The importance of T⋯T⋯T angles in the feasibility of zeolites

Liu, Xuehua; Cubas, Soledad Valero; Argente, Estefanía; Botti, Vicente; Sastre, Germán

doi:10.1515/zkri-2014-1801

Cited by 26 publications

(21 citation statements)

References 36 publications

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“…The selection was further limited to 3-dimensional channel systems, only having 4, 5, 6 and 8-rings present in the structure, as well as minimum 80 % of the 8-rings to be circular. Furthermore, the selected structures were also limited to satisfy feasibility criteria reported elsewhere ( 35), (36) To evaluate the potential of the selected OSDAs an extensive experimental evaluation under various conditions and using various raw materials was undertaken. Hydrothermal synthesis was explored using OSDA1-3 under alkali conditions using either NaOH or KOH as the mineralizing agent in combination with either amorphous silica-alumina (ASA) or using a FAU zeolite as the T-atom source.…”

Section: Resultsmentioning

confidence: 99%

Synthesis of High-Silica Erionite Driven by Computational Screening of Hypothetical Zeolites

et al. 2019

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A hypothetical zeolite framework was selected from a database of hypothetical structures and adapted based on structural features relevant for deNOx and MTO catalysis. To attempt the realization of this structure a computational energy-based approach was applied to select relevant OSDAs (organic structure directing agents) molecules with large OSDA-zeolite stabilization energies, leading to the selection of three OSDAs (OSDA1, OSDA2, OSDA3) as potential candidates for the synthesis of the hypothetical zeolite (Hypo#1). Instead of Hypo#1, ERI was found to dominate the experimental product outcome when potassium was used as a mineralizing agent. In the case of OSDA3 a novel high-silica ERI was found. The different ERI products were characterized, intergrowth structures ruled out, and special attention was paid to the compositional and morphological features arising from the use of the different OSDAs. In the specific high-Si product obtained using OSDA3 a distinct tubular to prismatic crystal morphology could be seen. Theoretical stabilization energies calculated for potentially competing phases (Hypo#1, ERI, OFF, CHA among others) could be used to rationaliz e the experimental outcome to a certain extent, but our results show that considering the zeolite-OSDA interaction is probably not sufficient to realize hypothetical frameworks alone, especially for Al-containing zeolites where alkali ions play an important role during crystallization.

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Section: Resultsmentioning

confidence: 99%

Synthesis of High-Silica Erionite Driven by Computational Screening of Hypothetical Zeolites

et al. 2019

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“…Restricting the range of correlations or discarding all angular information leads to degradation of classification performance, indicating that the structural features that distinguish real and hypothetical zeolites involve angular correlations and patterns in the relative positions of second and third neighbor atoms -i.e., at length scales beyond the typical indicators that have been hypothesized in previous studies [11][12][13][14][15][16][17][18].…”

Section: Resultsmentioning

confidence: 86%

“…Which hypothetical zeolites are most likely synthesizable, and in which chemical composition? Previous attempts to answer these questions [11][12][13][14][15][16][17][18] have relied on intuitive guesses for structural descriptors such as rings and angles, which provide incomplete [19] and thus biased results. In the present work, we answer all these questions via rigorous data science methods combining unsupervised and supervised machine learning, [20] along with the generalized convex hull (GCH) description of thermodynamic stability, [21] yielding a new and powerful approach for sorting real [22] and hypothetical [2][3][4][5] zeolites, as well as finding promising zeolite candidates and suggesting likely chemical compositions for them.…”

Section: Introductionmentioning

confidence: 99%

Ranking the Synthesizability of Hypothetical Zeolites with the Sorting Hat

Helfrecht¹,

Pireddu²,

Semino³

et al. 2021

Preprint

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Zeolites are nanoporous alumino-silicate frameworks widely used as catalysts and adsorbents.Even though millions of distinct siliceous networks can be generated by computer-aided searches, no new hypothetical framework has yet been synthesized. The needle-in-a-haystack problem of finding promising candidates among large databases of predicted structures has intrigued materials scientists for decades; most work to date on the zeolite problem has been limited to intuitive structural descriptors. Here, we tackle this problem through a rigorous data science scheme-the "zeolite sorting hat"-that exploits interatomic correlations to produce a 95% real versus theoretical zeolites classification accuracy. The hypothetical frameworks that are grouped together with known zeolites are promising candidates for synthesis, that can be further ranked by estimating their thermodynamic stability. A critical analysis of the classifier reveals the decisive structural features. Further partitioning into compositional classes provides guidance in the design of synthetic strategies.

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“…Zeolite structure prediction generates a large number of theoretical zeolite structures, from which synthetic targets can be selected according to functional need. − Traditional zeolite prediction involves two major steps. The first step is to generate hypothetical zeolite structure models based on thermodynamic, topologic, or geometric regulations; − the second step is to evaluate the predicted structures and screen out unfeasible ones that would be difficult to realize experimentally. − Such two-step procedures lack efficiency. The model-generating step is computationally expensive, and the majority of the generated models are synthetically inaccessible and need to be screened out in the structure evaluation step.…”

Section: Designing Structure-directing Agentsmentioning

confidence: 99%

Toward a New Era of Designed Synthesis of Nanoporous Zeolitic Materials

Cao

2018

ACS Nano

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Due to their nanoporous framework structures, zeolites have been widely used as catalysts, adsorbents, and ion exchangers in many industrial fields. Discovering zeolitic materials with new structures and desired functions is one of the most important tasks in the zeolite community. Traditional zeolite discovery relies primarily on low-efficiency trial-and-error processes. So far, many computational and experimental efforts have been devoted to the designed synthesis of zeolitic materials, representing a promising highway toward function-led discovery of nanoporous materials. In particular, the design of structure-directing agents, the design of target zeolites via structure enumeration, and the reorganization of disassembled building layers have led to the discovery of dozens of unprecedented zeolitic structures in the past 5 years. In this Perspective, we briefly discuss these advances and describe the research efforts that are needed in the coming era of function-led zeolite discovery.

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The importance of T⋯T⋯T angles in the feasibility of zeolites

Cited by 26 publications

References 36 publications

Synthesis of High-Silica Erionite Driven by Computational Screening of Hypothetical Zeolites

Synthesis of High-Silica Erionite Driven by Computational Screening of Hypothetical Zeolites

Ranking the Synthesizability of Hypothetical Zeolites with the Sorting Hat

Toward a New Era of Designed Synthesis of Nanoporous Zeolitic Materials

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