基于飞行时间质谱的金属团簇配合物组成、 结构和反应机理研究进展

Research Progresses in composition,structure and reaction mechanism of metal cluster complexes based on the time-of-flight mass spectrometry

金属团簇配合物的组成、结构和反应机理的研究对理性设计多功能金属团簇和全面理解团簇化学的本质至关重要.该文介绍了本课题组自主研发的一系列基于飞行时间质谱的检测系统,其中结合了高分辨电喷雾离子源飞行时间质谱(HR-ESI-TOF-MS)、原位程序升温热脱附质谱(TPD-MS)、速度成像光电子能谱(VMI-PES)、红外光解离光谱(IRPDS)等先进探测手段.在一些具体实例中的应用表明,这些表征方法在确定金属团簇的化学组成、揭示团簇的形成机理、解析团簇配体的热解行为、探测团簇的电子及几何结构等方面发挥着重要作用.结合电子结构和反应动态学计算发展更有效和多样的检测系统,在未来研究金属团簇配合物的组成、结构和反应机理方面是一项挑战和重要方向.

The study on the composition,structure and reaction mechanism of metal cluster complexes is of great importance in the rational design of multiple functional metal clusters,as well as in a comprehensive understanding of the nature of cluster chemistry.This review introduces a series of detection systems independently developed by our research group based on time-of-flight mass spectrometry,including high-resolution electrospray ionization time-of-flight mass spectrometry(HR-ESI-TOF-MS),in-situ temperature-programmed decomposition mass spectrometry(TPD-MS),velocity map imaging photoelectron spectroscopy(VMI-PES),and infrared photodissociation spectroscopy(IRPDS).Specific examples indicate that these characterization technologies play important roles in the study of metal clusters,including determining their chemical composition,revealing their formation mechanisms,analyzing ligand pyrolysis behaviors,and detecting their electronic and geometric structures.The development of more effective and diverse detection systems,together with electronic structure and reaction dynamics calculations,is a challenge and an important direction in the future for studying the composition,structure and reaction mechanism of metal cluster complexes.