Thermochemistry of Metal-ligand Bonds (Singly and Multiply Charged)

犹他大学的彼得·阿门特劳特受到实验物理化学计划的支持，继续他在气相有机金属离子化学和化学动力学方面的实验研究。这项工作将利用导引离子束串联质谱仪，结合使用直流放电/流动管离子源和新开发的电喷雾/离子漏斗/六极离子导引离子源产生离子。我们将研究化学相互作用的四个相关领域。首先，将继续研究第三排过渡金属离子的化学，旨在测量金属与各种氢、氧和碳配体之间的键能。将开发一种离子迁移源，以便能够对较重的过渡金属元素进行新的特定状态的化学研究，重点是定量评估自旋轨道对反应性的影响。其次，从双电荷碱土金属离子的水合作用入手，定量计算了多电荷金属离子的溶剂化能。接下来，我们将探索金属离子与生物相关分子之间的键离解能。最后，将对能量传递函数进行更多的研究，并将继续开发用于反应动力学分析的统计方法，包括用于顺序解离路径、多电荷金属-配体络合物和越来越大的体系的那些方法。在这项研究中获得和传播的热力学信息与表面科学、有机金属化学、催化、生物系统和等离子体化学的应用有关。数据分析程序CRUCK正在继续发展，目前已免费提供给世界各地的团体使用。本科生和研究生，以及博士后助理参与了这一跨学科的科学，接触到广泛的主题，使用最先进的物理和分析方法。

Peter Armentrout of the University of Utah is supported by the Experimental Physical Chemistry Program to continue his experimental research in gas-phase organometallic ion chemistry and chemical dynamics. This effort will utilize guided ion beam tandem mass spectrometry, coupled with ion production using a DC discharge/flow tube ion source and a newly developed electrospray/ion funnel/hexapole ion guided ion source. Four related areas of chemical interactions will be studied. First, studies of the chemistry of third row transition metal ions designed to measure bond energies between metals and various hydrogen, oxygen, and carbon ligands will be pursued. An ion mobility source will be developed to enable new state-specific chemistry studies on heavier transition metal elements with an emphasis on a quantitative evaluation of spin-orbit effects on reactivity. Second, solvation energies of multiply charged metal ions will be quantitatively assessed starting with the hydration of doubly-charged alkaline earth metal ions. Next, bond dissociation energies between metal ions and biologically relevant molecules will be explored. Finally, additional studies of the energy transfer function will be performed and statistical methods for analysis of reaction dynamics will continue to be developed, including those for sequential dissociation pathways, multiply-charged metal-ligand complexes, and increasingly large systems. The thermodynamic information that is acquired and disseminated in this research is relevant to applications in surface science, organometallic chemistry, catalysis, biological systems, and plasma chemistry. The data analysis program CRUNCH, which continues to evolve, is made freely available and used by groups around the world. The undergraduate and graduate students, and postdoctoral associates involved in this interdisciplinary science are exposed to a broad range of topics, working with state-of-the-art physical and analytical methods.