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (44) : 61371-61380 . |
MLA | Chen, Xiaoling et al. "Mesoscale Reorganization of the Depolymerized Aluminosilicate into Single-Crystalline Hierarchical Zeolite" . | ACS APPLIED MATERIALS & INTERFACES 16 . 44 (2024) : 61371-61380 . |
APA | Chen, Xiaoling , Li, Tiesen , Cui, Qingyan , Shi, Jie , Tan, Yisheng , Bao, Xiaojun et al. Mesoscale Reorganization of the Depolymerized Aluminosilicate into Single-Crystalline Hierarchical Zeolite . | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (44) , 61371-61380 . |
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The development of sustainable techniques to produce high-performance zeolite is essential to achieve green production in industry. Herein, we report an eco-friendly route to synthesizing hierarchical Beta zeolite from kaolinite and recycled mother liquor. The results reveal that the unutilized species (such as silicon species and Na+) in mother liquor stayed in a stable concentration during eleven recycled experiments. Moreover, the synthesized Beta zeolites still have comparable physicochemical properties and catalytic performance in the esterification of levulinic acid with ethanol over the initial zeolite although eleven recycled experiments. Life cycle assessment exhibits that the synthesis of Beta zeolite with recycled mother liquor can reduce global warming potential by 23% and resource depletion-water use by 36% compared to that without recycled mother liquor. This quantitatively demonstrates that the approach proposed in this work is really a sustainable one, extremely increasing the utilization efficiency of raw materials and decreasing the environmental burden. © 2024 Institute of Process Engineering, Chinese Academy of Sciences.
Keyword :
Eco-friendly synthesis Eco-friendly synthesis Hierarchical Beta zeolite Hierarchical Beta zeolite Life cycle assessment Life cycle assessment Recycled mother liquor Recycled mother liquor
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GB/T 7714 | Xiao, G. , Chen, X. , Li, T. et al. Eco-friendly synthesis and environmental impact assessment of hierarchical Beta zeolite from kaolinite and recycled mother liquor [J]. | Green Chemical Engineering , 2024 , 5 (4) : 501-510 . |
MLA | Xiao, G. et al. "Eco-friendly synthesis and environmental impact assessment of hierarchical Beta zeolite from kaolinite and recycled mother liquor" . | Green Chemical Engineering 5 . 4 (2024) : 501-510 . |
APA | Xiao, G. , Chen, X. , Li, T. , Wang, C. , Cui, Q. , Yue, Y. . Eco-friendly synthesis and environmental impact assessment of hierarchical Beta zeolite from kaolinite and recycled mother liquor . | Green Chemical Engineering , 2024 , 5 (4) , 501-510 . |
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A seed-directed approach to synthesizing FeZSM-22 zeolite without organic structure directing agent(OSDA)was developed by using Fe-rich diatomite as all aluminum and iron sources.The FeZSM-22 zeolite with optimal crystallinity and purity can be obtained by systematically adjusting feed composi-tion and synthesis conditions.Characterizations show that FeZSM-22 zeolite synthesized with OSDA-free owns high crystallinity,obvious thin needle-shaped morphology and high Bronsted/Lewis acid ratio.Significantly,when used for n-octane hydroisomerization reaction,its derived catalyst exhibits the best catalytic performance reflected by the highest selectivity to C8 isomers compared to the two reference catalysts prepared based on a Fe-containing and a Fe-free ZSM-22 synthesized through an OSDA-directed route from natural diatomite and conventional chemicals,respectively.This work provides an alternative route to sustainably synthesizing heteroatomic zeolites with high performance.
