A Facile Top‐Down Protocol for Postsynthesis Modification of Hierarchical Aluminum‐Rich MFI Zeolites

Yu, Lili; Huang, Sheng-Jun; Miao, Shu; Chen, Fucun; Zhang, Shuang; Liu, Zhenni; Xie, Sujuan; Xu, Longya

doi:10.1002/chem.201404817

Cited by 37 publications

(41 citation statements)

References 47 publications

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“…As ar esult, the sequential fluorination-desilication protocolh as been figured out for the Alrich MFI zeolite (Si/Al = 14.3). [32] This protocol is characteristic of as equential fluorination-desilication approach, which in-cludest he typical operations of incipient impregnation and high-temperature calcination (600 8C) in the antecedentf luorination step. For the first time, well-definedm esoporosity has been successfully introduced into the Al-rich MFI zeolites.…”

Section: The Pain Of Growing Up:w Elding Versatile Post-synthetic Appmentioning

confidence: 97%

“…Physical sorption, field-emission scanning electron microscopy (FESEM) and high-resolution transmission electron microscopy (HRTEM) measurements confirmed the creationo fi ntracrystalline mesopores centered at 6nm ( Figures 5a nd 6). [32] The final overall porosity highly depends on the interplay between fluorination and desilication. Generally,alower fluorination level requires ah igherd esilication temperature.…”

Section: The Pain Of Growing Up:w Elding Versatile Post-synthetic Appmentioning

confidence: 99%

“…There is also am inimum limit requirement on fluorination level, which depends on the pristine ZSM-5 zeolites and fluorination conditions. An extremelyl ow level of fluorination hardly benefits the following desilication.A sacomparison, ah igh fluorination level enables the mesoporosity development at al ower desilication [32] temperature;h owever,i rregular pore size distributions and overall porosities suffer from significant loss in microporosity. [32] Apparently,asuitable fluorination step paves the path for the subsequentd esilication.…”

Section: The Pain Of Growing Up:w Elding Versatile Post-synthetic Appmentioning

confidence: 99%

“…The first aspect is supported by the solid NMR results and concentrationvariation of extracted Al and Si as the function of desilication duration. [32] For the second aspect, it is challengingt op rovide directe vidence. The designed comparativee xperiments, based on the treatments of high-silica MFI zeolites( Si/Al = 197) in various designed inclusion modes of NaOH/Al(NO 3 ) 3 /NH 4 Fc omponent, ascertained the contribution of Al-F complexation to sustain the mesoporosityg rowth.…”

Section: The Pain Of Growing Up:w Elding Versatile Post-synthetic Appmentioning

confidence: 99%

“…The designed comparativee xperiments, based on the treatments of high-silica MFI zeolites( Si/Al = 197) in various designed inclusion modes of NaOH/Al(NO 3 ) 3 /NH 4 Fc omponent, ascertained the contribution of Al-F complexation to sustain the mesoporosityg rowth. [32] Given the successo ff luorination, more severep erturbations to the framework Al sites could also work. Steaming is ap ractical and provena pproach to decrease the density of framework [AlO 4 ]u nits, which certainly relievest he shielding effect to the desilication.B earing this in mind, we figuredo ut as equential steaming-desilicationp rotocol for the Al-rich ZSM-5 zeolites (Si/Al < 15).…”

Section: The Pain Of Growing Up:w Elding Versatile Post-synthetic Appmentioning

confidence: 99%

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Mesopore Engineering for Well‐Defined Mesoporosity in Al‐Rich Aluminosilicate Zeolites

