Gas-phase ion chemistry

世界各地的许多化学物质都与金属原子有关。这项研究提案探索了在各种化学和生物环境中，金属原子在其正单电荷和多电荷离子状态(一个或多个电子被移除)中所起的作用。将使用最先进的仪器进行测量，以表征和了解孤立的原子金属和非金属离子与包括许多大气气体在内的小分子的化学反应能力。这些测量的结果将在分析质谱学中得到应用，例如在元素分析和地质年代学中的应用。其他测量将探索当单电荷和双电荷的原子金属离子与有机或生物碎片(如多环芳烃和巴克球)结合时反应性的变化。金属阳离子也将被连接到多电荷的类DNA阴离子上。将特别强调这些类似DNA的阴离子的化学和紫外线裂解，以及这些离子的化学修复，这将在没有金属原子离子的情况下进行。我们将从实验和理论两个方面探讨金属阳离子在气相中烃的氧化反应中的作用，这可能会在催化转化器中得到应用，并加深我们对催化原理的理解。金属杂质将在新的有机半导体分子中进行测量，以试图确定它们在这些半导体性能中的重要性。我们还将展望原子金属阳离子在行星大气化学中的作用，包括我们自己的大气中金属被流星烧蚀沉积的地方，以及更远的星际云中，在星际云中，金属阳离子被认为既以自由原子离子的形式存在，也被束缚在有机小分子或粒子上。在这些后一种环境中，特别令人感兴趣的是金属催化的生物分子的生长，如氨基酸和多肽。人们对金属在太空化学中的重要性知之甚少。

Much of chemistry everywhere involves metal atoms. This research proposal explores the role of metal atoms in their positive singly and multiply-charged ionic state (with one or more) electrons removed in a variety of chemical and biological environments. Measurements will be taken with state-of-the-art instrumentation to characterize and understand the chemical reactivity of isolated atomic metal and non-metal ions with small molecules including many atmospheric gases. The results of these measurements will find application in analytical mass spectrometry as aplied in elemental analysis and geochronology, for example. Other measurements will explore the change in reactivity when singly and doubly-charged atomic metal ions are attached to organic or biological fragments such as polycyclic aromatic hydrocarbons and buckyballs. Metal cations will also be attached to multiply-charged DNA-like anions. Special emphasis will be given to the chemical and ultraviolet cleavage of these DNA-like anions, as well as the chemical repair of such ions, and this will be done in the absence and presence of metal atom ions. The role of metal cations as catalysts will be explored using both experiment and theory in the oxidation of hydrocarbons in the gas phase nd this may find application in catalytic converters as well as advancing our understanding of the fundamentals of catalysis. Metal impurities will be measured in new organic semiconductor molecules in an attempt to ascertain their importance in the performance of these semiconductors. We shall also look outward to the role of atomic metal cations in the chemistry of planetary atmospheres including our own where metals are deposited by meteor ablation and still further out in interstellar clouds where metal cations are thought to exist both as free atomic ions and bound to small organic molecules or particles. Of particular interest in these latter environments is the metal-catalyzed growth of biological molecules such as amino acids and peptides. Very little is known about the importance of metals in the chemistry of space.