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学者姓名：王廷海
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Abstract ：
Cyclohexane as liquid organic hydrogen carriers has attracted considerable interest in the field of hydrogen storage technology. However, the innovation of efficient catalyst for producing H2 through cyclohexane dehydrogenation remains a substantial challenge. In this study, we have successfully developed Pt/MgAl2O4 catalysts exhibiting outstanding catalytic performance in cyclohexane dehydrogenation. Notably, the optimal catalyst Pt/MgAl2O4-700 achieves cyclohexane conversion of 89.1 % and benzene selectivity of over 99 % at 345 °C, resulting in a high hydrogen evolution rate of 933 mmol/gPt/min. Moreover, this catalyst exhibits remarkable long-term stability, with no evident loss of activity in 225-hour dehydrogenation reaction. The catalyst was characterized by XRD, N2 adsorption–desorption, STEM, XPS, NH3-TPD, CO-FTIR and H2-TPR techniques, which provides detailed structure information for elucidation of structure–activity relationship. The spinel structure and moderate acid density of the support enable highly dispersed Pt species at the surface of MgAl2O4. This results in the formation of ultra-small and sintering-resistant Pt particles that exhibit exceptional activity in cyclohexane dehydrogenation. Additionally, the presence of positively charged Ptδ+ species in Pt/MgAl2O4 facilitates the rapid desorption of benzene product. This effectively prevents the formation of coke arising from benzene dehydrogenation, which ensures to achieve high stability. These findings provide valuable knowledge for the rational design of efficient metal-based catalysts for liquid organic hydrogen carriers in hydrogen storage systems. © 2024
Keyword ：
Ammonia Ammonia Benzene Benzene Catalyst selectivity Catalyst selectivity Cyclohexane Cyclohexane Dehydrogenation Dehydrogenation Desorption Desorption Hydrogen production Hydrogen production Hydrogen storage Hydrogen storage Sintering Sintering
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| GB/T 7714 | Guo, Lipeng , Xu, Zhikang , Wang, Tinghai et al. Stable Pt/MgAl2O4 catalysts for efficient production of H2 from cyclohexane dehydrogenation [J]. | Chemical Engineering Science , 2024 , 299 . |
| MLA | Guo, Lipeng et al. "Stable Pt/MgAl2O4 catalysts for efficient production of H2 from cyclohexane dehydrogenation" . | Chemical Engineering Science 299 (2024) . |
| APA | Guo, Lipeng , Xu, Zhikang , Wang, Tinghai , Zhu, Haibo . Stable Pt/MgAl2O4 catalysts for efficient production of H2 from cyclohexane dehydrogenation . | Chemical Engineering Science , 2024 , 299 . |
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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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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 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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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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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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In order to develop a high-efficiency iron oxide catalyst for the slurry-phase hydrocracking of poor heavy oil, the mesoporous iron oxide was successfully synthesized by using the waste wood powder as a template, and the influence of alkali concentration in the resulting solution on crystal phase, morphology and pore structure of the synthesized samples was investigated. The crystal phase of the synthesized iron oxide transfers from alpha-Fe2O3 to gamma-Fe2O3, and their crystal sizes gradually decrease with an increase of alkali concentration based on the XRD and HRTEM results. Additionally, the iron oxide with mesoporous structure, larger surface area and pore volume is obtained at the higher concentration of alkali in solution confirmed by N2 adsorption-desorption analysis. The assessment result of the iron oxide catalyst employed in the slurry-phase hydrocracking of vacuum residue (VR) illustrates that the yields of gasoline and diesel distillates obtained over Fe-O-B20, Fe-O-B24 and Fe-O-B30 cata-lysts are higher compared with those over Fe-O-B2 and Fe-O-B14 catalysts, it can be attributed that more exposure Fe active sites derived from their larger surface area and pore volume availably improve the catalyst hydroge-nation activity, which can inhibit the over-cracking reaction of intermediate products and the condensation of polycyclic aromatic hydrocarbon in VR to enhance the yields of gasoline and diesel distillates.
