Potential enhancement in atmospheric new particle formation by amine-assisted nitric acid condensation at room temperature
Potential enhancement in atmospheric new particle formation by amine-assisted nitric acid condensation at room temperature
复制标题
室温下胺辅助硝酸缩合可能增强大气新颗粒的形成
DOI：
10.1016/j.atmosenv.2022.119252
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发表时间：
2022
影响因子：
5
通讯作者：
Qiu, Chong
中科院分区：
文献类型：
--
作者：
Chen, Kuanfu;Zhang, Kai;Qiu, Chong
大气气溶胶在全球气候和公众健康中起着至关重要的作用。最近的实验室实验表明，在低温下硝酸和氨的快速冷凝显著增强了新颗粒的形成。胺是氨的衍生物，在大气中大量存在。例如，基于胺的燃烧后碳捕获（PCCC）单元的广泛实施可显著增加环境烷醇胺和多胺水平。利用热力学模拟，系统地评价了烷基胺、烷醇胺和多胺与硝酸在不同温度下的缩合反应。在与氨相当的温度下，烷基胺将与硝酸缩合。然而，与额外的氢键基团，链烷醇胺和多胺可以在室温下与硝酸缩合，这表明一个新的潜在途径，以消除这些胺从大气中。我们的研究结果表明，潜在的关键作用，胺在大气中的新粒子的形成，通过冷凝与硝酸快速增长的新鲜成核簇超过其临界尺寸在更高的温度比氨。缩合胺和硝酸也可以促进水的吸收气溶胶颗粒在低相对湿度，这可能会改变其随后的大气转化。
Atmospheric aerosol plays a critical role in global climate and public health. Recent laboratory experiments showed that new particle formation is significantly enhanced by rapid condensation of nitric acid and ammonia at low temperatures. Amines are derivatives of ammonia with a significant presence in the atmosphere. For example, the wide implementation of amine-based Post-Combustion Carbon Capture (PCCC) units may significantly increase the ambient alkanolamine and polyamine levels. Using thermodynamic simulations, the condensation of alkylamines, alkanolamines and polyamines with nitric acid at various temperatures was systematically evaluated. Alkylamines will condense with nitric acid at temperatures comparable to that of ammonia. However, with additional hydrogen bonding groups, alkanolamines and polyamines may condense with nitric acid at room temperature, suggesting a new potential pathway to remove these amines from the atmosphere. Our results suggest the potentially critical role of amines in the atmospheric new particle formation via condensation with nitric acid to rapidly grow freshly nucleated clusters over their critical size at a higher temperature than ammonia. The condensed amines and nitric acid can also facilitate water uptake by aerosol particles at low relative humidity, which may alter their subsequent atmospheric transformations.