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Confinement effects in methanol to olefins catalysed by zeolites: A computational review

German Sastre

《化学科学与工程前沿（英文）》 2016年 第10卷 第1期   页码 76-89 doi: 10.1007/s11705-016-1557-3

摘要： Small pore zeolites, containing 8-rings as the largest, are widely employed as catalysts in the process of methanol-to-olefins (MTO). Reactants and products diffuse with constraints through 8-rings and this is one of the reaction bottlenecks related to zeolite micropore topology. Small pore zeolites and silicon-aluminophosphates(SAPOs) containing cavities, where olefins are mainly formed through the hydrocarbon pool (HP) mechanism, are frequently tested for MTO. Shape selectivity of transition states within the side-chain methylation will be reviewed as this is one of the controlling steps of the MTO process, with particular attention to the role of hexamethylbenzene (HMB) and heptamethylbenzenium cation (HeptaMB ), which are the most tipically detected reaction intermediates, common to the paring and side-chain routes within the HP mechanism. The relative stability of these and other species will be reviewed in terms of confinement effects in different cage-based zeolites. The role of the different alkylating agents, methanol, dimethyl ether (DME), and surface methoxy species (SMS) will also be reviewed from the computational viewpoint.

关键词： small pore zeolites     SAPOs     methanol-to-olefins     hydrocarbon pool mechanism     alkylation of polymethylbenzenes    

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The effect of hierarchical single-crystal ZSM-5 zeolites with different Si/Al ratios on its pore structure

Yuexin Hou, Xiaoyun Li, Minghui Sun, Chaofan Li, Syed ul Hasnain Bakhtiar, Kunhao Lei, Shen Yu, Zhao Wang, Zhiyi Hu, Lihua Chen, Bao-Lian Su

《化学科学与工程前沿（英文）》 2021年 第15卷 第2期   页码 269-278 doi: 10.1007/s11705-020-1948-3

摘要： Hierarchical single-crystal ZSM-5 zeolites with different Si/Al ratios (Hier-ZSM-5- , where = 50, 100, 150 and 200) were synthesized using an ordered mesoporous carbon-silica composite as hard template. Hier-ZSM-5- exhibits improved mass transport properties, excellent mechanical and hydrothermal stability, and higher catalytic activity than commercial bulk zeolites in the benzyl alcohol self-etherification reaction. Results show that a decrease in the Si/Al ratio in hierarchical single-crystal ZSM-5 zeolites leads to a significant increase in the acidity and the density of micropores, which increases the final catalytic conversion. The effect of porous hierarchy on the diffusion of active sites and the final catalytic activity was also studied by comparing the catalytic conversion after selectively designed poisoned acid sites. These poisoned Hier-ZSM-5- shows much higher catalytic conversion than the poisoned commercial ZSM-5 zeolite, which indicates that the numerous intracrystalline mesopores significantly reduce the diffusion path of the reactant, leading to the faster diffusion inside the zeolite to contact with the acid sites in the micropores predominating in ZSM-5 zeolites. This study can be extended to develop a series of hierarchical single-crystal zeolites with expected catalytic performance.

关键词： hierarchical zeolites     single crystalline     interconnected pores     improved diffusion performance     benzyl alcohol self-etherification reaction    

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Solid-state NMR for metal-containing zeolites: From active sites to reaction mechanism

Xingling Zhao, Jun Xu, Feng Deng

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 159-187 doi: 10.1007/s11705-019-1885-1

摘要： Metal-containing zeolite catalysts have found a wide range of applications in heterogeneous catalysis. To understand the nature of metal active sites and the reaction mechanism over such catalysts is of great importance for the establishment of structure-activity relationship. The advanced solid-state NMR (SSNMR) spectroscopy is robust in the study of zeolites and zeolite-catalyzed reactions. In this review, we summarize recent developments and applications of SSNMR for exploring the structure and property of active sites in metal-containing zeolites. Moreover, detailed information on host-guest interactions in the relevant zeolite catalysis obtained by SSNMR is also discussed. Finally, we highlight the mechanistic understanding of catalytic reactions on metal-containing zeolites based on the observation of key surface species and active intermediates.