Zhang

Jin

Zou

et al. 2018

Chemistry A European J

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Desilication has been proven an effective approach for the construction of well‐defined hierarchical porosities inside zeolites with an optimal framework Al content (Si/Al=25–50). However, for the Al‐rich aluminosilicate zeolites, desilication is constrained by the excess and extensive shielding effects from high Al‐contents. The developments in the desilication of siliceous zeolites convey a simplified principle of controlled dissolution of the microporous matrix for the construction of hierarchical porosities, which benefits the innovation of synthetic approaches for Al‐rich zeolites. The perturbations to the environments of framework Al species may alleviate the excess shielding effects. This review highlights two corresponding protocols of sequential “fluorination–desilication” and “steaming–desilication” for the construction of hierarchical porosities inside Al‐rich ZSM‐5 zeolites. The success of these two protocols revitalizes the prevailing understanding of the interplay between dealumination and desilication, and implies the necessity of investigating the overlooked roles of extra‐framework Al species. Despite the long history and significant achievements in the last decade, fundamental understandings at the molecule level are still limited for the desilication‐based top‐down approaches. In particular, the investigations on Al‐rich zeolites just find their growing. The bridging of dealumination and desilication is essential for other industrially relevant Al‐rich zeolites (e.g., faujasite zeolites). The complexities in the inherent characters (topology, spatial distribution, proximity, etc.) and apparent parameters (morphology, crystal/particle size, etc.) demand constructive synthetic toolboxes and further fundamental understanding.

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Section: The Pain Of Growing Up:w Elding Versatile Post-synthetic Appmentioning

confidence: 97%

Section: The Pain Of Growing Up:w Elding Versatile Post-synthetic Appmentioning

confidence: 99%

Section: The Pain Of Growing Up:w Elding Versatile Post-synthetic Appmentioning

confidence: 99%

Section: The Pain Of Growing Up:w Elding Versatile Post-synthetic Appmentioning

confidence: 99%

Section: The Pain Of Growing Up:w Elding Versatile Post-synthetic Appmentioning

confidence: 99%

See 3 more Smart Citations

Mesopore Engineering for Well‐Defined Mesoporosity in Al‐Rich Aluminosilicate Zeolites

Zhang

Jin

Zou

et al. 2018

Chemistry A European J

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Toward rational design of hierarchical beta zeolites: An overview and beyond

2020

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The ever‐growing need to increase the efficiency of crude oil refining raises the prospects for utilizing advanced catalytic materials to supply increasing global demands for fine chemicals and petrochemicals. Zeolites have been used as indispensable catalysts in many commercial refining processes. Among them, zeolite beta is one of the most widely produced zeolite materials with industrial significance due to its large micropores and three‐dimensional pore structures. This article discusses recent progress on hierarchical beta zeolites from various synthetic strategies. Using zeolite beta as a representative case, we provide an overview on key aspects that are applicable to different zeolites via a variety of topics, such as selection of different template materials, tailoring of mesopore sizes by base leaching, organotemplate‐free synthesis of hierarchical zeolites, and selective desilication. This article concludes with a perspective on the design of scalable hierarchical zeolites that are more relevant as industrial catalysts in commercial processes.

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Faster and Safer “In situ” Synthesis of Germanane and Silicane

Georgantas,

Giousis,

Moissinac

et al. 2024

Small Methods

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Germanane (GeH) and silicane (SiH), members of the Xanes family, have garnered significant attention as 2D materials due to their diverse properties, which hold promise for applications in electronics, optoelectronics, energy storage, and sensing. Typically, highly concentrated hydrochloric acid (HCl) or hydrofluoric acid (HF) is employed in the synthesis of these Xanes, but both routes are problematic due to slow kinetics and safety concerns, respectively. Here for the first time, a faster and safer method is demonstrated for Xanes synthesis that harnesses the generation of HF “in situ” using a solution of HCl and lithium fluoride (LiF) salt, overcoming the key challenges of the conventional methods. A variety of characterization techniques to establish a baseline is utilized for both Xanes and to provide a holistic knowledge regarding this method, the possible consequences of this approach, and the possibility of applying it to other layered Zintl phases. The novel synthesis protocol results in high‐quality GeH and SiH with bandgaps (Eg) of 1.75 and 2.47 eV respectively, highlighting their potential suitability for integration into semiconductor applications.

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A Facile Top‐Down Protocol for Postsynthesis Modification of Hierarchical Aluminum‐Rich MFI Zeolites

Cited by 37 publications

References 47 publications

Mesopore Engineering for Well‐Defined Mesoporosity in Al‐Rich Aluminosilicate Zeolites

Mesopore Engineering for Well‐Defined Mesoporosity in Al‐Rich Aluminosilicate Zeolites

Toward rational design of hierarchical beta zeolites: An overview and beyond

Faster and Safer “In situ” Synthesis of Germanane and Silicane

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