Preparation, isolation, and characterization of fragile acid-base complexes including intermediates of potential biological relevance

二氧化碳和硫氧化物等小型反应性气体的化学行为在大尺度vis-à-vis全球变暖和酸雨中具有重要意义。它们在材料和生物系统中的作用常常被忽视。为了更多地了解这种化学反应，我们正在系统地探索这些小气体分子在各种环境中的反应性，包括不寻常的溶剂和多孔材料。这种探索可以通过配位化学的使用来指导，配位化学是一个小分子或离子向反应气体提供电子的过程。当相互作用发生时，形成一个新的键，这通常会导致母体气体的行为和反应性发生重大改变。在强相互作用的情况下，产物分子可以隔离气体。在弱相互作用的情况下，气体分子的化学性质可能被改变，但气体随后可以被释放，因为它只是弱持有的。在本提案中，我们概述了我们在各种化学环境中探索二氧化碳，二硫化碳，二氧化硫和三氧化硫化学的计划。如上所述，这种化学对我们大规模地了解这些工业气体是很重要的。在新的和不寻常的介质中进行的研究将提供有价值的见解，以了解大自然如何处理这些重要的分子，例如，酶的活性位点，即在更小的范围内。

The chemical behavior of small reactive gases such as carbon dioxide and the sulfur oxides is important on the large-scale vis-à-vis global warming and acid rain. Often overlooked is their role in materials and in biological systems. In order to understand more of this chemistry, we are systematically exploring the reactivity of these small gaseous molecules in a wide variety of environments, including unusual solvents and also within porous materials. This exploration can be guided by the use of coordination chemistry, a process wherein a small molecule or ion donates electrons to the reactive gas. When an interaction occurs a new bond is formed, which often results in significant modification of the behavior and reactivity of the parent gas. In the case of strong interactions, the product molecules can sequester the gas. In the case of weak interactions, the chemistry of the gaseous molecule may be altered but the gas can subsequently be released because it is only weakly held.In this proposal we outline our plan to explore the chemistry of carbon dioxide, carbon disulfide, sulfur dioxide and sulfur trioxide in a wide variety of chemical environments. As mentioned above, this chemistry will be important for our understanding of these industrial gases on a large-scale. The studies in new and unusual media will provide valuable insight as to how nature handles these important molecules within, for example, the active sites of enzymes, i.e., on a much smaller scale.