Although the positions of water guests in porous crystals can be identified, determination of their filling sequence remains challenging. We deciphered the water-filling mechanism for the state-of-the-art water-harvesting metal-organic framework MOF-303 by performing an extensive series of single-crystal x-ray diffraction measurements and density functional theory calculations. The first water molecules strongly bind to the polar organic linkers; they are followed by additional water molecules forming isolated clusters, then chains of clusters, and finally a water network. This evolution of water structures led us to modify the pores by the multivariate approach, thereby precisely modulating the binding strength of the first water molecules and deliberately shaping the water uptake behavior. This resulted in higher water productivity, as well as tunability of regeneration temperature and enthalpy, without compromising capacity and stability.

中文翻译：

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金属有机框架中水结构的演变以改善大气集水

尽管可以识别多孔晶体中水客的位置，但确定其填充顺序仍然具有挑战性。我们通过执行一系列广泛的单晶 X 射线衍射测量和密度泛函理论计算，破译了最先进的集水金属有机框架 MOF-303 的注水机制。第一个水分子与极性有机接头强烈结合；随后是额外的水分子形成孤立的簇，然后是簇链，最后是水网络。水结构的这种演变导致我们通过多元方法修改孔隙，从而精确调节第一个水分子的结合强度并刻意塑造吸水行为。这导致更高的水生产率，