Phases to Flow Laboratory, Chemical & Biological Engineering Department, Colorado School of Mines, 1500 Illinois Street, Golden, CO, 80401, USA.
Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, No.2, Nengyuan Road, Wushan, Tianhe District, Guangzhou, 510640, Guangdong, PR China.
Nat Commun. 2023 Feb 3;14(1):596. doi: 10.1038/s41467-023-36242-4.
Clathrate hydrates are a class of ordered structures that are stabilized via the delicate balance of hydrophobic interactions between water and guest molecules, of which the space-filling network of hydrogen-bonded (H-bonded) water molecules are closely related to tetrahedrally close-packed structures, known as Frank-Kasper (FK) phases. Here we report an alternative way to understand the intricate structures of clathrate hydrates, which unveils the diverse crystalline H-bonded networks that can be generated via assembly of one common building block. In addition to the intrinsic relations and pathways linking these crystals, we further illustrate the rich structural possibilities of clathrate hydrates. Given that the topological dual relations between networks of clathrate hydrates and tetrahedral close-packed structures, the descriptors presented for clathrate hydrates can be directly extended to other ordered materials for a more thorough understanding of their nucleation, phases transition, and co-existence mechanisms.
笼形水合物是一类通过水和客体分子之间的疏水相互作用的微妙平衡稳定的有序结构，其中填充空间的氢键（H 键）水分子网络与四面体紧密堆积结构密切相关，称为弗兰克-卡珀（FK）相。在这里，我们报告了一种理解笼形水合物复杂结构的替代方法，该方法揭示了通过组装一个常见的构筑块可以产生的多样化的结晶 H 键网络。除了这些晶体之间的内在关系和途径外，我们还进一步说明了笼形水合物的丰富结构可能性。鉴于笼形水合物网络和四面体紧密堆积结构之间的拓扑对偶关系，为笼形水合物提出的描述符可以直接扩展到其他有序材料，以更深入地了解它们的成核、相转变和共存机制。
