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Influences of Deprotonation and Modulation on Nucleation and Growth of UiO-66: Intergrowth and Orientation
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2018-01-19 00:00:00 , DOI: 10.1021/acs.jpcc.7b11012 Bohan Shan , Joshua B. James , Mitchell R. Armstrong , Emily C. Close , Portia A. Letham , Kassandra Nikkhah , Y. S. Lin , Bin Mu 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2018-01-19 00:00:00 , DOI: 10.1021/acs.jpcc.7b11012 Bohan Shan , Joshua B. James , Mitchell R. Armstrong , Emily C. Close , Portia A. Letham , Kassandra Nikkhah , Y. S. Lin , Bin Mu 1
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The most common products obtained in the synthesis of zirconium-based metal–organic frameworks (ZrMOFs) are fine powders. The particle size of a typical ZrMOF UiO-66 was first reported to be around 200 nm, so the original crystal structure was only solved by powder XRD coupled with Rietveld refinement due to the incapability of single crystal XRD to solve such small crystals with poor crystallinity. One may ask the reason why the particle size of UiO-66 is so small compared to that of other common MOFs and what the key factor terminating the growth of UiO-66 is. In this work, we try to answer this question by proposing a hypothesis that the partially deprotonated ligand caused by the accumulated protons in the reaction solution is the key factor preventing the continuous growth of the UiO-66 crystal. The hypothesis is verified by growth reactivation with the addition of a deprotonating agent in an in situ biphase solvothermal reaction. As long as the protons were sufficiently coordinated by the deprotonating agent, the continuous growth of UiO-66 is guaranteed. Moreover, the modulation effect can impact the coordination equilibrium and nucleation so that an oriented attachment growth of UiO-66 film was achieved in membrane structures.
中文翻译：
去质子化和调制对UiO-66成核和生长的影响：共生和方向。
锆基金属-有机骨架（ZrMOF）的合成中获得的最常见产品是细粉。据报道，典型的ZrMOF UiO-66的粒径约为200 nm，因此原始粉末仅通过粉末XRD和Rietveld精炼才能解决，因为单晶XRD无法解决这种结晶度差的小晶体。有人可能会问为什么UiO-66的粒径比其他常见的MOF这么小，以及终止UiO-66增长的关键因素是什么。在这项工作中，我们尝试提出一个假设，即由反应溶液中积聚的质子引起的部分去质子化的配体是阻止UiO-66晶体连续生长的关键因素，从而回答这个问题。通过在原位双相溶剂热反应中添加去质子剂进行生长再活化来验证该假设。只要质子被去质子剂充分配位，就可以保证UiO-66的连续生长。此外，调制效应可影响配位平衡和成核作用，从而在膜结构中实现了UiO-66薄膜的定向附着生长。
更新日期：2018-01-19
中文翻译：
去质子化和调制对UiO-66成核和生长的影响：共生和方向。
锆基金属-有机骨架（ZrMOF）的合成中获得的最常见产品是细粉。据报道，典型的ZrMOF UiO-66的粒径约为200 nm，因此原始粉末仅通过粉末XRD和Rietveld精炼才能解决，因为单晶XRD无法解决这种结晶度差的小晶体。有人可能会问为什么UiO-66的粒径比其他常见的MOF这么小，以及终止UiO-66增长的关键因素是什么。在这项工作中，我们尝试提出一个假设，即由反应溶液中积聚的质子引起的部分去质子化的配体是阻止UiO-66晶体连续生长的关键因素，从而回答这个问题。通过在原位双相溶剂热反应中添加去质子剂进行生长再活化来验证该假设。只要质子被去质子剂充分配位，就可以保证UiO-66的连续生长。此外，调制效应可影响配位平衡和成核作用，从而在膜结构中实现了UiO-66薄膜的定向附着生长。
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