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GB/T 7714 | Tiesen Li , Ting Chen , Yinghui Ye et al. OSDA-free synthesis of FeZSM-22 zeolite from natural minerals for n-octane hydroisomerization [J]. | 中国化学工程学报(英文版) , 2024 , 66 (2) : 51-59 . |
MLA | Tiesen Li et al. "OSDA-free synthesis of FeZSM-22 zeolite from natural minerals for n-octane hydroisomerization" . | 中国化学工程学报(英文版) 66 . 2 (2024) : 51-59 . |
APA | Tiesen Li , Ting Chen , Yinghui Ye , Peng Dong , Tinghai Wang , Qingyan Cui et al. OSDA-free synthesis of FeZSM-22 zeolite from natural minerals for n-octane hydroisomerization . | 中国化学工程学报(英文版) , 2024 , 66 (2) , 51-59 . |
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A seed-directed approach to synthesizing FeZSM-22 zeolite without organic structure directing agent (OSDA) was developed by using Fe-rich diatomite as all aluminum and iron sources. The FeZSM-22 zeolite with optimal crystallinity and purity can be obtained by systematically adjusting feed composition and synthesis conditions. Characterizations show that FeZSM-22 zeolite synthesized with OSDA-free owns high crystallinity, obvious thin needle-shaped morphology and high Bronsted/Lewis acid ratio. Significantly, when used for n-octane hydroisomerization reaction, its derived catalyst exhibits the best catalytic performance reflected by the highest selectivity to C-8 isomers compared to the two reference catalysts prepared based on a Fe-containing and a Fe-free ZSM-22 synthesized through an OSDA-directed route from natural diatomite and conventional chemicals, respectively. This work provides an alternative route to sustainably synthesizing heteroatomic zeolites with high performance. (c) 2023 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved.
Keyword :
FeZSM-22 zeolite FeZSM-22 zeolite Natural minerals Natural minerals n-octane hydroisomerization n-octane hydroisomerization OSDA-free synthesis OSDA-free synthesis
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GB/T 7714 | Li, Tiesen , Chen, Ting , Ye, Yinghui et al. OSDA-free synthesis of FeZSM-22 zeolite from natural minerals for n-octane hydroisomerization [J]. | CHINESE JOURNAL OF CHEMICAL ENGINEERING , 2024 , 66 : 51-59 . |
MLA | Li, Tiesen et al. "OSDA-free synthesis of FeZSM-22 zeolite from natural minerals for n-octane hydroisomerization" . | CHINESE JOURNAL OF CHEMICAL ENGINEERING 66 (2024) : 51-59 . |
APA | Li, Tiesen , Chen, Ting , Ye, Yinghui , Dong, Peng , Wang, Tinghai , Cui, Qingyan et al. OSDA-free synthesis of FeZSM-22 zeolite from natural minerals for n-octane hydroisomerization . | CHINESE JOURNAL OF CHEMICAL ENGINEERING , 2024 , 66 , 51-59 . |
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To gain a profound understanding of the reaction pathway and the controlling step of residue oil slurry-phase hydrocracking over Fe2O3 catalyst, a six-lumped kinetic model was proposed and employed to acquire the kinetic rate constants based on each fraction yield obtained at 400 to 420 °C under initial H2 pressures of 8 to 10 MPa for 1 to 3 h. The optimal kinetic rate constant for each step of vacuum residue (VR) conversion process was determined via Levenberg-Marquardt algorithm and the sum of squares error (SSE). The results reveal that VR converted into naphtha and diesel is dominant according to their kinetic rate constants, followed by the conversion of vacuum gas oil (VGO) to diesel, diesel to naphtha, and diesel to gas. Furthermore, the sensitivity analysis confirms a strong agreement between the predicted and experimental values. The combination of kinetic rate constants and activation energy illustrates that the gas product primarily originates from naphtha. Additionally, the higher H2 pressure effectively mitigates coke deposition by restricting the aggregation of polycyclic aromatics, as evidenced by the increase in the reaction activation energy for the conversion of VR to coke and the analysis of the used catalyst. © 2024 Elsevier Ltd
Keyword :
Activation analysis Activation analysis Activation energy Activation energy Catalysts Catalysts Coke Coke Hematite Hematite Hydrocracking Hydrocracking Kinetic parameters Kinetic parameters Kinetic theory Kinetic theory Naphthas Naphthas Rate constants Rate constants Sensitivity analysis Sensitivity analysis
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GB/T 7714 | Cui, Qingyan , Zheng, Bin , Wang, Boshi et al. Kinetics study on residue oil slurry-phase hydrocracking with Fe2O3 catalyst [J]. | Fuel , 2024 , 374 . |
MLA | Cui, Qingyan et al. "Kinetics study on residue oil slurry-phase hydrocracking with Fe2O3 catalyst" . | Fuel 374 (2024) . |
