Lengyel Jozef, Fedor Juraj, Fárník Michal
Lehrstuhl für Physikalische Chemie, Fakultät für Chemie und Zentralinstitut für Katalyseforschung, Technische Universität München, Lichtenbergstraße 4, 85748 Garching, Germany.
Phys Chem Chem Phys. 2019 Apr 24;21(17):8691-8697. doi: 10.1039/c9cp00990f.
We probe the negative ion production upon the interaction of free electrons with gas-phase HNO3 and its mixed clusters with water. The electron-induced chemistry changes strongly with clustering, exhibiting significant electron energy dependence. For HNO3 hydrates, we identified three involved energy ranges with different behavior: low energies up to about 3.5 eV, an intermediate energy range around 6 eV, and a high energy range, approximately above 9 eV. The major difference is the degree to which the major gas-phase product, NO2-, is converted to NO3-. The latter is the dominant stratospheric anion. Its appearance due to the electron interaction with mixed HNO3/water ice particles thus strongly depends on the electron energy. We discuss the elementary processes and reaction pathways behind the anion conversion.
我们探究了自由电子与气相HNO₃及其与水的混合团簇相互作用时负离子的产生情况。电子诱导化学过程随团簇化而强烈变化,表现出显著的电子能量依赖性。对于HNO₃水合物,我们确定了三个具有不同行为的相关能量范围:高达约3.5 eV的低能量范围、约6 eV的中间能量范围以及大约高于9 eV的高能量范围。主要区别在于主要气相产物NO₂⁻转化为NO₃⁻的程度。后者是平流层中的主要阴离子。因此,由于电子与HNO₃/水冰混合颗粒的相互作用而产生的NO₃⁻强烈依赖于电子能量。我们讨论了阴离子转化背后的基本过程和反应途径。