Amorphous-to-Crystalline Transformation: How Cluster Aggregation Drives the Multistep Nucleation of ZIF-8

化学 成核 无定形固体 星团(航天器) 转化(遗传学) 化学工程 化学物理 结晶学 有机化学 生物化学 计算机科学 工程类 基因 程序设计语言
作者
Ahmet Dok,Sambhu Radhakrishnan,Flip de Jong,Estelle Becquevort,Olivier Deschaume,C. Vinod Chandran,Yovan de Coene,Carmen Bartic,Mark Van der Auweraer,Wim Thielemans,Christine E. A. Kirschhock,Monique A. Van Der Veen,Thierry Verbiest,Eric Breynaert,Stijn Van Cleuvenbergen
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
被引量:1
标识
DOI:10.1021/jacs.4c16615
摘要

Nucleation, the pivotal first step of crystallization, governs the essential characteristics of crystallization products, including size distribution, morphology, and polymorphism. While understanding this process is paramount to the design of chemical, pharmaceutical, and industrial production processes, major knowledge gaps remain, especially with respect to the crystallization of porous solids. Also for nanocrystalline ZIF-8, one of the most widely studied metal–organic frameworks, questions regarding the species involved in the nucleation pathway and their structural and chemical transformations remain unanswered. By combining harmonic light scattering, inherently sensitive to structural changes, with NMR spectroscopy, which reveals molecular exchanges between particles and solution, we were able to capture the crystallization mechanism of ZIF-8 in unprecedented detail. This dual approach provides concurrent structural and chemical insights, revealing key processes not previously observed in ZIF crystallization. Upon mixing, small charged prenucleation clusters (PNCs) are formed, exhibiting an excess of ligands and net positive charge. We show that nucleation is initiated by aggregation of PNCs, through the release of ligands and associated protons to the liquid. This leads to the formation of charge neutral amorphous precursor particles (APPs), which incorporate neutral monomers from the solution and crystallized ZIF-8. Our work highlights chemical dynamics as a vital, yet often overlooked, dimension in the multistage structural evolution of MOFs. By establishing the critical role of PNCs in the nucleation of ZIF-8, new pathways open up for controlling crystallization of metal–organic frameworks through targeted chemical interactions with these species.
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