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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Equilibrium Partial Pressures, Thermodynamic Properties of Aqueous and Solid Phases, and Cl_2 Production from Aqueous HCl and HNO_3 and Their Mixtures
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Equilibrium Partial Pressures, Thermodynamic Properties of Aqueous and Solid Phases, and Cl_2 Production from Aqueous HCl and HNO_3 and Their Mixtures

机译：平衡分压，水相和固相的热力学性质以及HCl和HNO_3水溶液及其混合物产生的Cl_2

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Equilibrium total pressures have been measured above aqueous HNO_3 (for 7.82, 15.73, and 35.99 mol kg~(-1) solutions from 294.6 to 224.7 K) and aqueous HCl (9.45 and 10.51 mol kg~(-1), from 289.4 to 199.5 K) using a capacitance manometer. Equilibrium partial pressures of the acids have also been determined, by mass spectrometry, from 274.8 to 234.6 K for both HCl solutions, and from 265.0 to 240.1 K for 15.73 mol kg~(-1) HNO_3. Results are generally consistent with model predictions, though with small (approx 10%) systematic deviations for the total pressure measurements over aqueous HCl at about 220 K. Mixtures of HCl-HNO_3-H_2O composition yielded measured total pressures orders of magnitude greater than predicted for the gases H_2O, HNO_3, and HCl. Mass spectrometric determinations and equilibrium thermodynamic calculations suggest that Cl_2 and NOCl were produced by the reaction: 4H~+_(aq) + NO_(3~-)_(aq) + 3Cl~-_(aq) mutually impiles NOCl_(aq) + Cl_(2(aq)) + 2H_2O_(1), which is known to occur in aqua regia (a mixture of concentrated hydrochloric and nitric acids). Calculations for aqueous solutions of stratospheric aerosol composition suggest, purely on equilibrium grounds (and neglecting kinetics), that the reaction could be a source of active chlorine in the stratosphere. The correlation of Clegg and Brimblecombe (J. Phys. Chem. 1990, 94, 5369-5380; and 1994, 96, 6854) of the thermodynamic properties of aqueous HNO_3 activities has been revised, and vapor pressure products (for the reaction HNO_3 centre dot nH_2O_(cr) mutually impiles HNO_(3(g)) + nH_2O_(g), where 1 <= n <= 3) assessed from literature studies. The activity product for the reaction HNO_3 centre dot 2H_2O_(cr) mutually impiles H_(aq)~+ + NO_(3~-)_(aq) + 2H_2O_(1) has also been determined. The model of Carslaw et al. (J. Phys. Chem. 1995, 99, 11557-11574) has been revised for the solubility of HBr in aqueous H_2SO_4 to stratospheric temperatures.
机译：在HNO_3水溶液（对于29.4.6至224.7 K的7.82、15.73和35.99 mol kg〜（-1）溶液）和HCl水溶液（289.4至199.5的9.45％和10.51 mol kg〜（-1））上测量了平衡总压力。 K）使用电容压力计。酸的平衡分压也已通过质谱法确定，对于两种HCl溶液，从274.8至234.6 K，对于15.73 mol kg〜（-1）HNO_3，从265.0至240.1K。结果通常与模型预测相符，尽管在约220 K的HCl水溶液上进行总压力测量时，系统偏差很小（约10％）。HCl-HNO_3-H_2O成分的混合物产生的测得总压力比预测值大几个数量级。气体H_2O，HNO_3和HCl。质谱测定和平衡热力学计算表明，Cl_2和NOCl是通过以下反应生成的：4H〜+ _（aq）+ NO_（3〜-）_（aq）+ 3Cl〜-__（aq）相互推动NOCl_（aq） + Cl_（2（aq））+ 2H_2O_（1），已知发生在王水（浓盐酸和硝酸的混合物）中。平流层气溶胶成分水溶液的计算表明，纯粹出于平衡的考虑（并忽略动力学），该反应可能是平流层中活性氯的来源。修改了Clegg和Brimblecombe（J. Phys。Chem。1990，94，5369-5380;和1994，96，6854）的水溶液HNO_3活性的热力学性质的相关性，蒸气压产物（用于反应HNO_3中心）点nH_2O_（cr）相互推动HNO_（3（g））+ nH_2O_（g），其中1 <= n <= 3）是根据文献研究得出的。还确定了反应HNO_3中心点2H_2O_（cr）相互推动H_（aq）〜+ + NO_（3〜-）_（aq）+ 2H_2O_（1）的活性产物。 Carslaw等人的模型。 （J. Phys。Chem。1995，99，11557-11574）已针对HBr在H_2SO_4水溶液中至平流层温度的溶解度进行了修订。

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