关键词： metal-containing zeolites     solid-state NMR     active site     host-guest interaction     reaction mechanism    

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Analyzing the characterization of pore structures and permeability of diesel contaminated clays under

《结构与土木工程前沿（英文）》   页码 1264-1280 doi: 10.1007/s11709-023-0921-x

摘要： In this study, mercury intrusion porosimetry (MIP) and X-ray micro-computed tomography (XRμCT) were used to characterize the pore structures and investigate the permeability characteristics of clay after aging and contamination with diesel. The results of the MIP tests showed that aging leads to reductions in porosity and average diameter, as well as an increase in tortuosity. The XRμCT analysis yielded consistent results; it showed that aging renders pores more spherical and isotropic and pore surfaces smoother. This weakens the pore connectivity. Micromorphological analysis revealed that aging led to the rearrangement of soil particles, tighter interparticle overlapping, and a reduction in pore space. The combination of MIP and XRμCT provided a comprehensive and reliable characterization of the soil pore structure. An increased diesel content increased the porosity and average diameter and reduced the tortuosity of the pores. Mechanistic analysis showed that aging weakens interparticle cohesion; this causes large agglomerates to break down into smaller agglomerates, resulting in a tighter arrangement and a subsequent reduction in porosity. An increase in diesel content increases the number of large agglomerates and pore spaces between agglomerates, resulting in increased porosity. Both aging and diesel content can weaken the permeation characteristics of soil.

关键词： MIP     XRμCT     aging     diesel content     pore structure     permeability characteristics    

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Multifunctional heteroatom zeolites: construction and applications

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1462-1486 doi: 10.1007/s11705-021-2099-x

摘要： Multifunctional heteroatom zeolites have drawn broad attentions due to the possible synergistic effects in the catalytic reactions. Remarkable achievements have been made on the synthesis, characterization and catalytic applications of multifunctional heteroatom zeolite, while a review on this important topic is still missing. Herein, current research status of multifunctional heteroatom zeolites is briefly summarized, aiming to boost further researches. First, the synthesis strategies toward heteroatom zeolites are introduced, including the direct synthesis and postsynthesis routes; then, the spectroscopic techniques to identify the existing states of heteroatom sites and the corresponding physiochemical properties are shown and compared; finally, the catalytic applications of multifunctional heteroatom zeolites in various chemical reactions, especially in one-step tandem reactions, are discussed.

关键词： zeolite     multifunctional active sites     heteroatom     characterization     catalysis    

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Catalyst particle shapes and pore structure engineering for hydrodesulfurization and hydrodenitrogenation

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 897-908 doi: 10.1007/s11705-021-2127-x

摘要： Catalyst particle shapes and pore structure engineering are crucial for alleviating internal diffusion limitations in the hydrodesulfurization (HDS)/hydrodenitrogenation (HDN) of gas oil. The effects of catalyst particle shapes (sphere, cylinder, trilobe, and tetralobe) and pore structures (pore diameter and porosity) on HDS/HDN performance at the particle scale are investigated via mathematical modeling. The relationship between particle shape and effectiveness factor is first established, and the specific surface areas of different catalyst particles show a positive correlation with the average HDS/HDN reaction rates. The catalyst particle shapes primarily alter the average HDS/HDN reaction rate to adjust the HDS/HDN effectiveness factor. An optimal average HDS/HDN reaction rate exists as the catalyst pore diameter and porosity increase, and this optimum value indicates a tradeoff between diffusion and reaction. In contrast to catalyst particle shapes, the catalyst pore diameter and the porosity of catalyst particles primarily alter the surface HDS/HDN reaction rate to adjust the HDS/HDN effectiveness factor. This study provides insights into the engineering of catalyst particle shapes and pore structures for improving HDS/HDN catalyst particle efficiency.

关键词： hydrodesulfurization     hydrodenitrogenation     particle shape     pore structure    

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Hierarchically porous zeolites synthesized with carbon materials as templates

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1444-1461 doi: 10.1007/s11705-021-2090-6

摘要： Hierarchically porous zeolites are promising candidates in catalytic conversion of relatively bulky molecules, and their syntheses have attracted significant attention. From both industrial and scientific perspectives, different carbon materials have been widely employed as hard templates for the preparation of hierarchically porous zeolites during the past two decades. In this review, the progress in synthetic strategies using carbon materials as templates is comprehensively summarized. Depending on the affinity between the carbon templates and zeolite precursors, the substantial strategies for synthesizing hierarchical zeolites are introduced in direct templates and indirect templates. Direct templates methods, by which the carbon materials are directly mixed with precursors gel as hard templates, are first reviewed. Then, we discuss the indirect templates method (crystallization of carbon-silica composites), by which the carbon is produced by in situ pyrolysis of organic-inorganic precursors. In addition, the technique of encapsulating metal species into zeolites crystals with the assistance of carbon templates is also discussed. In the conclusion part, the factors affecting the synthesis of carbon-templated hierarchically porous zeolites are remarked. This review is expected to attract interest in the synthesis strategies of hierarchically porous zeolites, especially cost-effective and large-scale production methodologies, which are essential to the industrial application of hierarchical zeolites.

