PDF(Pubmed)
Abstract：
Nature creates exquisite molecular assemblies, required for the molecular-level functions of life, via self-assembly. Understanding and harnessing these complex processes presents an immense opportunity for the design and fabrication of advanced functional materials. However, the significant industrial potential of self-assembly to fabricate highly functional materials is hampered by a lack of knowledge of critical reaction intermediates, mechanisms, and kinetics. As we move beyond the covalent synthetic regime, into the domain of non-covalent interactions occupied by self-assembly, harnessing and embracing complexity is a must, and non-targeted analyses of dynamic systems are becoming increasingly important. Coordination driven self-assembly is an important subtype of self-assembly that presents several wicked analytical challenges. These challenges are \"wicked\" due the very complexity desired confounding the analysis of products, intermediates, and pathways, therefore limiting reaction optimisation, tuning, and ultimately, utility. Ion Mobility-Mass Spectrometry solves many of the most challenging analytical problems in separating and analysing the structure of both simple and complex species formed via coordination driven self-assembly. Thus, due to the emerging importance of ion mobility mass spectrometry as an analytical technique tackling complex systems, this review highlights exciting recent applications. These include equilibrium monitoring, structural and dynamic analysis of previously analytically inaccessible complex interlinked structures and the process of self-sorting. The vast and largely untapped potential of ion mobility mass spectrometry to coordination driven self-assembly is yet to be fully realised. Therefore, we also propose where current analytical approaches can be built upon to allow for greater insight into the complexity and structural dynamics involved in self-assembly.
摘要：
大自然创造了精致的分子组装，生命的分子水平功能所必需的，通过自组装。理解和利用这些复杂的过程为设计和制造先进的功能材料提供了巨大的机会。然而,由于缺乏关键反应中间体的知识，阻碍了自组装制造高功能材料的显着工业潜力，机制,和动力学。当我们超越共价合成体系时，进入自组装占据的非共价相互作用域，利用和拥抱复杂性是必须的，和动态系统的非目标分析变得越来越重要。协调驱动的自组装是自组装的重要子类型，提出了几个邪恶的分析挑战。这些挑战是“邪恶的”，因为所需的复杂性混淆了产品的分析，中间体,和路径，因此限制了反应优化，调谐，最终,公用事业。离子迁移率-质谱法在分离和分析通过配位驱动的自组装形成的简单和复杂物种的结构中解决了许多最具挑战性的分析问题。因此，由于离子迁移质谱作为处理复杂系统的分析技术的重要性，这篇评论突出了令人兴奋的最新应用。这些包括平衡监测，结构和动态分析以前分析不可访问的复杂互连结构和自排序过程。离子迁移质谱对协调驱动的自组装的巨大且尚未开发的潜力尚未完全实现。因此,我们还提出了可以建立当前分析方法的地方，以更深入地了解自组装中涉及的复杂性和结构动力学。
