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引用次数: 0
摘要
观测数据显示星际介质(ISM)中存在复杂的有机分子。小的不饱和碳双键的氢化可能是分子复杂化的一种方式。了解这种反应性如何在非常寒冷和低压的 ISM 中发生非常重要。然而,ISM 中存在水冰,要么是晶粒,要么是晶粒周围的地幔。因此,我们研究了在一系列七个分子的双键碳上添加原子氢的情况,发现水催化了这一反应。催化作用的起源是不饱和分子的 π MO 与氢原子之间的微弱电荷转移,从而与 H2O 发生稳定的相互作用。利用非共价相互作用和分子中原子的量子理论方法对这一机制进行了合理解释。
How the addition of atomic hydrogen to a multiple bond can be catalyzed by water molecules
Observational data show complex organic molecules in the interstellar medium (ISM). Hydrogenation of small unsaturated carbon double bond could be one way for molecular complexification. It is important to understand how such reactivity occurs in the very cold and low-pressure ISM. Yet, there is water ice in the ISM, either as grain or as mantle around grains. Therefore, the addition of atomic hydrogen on double-bonded carbon in a series of seven molecules have been studied and it was found that water catalyzes this reaction. The origin of the catalysis is a weak charge transfer between the π MO of the unsaturated molecule and H atom, allowing a stabilizing interaction with H2O. This mechanism is rationalized using the non-covalent interaction and the quantum theory of atoms in molecules approaches.
期刊介绍:
This distinguished journal publishes articles concerned with all aspects of computational chemistry: analytical, biological, inorganic, organic, physical, and materials. The Journal of Computational Chemistry presents original research, contemporary developments in theory and methodology, and state-of-the-art applications. Computational areas that are featured in the journal include ab initio and semiempirical quantum mechanics, density functional theory, molecular mechanics, molecular dynamics, statistical mechanics, cheminformatics, biomolecular structure prediction, molecular design, and bioinformatics.