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Time-resolved dissolution elucidates the mechanism of zeolite MFI crystallization
Science Advances ( IF 13.6 ) Pub Date : 2021-06-16 , DOI: 10.1126/sciadv.abg0454
Krassimir N Bozhilov 1 , Thuy Thanh Le 2 , Zhengxing Qin 3 , Tanguy Terlier 4 , Ana Palčić 5 , Jeffrey D Rimer 2 , Valentin Valtchev 6, 7
Affiliation  

Zeolite crystal growth mechanisms are not fully elucidated owing to their complexity wherein the formation of a particular zeolite can occur by more than one crystallization pathway. Here, we have conducted time-resolved dissolution experiments of MFI-type zeolite crystals in ammonium fluoride medium where detailed structural analysis allowed us to extrapolate and elucidate the possible mechanism of nucleation and crystal growth. A combination of electron and scanning probe microscopy shows that dissolution initiates preferentially at lattice defects and progressively removes defect zones to reveal a mosaic structure of crystalline domains within each zeolite crystal. This mosaic architecture evolves during the growth process, reflecting the changing conditions of zeolite formation that can be retroactively assessed during zeolite crystal dissolution. Moreover, a more general implication of this study is the establishment that dissolution can be used successfully as an ex situ technique to uncover details about crystal growth features inaccessible by other methods.



中文翻译:

时间分辨溶解阐明了沸石 MFI 结晶的机理

沸石晶体生长机制由于其复杂性而未完全阐明,其中特定沸石的形成可通过不止一种结晶途径发生。在这里,我们在氟化铵介质中进行了 MFI 型沸石晶体的时间分辨溶解实验,其中详细的结构分析使我们能够推断和阐明成核和晶体生长的可能机制。电子和扫描探针显微镜的组合表明,溶解优先在晶格缺陷处开始,并逐渐去除缺陷区域,以揭示每个沸石晶体内结晶域的镶嵌结构。这种马赛克建筑在成长过程中不断演变,反映了沸石形成的变化条件,可以在沸石晶体溶解过程中进行追溯评估。此外,这项研究的一个更普遍的意义是确定溶解可以成功地用作一种非原位技术来揭示其他方法无法获得的晶体生长特征的细节。

更新日期:2021-06-16
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