Keyword ：
Iron oxide catalyst Iron oxide catalyst Mesoporous Mesoporous Slurry-phase hydrocracking Slurry-phase hydrocracking Synthesis Synthesis Vacuum residue Vacuum residue
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| GB/T 7714 | Hu, Xiubin , Wang, Jianbo , Wang, Tinghai et al. Synthesis and performance of mesoporous iron oxide in vacuum residue slurry-phase hydrocracking [J]. | FUEL , 2023 , 332 . |
| MLA | Hu, Xiubin et al. "Synthesis and performance of mesoporous iron oxide in vacuum residue slurry-phase hydrocracking" . | FUEL 332 (2023) . |
| APA | Hu, Xiubin , Wang, Jianbo , Wang, Tinghai , Wang, Chan , Zhang, Hongwei , Yuan, Pei et al. Synthesis and performance of mesoporous iron oxide in vacuum residue slurry-phase hydrocracking . | FUEL , 2023 , 332 . |
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Aiming at improving reaction selectivity of zeolite Beta-catalyzed isomerization of normal alkane, we reported a facile but efficient route to prepare the Beta@SBA-15 composite supports with low surface diffusion barriers in isomers formation from normal alkane. Microporous Beta zeolite and mesoporous SBA-15 zeolite were physically mixed and milled by high-energy planetary ball-mill. The addition of SBA-15 and milling, which have little effect on the acid properties of Beta zeolites, disaggregate the Beta particles and anchor the Beta nanocrystals on the surface of SBA-15 mesostructure. The apparent diffusivities of 2-methyl pentane measured by zero-length column method increased by 50%. n-Hexane isomerization tests show that the Pt/Beta@SBA-15 catalysts exhibit much higher selectivity to isomers, especially the dibranched isomers and lower selectivity to cracking reaction, owning to the reduced transport limitation of composite supports.
Keyword ：
Alkane isomerization Alkane isomerization Ball milling Ball milling Beta zeolite Beta zeolite Diffusion barriers Diffusion barriers SBA-15 addition SBA-15 addition
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| GB/T 7714 | Liu, Pengpeng , Qiu, Zihui , Shi, Huibing et al. Reducing the diffusion barriers of Pt/Beta catalyzed n-hexane isomerization by SBA-15 addition and high-energy milling [J]. | MICROPOROUS AND MESOPOROUS MATERIALS , 2023 , 356 . |
| MLA | Liu, Pengpeng et al. "Reducing the diffusion barriers of Pt/Beta catalyzed n-hexane isomerization by SBA-15 addition and high-energy milling" . | MICROPOROUS AND MESOPOROUS MATERIALS 356 (2023) . |
| APA | Liu, Pengpeng , Qiu, Zihui , Shi, Huibing , Song, Yu , Zhao, Deming , Wang, Pengzhao et al. Reducing the diffusion barriers of Pt/Beta catalyzed n-hexane isomerization by SBA-15 addition and high-energy milling . | MICROPOROUS AND MESOPOROUS MATERIALS , 2023 , 356 . |
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采用共沉淀-浸渍法制备了系列硫酸负载催化剂Pt/SO42--(ZrO2-Al2O3),利用X射线衍射仪、物理吸附仪、红外光谱仪等对其进行了表征,并在固定床微型反应装置上对其催化异丁烷正构化反应性能进行了评价.结果表明:硫酸单层分散于载体表面,硫酸负载不利于四方晶相ZrO2长大;随着硫酸负载量的增加,催化剂介孔结构的有序性增强且孔径减小,孔径最小降为3.41 nm,孔容可提高至0.091 cm3/g,比表面积增至100m2/g以上;在反应温度为250℃的条件下,硫酸负载量为15％时,异丁烷转化率高达41.74％;硫酸负载量为2％时,正丁烷选择性最高为93.91％.
Keyword ：
Pt/SO42--(ZrO2-Al2O3) Pt/SO42--(ZrO2-Al2O3) 催化剂 催化剂 单层分散 单层分散 异丁烷 异丁烷 正构化 正构化 硫酸 硫酸 酸性位 酸性位
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| GB/T 7714 | 宋宇 , 辛靖 , 张海洪 et al. 硫酸负载对Pt/SO42-(ZrO2-Al2O3)催化剂性能的影响 [J]. | 石化技术与应用 , 2023 , 41 (4) : 251-255 . |
| MLA | 宋宇 et al. "硫酸负载对Pt/SO42-(ZrO2-Al2O3)催化剂性能的影响" . | 石化技术与应用 41 . 4 (2023) : 251-255 . |
| APA | 宋宇 , 辛靖 , 张海洪 , 曾土城 , 范文轩 , 王廷海 et al. 硫酸负载对Pt/SO42-(ZrO2-Al2O3)催化剂性能的影响 . | 石化技术与应用 , 2023 , 41 (4) , 251-255 . |
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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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