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学者姓名：李铁森
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Abstract ：
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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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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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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Abstract ：
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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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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A sustainable defect-engineering strategy for the dealumination of Y zeolite is described. This strategy includes the green synthesis of a well-crystallized Y zeolite with point defects arising from the incorporation of Fe atoms by using Fe-containing perlite and the subsequent preparation of ultra-stable Y (USY) zeolite by efficient steaming dealumination. The systematic characterizations verify that Fe atoms originally existing in the perlite are incorporated into the as-synthesized Y zeolite and function as point defects, leading to the distortion of framework Al. The step-by-step investigation of dealumination process shows that vacancies are formed by the extraction of framework Fe in ammonium exchange, and the framework dealumination is promoted under the combined effect of the distorted framework Al and the formed vacancies during steaming treatment. The resulting USY zeolite owns excellent features in (hydro)thermal stability, pore structure and acid property, and exhibits outstanding catalytic performance in the cracking of n-octane and 1,3,5-triisopropylbenzene.
Keyword ：
catalytic cracking catalytic cracking dealumination dealumination defect engineering defect engineering USY zeolite USY zeolite Y zeolite Y zeolite
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| GB/T 7714 | Dong, Peng , Zhang, Jinyu , Li, Tiesen et al. Dealumination of Y zeolite through an economic and eco-friendly defect-engineering strategy [J]. | AICHE JOURNAL , 2023 , 69 (9) . |
| MLA | Dong, Peng et al. "Dealumination of Y zeolite through an economic and eco-friendly defect-engineering strategy" . | AICHE JOURNAL 69 . 9 (2023) . |
| APA | Dong, Peng , Zhang, Jinyu , Li, Tiesen , Wang, Chan , Xu, Jingdong , Wang, Tinghai et al. Dealumination of Y zeolite through an economic and eco-friendly defect-engineering strategy . | AICHE JOURNAL , 2023 , 69 (9) . |
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Deep understanding of the formation mechanism is crucial to the rational design and controllable synthesis of zeolites with desired pore architecture and acidity. Herein, we take the synthesis of NaA zeolite from a submolten salt depolymerized kaolin (SMS-K) as an example to elucidate the formation mechanism of NaA zeolite. By using SMS-K as sole Si and Al sources, a highly pure and crystalline NaA zeolite with superior ion exchange ability was synthesized. By using various ex-situ and in-situ characterizations and studying the crystallization kinetics, a plausible formation mechanism of NaA zeolite via the mesoscale reorganization of SMS-K was proposed. The results indicate that the reorganization of SMS-K into NaA zeolite follows the solid-phase transformation route. Upon being mixed with H2O, SMS-K that is mainly composed of silicate monomers and chain/ring microstruc-tures is in-situ transformed rapidly into mesoscale intermediates containing double four-membered rings and beta cages, sufficient stirring during aging generates more mesoscale intermediates. During the subsequent crystal-lization process, the mesoscale intermediates are further self-assembled into NaA nanoparticles when theirs amount reaches a maximum, and finally the nanoparticles grow into well-shaped cubic NaA zeolite particles with smooth surfaces through layer spreading. Our work provides the theoretical foundation for the design and green synthesis of zeolites directly from the natural minerals.
Keyword ：
Crystallization kinetics Crystallization kinetics Mesoscale reorganization mechanism Mesoscale reorganization mechanism NaA zeolite NaA zeolite Submolten salt depolymerized kaolin Submolten salt depolymerized kaolin
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| GB/T 7714 | Chen, Xiaoling , Wang, Ying , Li, Tiesen et al. Synthesis of NaA zeolite via the mesoscale reorganization of submolten salt depolymerized kaolin: A mechanistic study [J]. | CHEMICAL ENGINEERING JOURNAL , 2023 , 454 . |
| MLA | Chen, Xiaoling et al. "Synthesis of NaA zeolite via the mesoscale reorganization of submolten salt depolymerized kaolin: A mechanistic study" . | CHEMICAL ENGINEERING JOURNAL 454 (2023) . |
| APA | Chen, Xiaoling , Wang, Ying , Li, Tiesen , Bi, Xiaotao , Jiang, Lilong , Bao, Xiaojun et al. Synthesis of NaA zeolite via the mesoscale reorganization of submolten salt depolymerized kaolin: A mechanistic study . | CHEMICAL ENGINEERING JOURNAL , 2023 , 454 . |
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Platinum nanoparticles (Pt NPs) embedded in the multi-hollow silicalite-1 zeolite (Pt@MH-S-1) were prepared by the sequential alkali etching and recrystallization of parent microporous silicalite-1 zeolite. Then, toluene and acetone were employed as probe molecules to determine the catalytic behavior of Pt@MH-S-1 for the elimination of volatile organic compounds (VOCs). The results reveal that Pt@MH-S-1 with multi-hollow structure owns large external specific surface area for dispersing the Pt NPs, and abundant mesoporous channels for improving the accessibility of toluene to Pt NPs as well as high reactive oxygen content, excellent toluene adsorption capacity and moderate adsorption strength. Owing to these characteristics, Pt@MH-S-1 exhibits superior performance both in toluene and acetone catalytic oxidations as reflected by 100% conversion acquired at even a low temperature of 137 and 180 degrees C, respectively. Moreover, Pt@MH-S-1 also shows good stability toward the various conditions, signifying its superiority and potential in practical application for VOCs treatment.
Keyword ：
Catalytic oxidation Catalytic oxidation Multi-hollow silicalite-1 Multi-hollow silicalite-1 Pt nanoparticles Pt nanoparticles Volatile organic compounds Volatile organic compounds
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| GB/T 7714 | Tang, Siyao , Liu, Haiyan , Li, Tiesen et al. Encapsulating platinum nanoparticles into multi-hollow silicalite-1 zeolite for catalytic oxidation of volatile organic compounds [J]. | CHEMICAL ENGINEERING SCIENCE , 2023 , 286 . |
| MLA | Tang, Siyao et al. "Encapsulating platinum nanoparticles into multi-hollow silicalite-1 zeolite for catalytic oxidation of volatile organic compounds" . | CHEMICAL ENGINEERING SCIENCE 286 (2023) . |
| APA | Tang, Siyao , Liu, Haiyan , Li, Tiesen , Wang, Chan , Cui, Qingyan , Yue, Yuanyuan et al. Encapsulating platinum nanoparticles into multi-hollow silicalite-1 zeolite for catalytic oxidation of volatile organic compounds . | CHEMICAL ENGINEERING SCIENCE , 2023 , 286 . |
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