APA | Cui, Qingyan , Zheng, Bin , Wang, Boshi , Yan, Jianteng , Liu, Jiangyong , Li, Tiesen et al. Kinetics study on residue oil slurry-phase hydrocracking with Fe2O3 catalyst . | Fuel , 2024 , 374 . |
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Synthesizing zeolites, which are important materials used in the petroleum and chemical industries, from natural aluminosilicate minerals has been qualitatively recognized as a greener approach compared to that from traditional Si- and Al-containing chemicals; however, studies on the quantitative environmental impacts are still lacking. Herein, life cycle assessment (LCA) and green metrics (atom economy and environmental factor) were employed to comparatively assess the life cycle environmental impacts of zeolites synthesized from chemicals and natural minerals at the industrial scale. The values of seven LCA impact categories and sensitivity analysis between them were thoroughly compared. The results showed that, for each category, the synthesis from natural minerals has lower environmental impacts to varying degrees than that from chemicals. Further efficiency analysis of zeolite manufacturing technologies by green metrics indicated that the synthesis from natural minerals outperforms that from chemicals in terms of the resource utilization rate. The quantitative results indicate that significant benefits stem from the replacement of raw materials from chemicals to natural minerals. This work may provide a basis for the future selection and upgrade of zeolite production processes. Life cycle assessment and green metrics were used to comparatively assess the synthesis of zeolites from natural minerals and chemicals in which the former exhibits a better balance between efficiency and environmental impacts than the latter.
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GB/T 7714 | Chen, Xiaoling , Xiao, Guoxi , Li, Tiesen et al. Comparative environmental assessment of zeolites synthesized from chemicals and natural minerals [J]. | GREEN CHEMISTRY , 2024 , 26 (9) : 5273-5283 . |
MLA | Chen, Xiaoling et al. "Comparative environmental assessment of zeolites synthesized from chemicals and natural minerals" . | GREEN CHEMISTRY 26 . 9 (2024) : 5273-5283 . |
APA | Chen, Xiaoling , Xiao, Guoxi , Li, Tiesen , Wang, Chan , Cui, Qingyan , Bao, Xiaojun et al. Comparative environmental assessment of zeolites synthesized from chemicals and natural minerals . | GREEN CHEMISTRY , 2024 , 26 (9) , 5273-5283 . |
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FAU型分子筛因其独特的孔道结构已成为化学工业中应用最广泛、用量最大的催化剂、催化剂载体及吸附剂之一.然而, FAU型分子筛单一的微孔孔道限制了客体分子的扩散,导致其性能严重下降.相比之下,等级孔FAU型分子筛具有微-介/大孔复合的多级孔道结构,能够促进大分子的扩散、提高活性位点的可接近性,进而改善其吸附和催化性能.目前,等级孔分子筛的制备方法主要包括“自下而上”的直接合成法和“自上而下”的后处理法.本文主要介绍了近年来等级孔X型和Y型分子筛制备方法的研究现状,重点总结了等级孔X型和Y型分子筛在吸附、催化等过程中的应用性能,并对等级孔FAU型分子筛的绿色化制备进行展望.
Keyword :
催化 催化 后处理 后处理 吸附 吸附 直接合成 直接合成 等级孔FAU型分子筛 等级孔FAU型分子筛
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GB/T 7714 | 董鹏 , 朱琳 , 骆龙华 et al. 等级孔FAU型分子筛的制备及应用的研究进展 [J]. | 科学通报 , 2024 , 69 (19) : 2718-2728 . |
MLA | 董鹏 et al. "等级孔FAU型分子筛的制备及应用的研究进展" . | 科学通报 69 . 19 (2024) : 2718-2728 . |
APA | 董鹏 , 朱琳 , 骆龙华 , 李铁森 , 王廷海 , 王婵 et al. 等级孔FAU型分子筛的制备及应用的研究进展 . | 科学通报 , 2024 , 69 (19) , 2718-2728 . |
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Natural rectorite modified by the hydrothermal method was employed to prepare a catalyst for the slurry-phase hydrocracking of vacuum residue (VR). The influence of hydrothermal treatment on the properties of rectorite and the performance of the corresponding catalyst was examined. Hydrothermal treatment of the rectorite led to the formation of Fe3O4, as evidenced by H2-TPR analysis. XPS results indicate that the hydrothermal treatment of rectorite can intensify the sulfidation process of Mo species supported on it, possibly due to modifications in the surface properties of the rectorite. Comparative slurry-phase hydrocracking tests showed that the catalyst supported on hydrothermally treated rectorite exhibited significantly higher VR conversion, higher liquid product yield, and higher yields of gasoline and diesel fractions, but lower gas yield compared to the catalyst supported on untreated rectorite. This is ascribed to the high hydrogenation activity of the catalyst supported on hydrothermally treated rectorite, which effectively suppresses the over-cracking reactions of intermediate products that would otherwise produce gas, illustrating the process intensification achieved through hydrothermal treatment. © 2024 Elsevier B.V.