关键词： hierarchical zeolites     carbon materials     direct templates     indirect templates     carbon-silica composites    

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High-precision diffusion measurement of ethane and propane over SAPO-34 zeolites for methanol-to-olefin

Dali Cai, Yu Cui, Zhao Jia, Yao Wang, Fei Wei

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 77-82 doi: 10.1007/s11705-017-1684-5

摘要： The methanol-to-olefin (MTO) process has attracted much attention and many problems including lifetime and selectivity of light olefins have all been connected to the diffusion problems in zeolite crystals. However, a quantitative study of diffusion problems in SAPO-34 zeolites is lacking. In this paper, we performed a high-precision diffusion measurement of the diffusion behavior of ethane and propane, which represent ethylene and propylene respectively, over SAPO-34. The diffusions of ethane and propane over fresh and coked SAPO-34 zeolites with different crystal sizes were carefully studied. Ethane and propane show different diffusion behavior in SAPO-34. The diffusion of ethane is almost not influenced by the crystal size and coke percentage, whereas that of propane is strongly affected. A slower diffusion velocity was observed in bigger crystals, and the diffusion velocity decline significantly with the coke percentage increasing. The diffusion coefficient was calculated with both the internal and surface diffusion models, and the results show that the surface diffusion plays a key role in the diffusion process of both ethane and propane. We believe that this work would be helpful for understanding the diffusion of different molecules in SAPO-34 zeolites, and may lay the foundation of MTO research.

关键词： diffusion measurement     methanol-to-olefin process    

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Uncoupled state space solution to layered poroelastic medium with anisotropic permeability and compressible pore

Zhiyong AI, Wenze ZENG, Yichong CHENG, Chao WU

《结构与土木工程前沿（英文）》 2011年 第5卷 第2期   页码 171-179 doi: 10.1007/s11709-011-0103-0

摘要： This paper presents an uncoupled state space solution to three-dimensional consolidation of layered poroelastic medium with anisotropic permeability and compressible pore fluid. Starting from the basic equations of poroelastic medium, and introducing intermediate variables, the state space equation usually comprising eight coupled state vectors is uncoupled into two sets of equations of six and two state vectors in the Laplace-Fourier transform domain. Combined with the continuity conditions between adjacent layers and boundary conditions, the uncoupled state space solution of a layered poroelastic medium is obtained by using the transfer matrix method. Numerical results show that the anisotropy of permeability and the compressibility of pore fluid have remarkable influence on the consolidation behavior of poroelastic medium.

关键词： uncoupled state space solution     layered poroelastic medium     three-dimensional consolidation     anisotropic permeability     compressible pore fluid    

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Influence of pore structure on biologically activated carbon performance and biofilm microbial characteristics

《环境科学与工程前沿（英文）》 2021年 第15卷 第6期 doi: 10.1007/s11783-021-1419-1

摘要：

• Pore structure affects biologically activated carbon performance.

关键词： Granular activated carbon     Biologically activated carbon filter     Bacterial community structure     Pore structure    

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Effect of catalyst layer mesoscopic pore-morphology on cold start process of PEM fuel cells

Ahmed Mohmed DAFALLA, Fangming JIANG

《能源前沿（英文）》 2021年 第15卷 第2期   页码 460-472 doi: 10.1007/s11708-021-0733-4

摘要： Water transport is of paramount importance to the cold start of proton exchange membrane fuel cells (PEMFCs). Analysis of water transport in cathode catalyst layer (CCL) during cold start reveals the distinct characteristics from the normal temperature operation. This work studies the effect of CCL mesoscopic pore-morphology on PEMFC cold start. The CCL mesoscale morphology is characterized by two tortuosity factors of the ionomer network and pore structure, respectively. The simulation results demonstrate that the mesoscale morphology of CCL has a significant influence on the performance of PEMFC cold start. It was found that cold-starting of a cell with a CCL of less tortuous mesoscale morphology can succeed, whereas starting up a cell with a CCL of more tortuous mesoscale morphology may fail. The CCL of less tortuous pore structure reduces the water back diffusion resistance from the CCL to proton exchange membrane (PEM), thus enhancing the water storage in PEM, while reducing the tortuosity in ionomer network of CCL is found to enhance the water transport in and the water removal from CCL. For the sake of better cold start performance, novel preparation methods, which can create catalyst layers of larger size primary pores and less tortuous pore structure and ionomer network, are desirable.

