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Heterogeneous Reactivity of HCl on CaCO3 Aerosols at Stratospheric Temperature
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2021-07-29 , DOI: 10.1021/acsearthspacechem.1c00151
Han N. Huynh 1 , V. Faye McNeill 1, 2
Affiliation  

Recently proposed as a possible alternative to sulfate particles for stratospheric solar radiation management (SSRM), calcite (CaCO3) aerosols have been modeled to have minimal negative impact on both stratospheric ozone level, through heterogeneous chemistry, and stratospheric temperature. However, the heterogeneous chemistry of CaCO3 aerosols with relevant trace gases, such as HCl, at stratospheric conditions is still underexamined. We studied the kinetics of HCl uptake on airborne CaCO3 aerosols at stratospheric temperature, 207 ± 3 K, by performing experiments under dry conditions using an aerosol flow tube coupled with a custom-built quadrupole chemical ionization mass spectrometer (CIMS) for HCl detection. The reactive uptake coefficient for HCl was measured to be 0.076 ± 0.009. This exceeds the reactive uptake coefficient of 0.013 ± 0.001 that we previously reported for this system at 296 K, consistent with the expected negative temperature dependence of gas uptake on solid surfaces. This finding suggests an initial strong reactive uptake of HCl gas on CaCO3 aerosol surfaces in the stratosphere.

中文翻译:

在平流层温度下 HCl 对 CaCO3 气溶胶的非均相反应性

最近提出作为用于平流层太阳辐射管理 (SSRM) 的硫酸盐颗粒的可能替代品,方解石 (CaCO 3 ) 气溶胶已被建模为通过异质化学和平流层温度对平流层臭氧水平的负面影响最小。然而,在平流层条件下,CaCO 3气溶胶与相关痕量气体(如 HCl)的非均相化学仍未得到充分研究。我们研究了空气中 CaCO 3吸收 HCl 的动力学通过在干燥条件下使用气溶胶流管和定制的四极杆化学电离质谱仪 (CIMS) 进行 HCl 检测,在 207 ± 3 K 的平流层温度下进行气溶胶检测。测量的 HCl 反应吸收系数为 0.076 ± 0.009。这超过了我们之前在 296 K 下为该系统报告的反应吸收系数 0.013 ± 0.001,与固体表面上气体吸收的预期负温度依赖性一致。这一发现表明在平流层的CaCO 3气溶胶表面上 HCl 气体的初始强反应性吸收。
更新日期:2021-08-19
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