Keyword :
Hydrocracking Hydrocracking Hydrothermal treatment Hydrothermal treatment Mo catalyst Mo catalyst Sulfidation Sulfidation Vacuum residue Vacuum residue
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GB/T 7714 | Cui, Q. , Yan, J. , Zhang, H. et al. Hydrothermal treatment of natural rectorite enhanced Mo sulfidation for slurry-phase hydrocracking of vacuum residue [J]. | Chemical Engineering and Processing - Process Intensification , 2024 , 205 . |
MLA | Cui, Q. et al. "Hydrothermal treatment of natural rectorite enhanced Mo sulfidation for slurry-phase hydrocracking of vacuum residue" . | Chemical Engineering and Processing - Process Intensification 205 (2024) . |
APA | Cui, Q. , Yan, J. , Zhang, H. , Feng, W. , Yue, Y. , Li, T. et al. Hydrothermal treatment of natural rectorite enhanced Mo sulfidation for slurry-phase hydrocracking of vacuum residue . | Chemical Engineering and Processing - Process Intensification , 2024 , 205 . |
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The catalytic dehydration of glycerol to acrolein offers a sustainable route for efficiently utilizing low-cost and renewable bioglycerol. This work deeply explores glycerol dehydration to acrolein over ZSM-5 zeolite catalysts with various pore structures and aluminum distributions. The results reveal that glycerol conversion is enhanced through the construction of a mesoporous structure and the increase in Br & oslash;nsted acid sites of the catalysts, but acrolein selectivity is not directly related to these factors. Further characterizations, density functional theory calculation, kinetic study, and reaction mechanism analysis demonstrate that the richest Alsingle sites in the zeolite framework and the least Alpair sites in the straight and sinusoidal channels can prevent the generated acrolein from adsorbing on adjacent Al sites. This allows acrolein to immediately escape from the catalyst surface, reducing side reactions and enhancing its selectivity. Therefore, the synergistic between the mesoporous structure and more Alsingle sites in the ZSM-5 zeolite framework promotes acrolein yield. Additionally, a descriptor phi, reflecting the amount of Alsingle sites and the external specific surface area of the ZSM-5 zeolite, is first proposed to more clearly elucidate the structure-performance relationship. This study provides a new perspective for understanding the mechanism of catalytic dehydration of glycerol to acrolein, guiding the development of highly efficient catalysts. It is significant for the sustainable development of the biodiesel and acrolein production industry.
Keyword :
aluminum distribution aluminum distribution catalytic dehydration catalytic dehydration glycerol glycerol pore structure pore structure ZSM-5 zeolitecatalyst ZSM-5 zeolitecatalyst
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GB/T 7714 | Luo, Wei , Shi, Jie , Li, Tiesen et al. Catalytic Dehydration of Glycerol to Acrolein over ZSM-5 Zeolites: Synergistic Effect of Pore Structure and Aluminum Distribution [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 13 (1) : 321-332 . |
MLA | Luo, Wei et al. "Catalytic Dehydration of Glycerol to Acrolein over ZSM-5 Zeolites: Synergistic Effect of Pore Structure and Aluminum Distribution" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 13 . 1 (2024) : 321-332 . |
APA | Luo, Wei , Shi, Jie , Li, Tiesen , Wang, Tinghai , Liu, Jiangyong , Cui, Qingyan et al. Catalytic Dehydration of Glycerol to Acrolein over ZSM-5 Zeolites: Synergistic Effect of Pore Structure and Aluminum Distribution . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 13 (1) , 321-332 . |
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