Gas-phase ion chemistry

任何地方的化学都与金属原子有关。本研究计划探讨了金属原子在各种化学和生物环境中，在其正的单电荷和多电荷离子状态下（带有一个或多个）电子被移除的作用。将采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小分子（包括许多大气气体）的化学反应性。这些测量的结果将在质谱分析中得到应用，例如元素分析和地质年代学。其他测量将探索当单电荷和双电荷原子金属离子附着在有机或生物碎片（如多环芳烃和巴基球）上时反应性的变化。金属阳离子也会附着在带多重电荷的类dna阴离子上。特别强调的是这些类dna阴离子的化学和紫外线切割，以及这些离子的化学修复，这将在没有和存在金属原子离子的情况下进行。金属阳离子作为催化剂的作用将通过实验和理论在气相碳氢化合物的氧化中进行探索，这可能会在催化转化器中找到应用，并推进我们对催化基本原理的理解。将测量新的有机半导体分子中的金属杂质，以试图确定它们在这些半导体性能中的重要性。我们还将向外看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层，金属是由流星烧蚀沉积的，而在更远的星际云中，金属阳离子被认为既以自由原子离子的形式存在，又与小有机分子或粒子结合。在后一种环境中，金属催化的生物分子如氨基酸和多肽的生长特别有趣。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.