Journet E, Le Calvé S, Mirabel Ph
Centre de Géochimie de la Surface / CNRS and Université Louis Pasteur, 1 rue Blessig, F-67084 Strasbourg Cedex, France.
J Phys Chem B. 2005 Jul 28;109(29):14112-7. doi: 10.1021/jp051524u.
Adsorption studies of acetone on pure ice surfaces obtained by water freezing or deposition or on frozen ice surfaces doped either with HNO3 or H2SO4 have been performed using a coated wall flow tube coupled to a mass spectrometric detection. The experiments were conducted over the temperature range 203-233 K and freezing solutions containing either H2SO4 (0.2 N) or HNO3 (0.2-3 N). Adsorption of acetone on these ice surfaces was always found to be totally reversible whatever were the experimental conditions. The number of acetone molecules adsorbed per ice surface unit N was conventionally plotted as a function of acetone concentration in the gas phase. For the same conditions, the amount of acetone molecules adsorbed on pure ice obtained by deposition are about 3-4 times higher than those measured on frozen ice films, H2SO4-doped ice surfaces lead to results comparable to those obtained on pure ice. On the contrary, N increases largely with increasing concentrations of nitric acid in ice surfaces, up to about 300 times under our experimental conditions and for temperatures ranging between 213 and 233 K. Finally, the results are discussed and used to reestimate the partitioning of acetone between the ice and gas phases in clouds of the upper troposphere.
利用与质谱检测联用的涂壁流动管,对通过水冻结、沉积获得的纯冰表面,或掺杂了HNO₃或H₂SO₄的冻结冰表面上丙酮的吸附进行了研究。实验在203 - 233 K的温度范围内进行,使用含有H₂SO₄(0.2 N)或HNO₃(0.2 - 3 N)的冷冻溶液。无论实验条件如何,始终发现丙酮在这些冰表面上的吸附是完全可逆的。通常将每单位冰表面吸附的丙酮分子数N绘制为气相中丙酮浓度的函数。在相同条件下,通过沉积获得的纯冰上吸附的丙酮分子数量比在冷冻冰膜上测得的高出约3 - 4倍,掺杂H₂SO₄的冰表面得到的结果与在纯冰上获得的结果相当。相反,随着冰表面硝酸浓度的增加,N大幅增加,在我们的实验条件下以及213至233 K的温度范围内,增加高达约300倍。最后,对结果进行了讨论,并用于重新估计对流层上部云层中丙酮在冰相和气相间的分配情况。