Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607, Hamburg, Germany.
Institut für Physikalische Chemie, Christian-Albrechts-Universität zu Kiel, Max-Eyth-Str. 1, 24118, Kiel, Germany.
Angew Chem Int Ed Engl. 2023 Mar 27;62(14):e202218539. doi: 10.1002/anie.202218539. Epub 2023 Feb 24.
The initial stages of the gas-phase nucleation between CO and monoethanolamine were investigated via broadband rotational spectroscopy with the aid of extensive theoretical structure sampling. Sub-nanometer-scale aggregation patterns of monoethanolamine-(CO ) , n=1-4, were identified. An interesting competition between the monoethanolamine intramolecular hydrogen bond and the intermolecular interactions between monoethanolamine and CO upon cluster growth was discovered, revealing an intriguing CO binding priority to the hydroxyl group over the amine group. These findings are in sharp contrast to the general results for aqueous solutions. In the quinary complex, a cap-like CO tetramer was observed cooperatively surrounding the monoethanolamine. As the cluster approaches the critical size of new particle formation, the contribution of CO self-assembly to the overall stability increases.
通过宽带旋转光谱学和广泛的理论结构采样,研究了 CO 和单乙醇胺之间的气相成核初始阶段。鉴定了单乙醇胺-(CO)n=1-4 的亚纳米级聚集模式。在簇生长过程中,发现了单乙醇胺分子内氢键与单乙醇胺和 CO 之间的分子间相互作用之间的有趣竞争,揭示了 CO 与羟基的结合优先于与胺基的结合。这些发现与水溶液的一般结果形成鲜明对比。在五元复合物中,观察到帽状 CO 四聚体协同地包围单乙醇胺。随着簇接近新粒子形成的关键尺寸,CO 自组装对整体稳定性的贡献增加。