Bridging the Gap Between Solution & Solid State, Low & High Nuclearity Studies in the Self Assembly of Nanoscale Polyoxometalate Clusters

目的：提出一种利用低温喷雾质谱、配体设计和晶体学分析相结合的方法来理解纳米尺度多金属氧酸盐团簇的自组装，首次弥合了溶液和固态研究之间的差距。通过使用低温喷雾质谱“扫描”我们的反应系统，我们将能够在溶液中“发现”从低核到高核的新团簇，了解存在的复杂平衡，“捕获”和稳定高活性团簇，并组装基本新型的团簇。最终的目标是建立和控制一个真正的构建块库，可以用于预先设计的纳米级多金属酸盐簇的组装。这将使我们从发现转向像有机分子合成一样可靠地预先确定团簇形成的宏伟目标。这一目标的实现将为多金属氧酸盐从新材料到催化剂和纳米电子元件的大量科学、工业和技术应用开辟道路。

Aim: To propose an approach to understanding the self assembly of nanoscale polyoxometalate clusters using a combination of cryospray mass spectrometry, ligand design, and crystallographic analysis, bridging the gap between solution and solid state studies for the first time. By using the cryospray mass spectrometry to 'scan' our reaction systems we will be able to 'discover' new clusters in solution that range from low to high nuclearity clusters, understand the complex equilibria present, 'trap' and stabilize highly reactive clusters, and assemble fundamentally new types of cluster. Ultimately the aim is to establish and control a library of real building blocks that can be used in the assembly of pre-designed nanoscale polyoxometalate clusters. This will allow us to move from discovery with the grand aim of pre-determining cluster formation as reliably as the synthesis of organic molecules. The realisation of this goal would open up a plethora of scientific, industrial and technological applications of polyoxometalates from new materials to catalysts and nano-electronic components.