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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Hydrolysis of Glyoxal in Water-Restricted Environments: Formation of Organic Aerosol Precursors through Formic Acid Catalysis
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Hydrolysis of Glyoxal in Water-Restricted Environments: Formation of Organic Aerosol Precursors through Formic Acid Catalysis

机译：缺水环境中乙二醛的水解：通过甲酸催化形成有机气溶胶前体

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摘要

The hydrolysis of glyoxal involving one to three water molecules and also in the presence of a water molecule and formic acid has been investigated. Our results show that glyoxal-diol is the major product of the hydrolysis and that formic acid, through its ability to facilitate intermolecular hydrogen atom transfer, is considerably more efficient than water as a catalyst in the hydrolysis process. Additionally, once the glyoxal-diol is formed, the barrier for further hydrolysis to form the glyoxal-tetrol is effectively reduced to zero in the presence of a single water and formic acid molecule. There are two important implications arising from these findings. First, the results suggest that under the catalytic influence of formic acid, glyoxal hydrolysis can impact the growth of atmospheric aerosols. As a result of enhanced hydrogen bonding, mediated through their polar OH functional groups, the diol and tetrol products are expected to have significantly lower vapor pressure than the parent glyoxal molecule; hence they can more readily partition into the particle phase and contribute to the growth of secondary organic aerosols. In addition, our findings provide insight into how glyoxal-diol and glyoxal-tetrol might be formed under atmospheric conditions associated with water-restricted environments and strongly suggest that the formation of these precursors for secondary organic aerosol growth is not likely restricted solely to the bulk aqueous phase as is currently assumed.
机译：已经研究了涉及一到三个水分子并且还在水分子和甲酸存在下的乙二醛的水解。我们的结果表明乙二醛二醇是水解的主要产物，而甲酸通过其促进分子间氢原子转移的能力，在水解过程中比水作为催化剂的效率要高得多。另外，一旦形成乙二醛二醇，在单个水和甲酸分子的存在下，用于进一步水解以形成乙二醛-四醇的屏障被有效地降低至零。这些发现产生了两个重要的含义。首先，结果表明在甲酸的催化作用下，乙二醛水解会影响大气气溶胶的生长。由于氢键的极性OH官能团介导的氢键作用增强，因此，二醇和四氢萘酚产品的蒸气压明显低于母体乙二醛分子。因此它们可以更容易地分配到颗粒相中，并有助于二次有机气溶胶的生长。另外，我们的发现提供了关于在与水限制环境相关的大气条件下可能如何形成乙二醛-二醇和乙二醛-四醇的见解，并强烈暗示用于二次有机气溶胶生长的这些前体的形成不可能仅局限于大部分目前假设的水相。

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