关键词： cold start     energy conversion     fuel cells     mesoscale morphology     tortuosity     water management    

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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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Crystalline porous materials: from zeolites to metal-organic frameworks (MOFs)

Zaiku Xie, Bao-Lian Su

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 123-126 doi: 10.1007/s11705-020-1921-1

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A ruptured recurrent small bowel gastrointestinal stromal tumour causing hemoperitoneum

null

《医学前沿（英文）》 2015年 第9卷 第1期   页码 108-111 doi: 10.1007/s11684-014-0344-0

摘要：

Hemoperitoneum is a rare and potentially life-threatening complication of GIST. We reported a 54-year-old man who developed disseminated intra-abdominal recurrence from a previously resected gastrointestinal stromal tumour (GIST) of the small bowel, and the patient presented with hemoperitoneum. Emergent debulking surgery was performed. A high dose imatinib was prescribed. Despite the presence of residual disease, the patient was well clinically 8 months after the operation. Even though, there is no evidence to support the routine use of debulking surgery in the management of GIST. In our patient, disease progression after second line targeted therapy and the absence of alternative treatment options for spontaneous rupture and hemoperitoneum prompted us to treat the patient aggressively. Resection of the ruptured GIST was carried out for control of bleeding and to prevent recurrent bleeding in this patient with good surgical risks. During the treatment decision-making, the patient’s general condition, the risk of surgery and the extent of dissemination were taken into consideration. In this patient who presented with spontaneous rupture of a small intestinal GIST, the novel use of targeted therapy and aggressive surgical treatment produced reasonably good survival outcome.

关键词： gastrointestinal stromal tumour     hemoperitoneum     small bowel GIST     small bowel neoplasm     imatinib    

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Mesoporous zeolites as efficient catalysts for oil refining and natural gas conversion

Jie ZHU, Xiangju MENG, Fengshou XIAO

《化学科学与工程前沿（英文）》 2013年 第7卷 第2期   页码 233-248 doi: 10.1007/s11705-013-1329-2

摘要： Zeolites have been regarded as one of the most important catalysts in petrochemical industry due to their excellent catalytic performance. However, the sole micropores in zeolites severely limit their applications in oil refining and natural gas conversion. To solve the problem, mesoporous zeolites have been prepared by introducing mesopores into the zeolite crystals in recent years, and thus have the advantages of both mesostructured materials (fast diffusion and accessible for bulky molecules) and microporous zeolite crystals (strong acidity and high hydrothermal stability). In this review, after giving a brief introduction to preparation, structure, and characterization of mesoporous zeolites, we systematically summarize catalytic applications of these mesoporous zeolites as efficient catalysts in oil refining and natural gas conversion including catalytic cracking of heavy oil, alkylation, isomerization, hydrogenation, hydrodesulfurization, methane dehydroaromatization, methanol dehydration to dimethyl ether, methanol to olefins, and methanol to hydrocarbons.

关键词： mesoporous zeolite     catalysis     oil refining     natural gas conversion    

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标题 作者 时间 类型 操作

Confinement effects in methanol to olefins catalysed by zeolites: A computational review

German Sastre

期刊论文

The effect of hierarchical single-crystal ZSM-5 zeolites with different Si/Al ratios on its pore structure

Yuexin Hou, Xiaoyun Li, Minghui Sun, Chaofan Li, Syed ul Hasnain Bakhtiar, Kunhao Lei, Shen Yu, Zhao Wang, Zhiyi Hu, Lihua Chen, Bao-Lian Su

期刊论文

Solid-state NMR for metal-containing zeolites: From active sites to reaction mechanism

Xingling Zhao, Jun Xu, Feng Deng

期刊论文

Analyzing the characterization of pore structures and permeability of diesel contaminated clays under

期刊论文

Multifunctional heteroatom zeolites: construction and applications

期刊论文

Catalyst particle shapes and pore structure engineering for hydrodesulfurization and hydrodenitrogenation

期刊论文

Hierarchically porous zeolites synthesized with carbon materials as templates

期刊论文

High-precision diffusion measurement of ethane and propane over SAPO-34 zeolites for methanol-to-olefin

Dali Cai, Yu Cui, Zhao Jia, Yao Wang, Fei Wei

期刊论文

Uncoupled state space solution to layered poroelastic medium with anisotropic permeability and compressible pore

Zhiyong AI, Wenze ZENG, Yichong CHENG, Chao WU

期刊论文

Influence of pore structure on biologically activated carbon performance and biofilm microbial characteristics

期刊论文

Effect of catalyst layer mesoscopic pore-morphology on cold start process of PEM fuel cells

Ahmed Mohmed DAFALLA, Fangming JIANG

期刊论文

Mesoporous zeolites for biofuel upgrading and glycerol conversion

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

期刊论文

Crystalline porous materials: from zeolites to metal-organic frameworks (MOFs)

Zaiku Xie, Bao-Lian Su

期刊论文

A ruptured recurrent small bowel gastrointestinal stromal tumour causing hemoperitoneum

null

期刊论文

Mesoporous zeolites as efficient catalysts for oil refining and natural gas conversion

Jie ZHU, Xiangju MENG, Fengshou XIAO

期刊论文