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单乙醇胺水溶液脱除羰基硫的动力学

Kinetics of removal of carbonyl sulfide by aqueous monoethanolamine.

作者信息

Lee S C, Snodgrass M J, Park M K, Sandall O C

机构信息

Department of Chemical Engineering, Kunsan National University, Miryong Dong, Kunsan, Chonbuk 573-701, South Korea.

出版信息

Environ Sci Technol. 2001 Jun 1;35(11):2352-7. doi: 10.1021/es0017312.

Abstract

The kinetics of the reaction between carbonyl sulfide and aqueous monoethanolamine (MEA) were studied over a range in temperature (298-348 K) and amine concentrations (5-20 wt%) using a wetted-sphere absorber. The experimental data were interpreted using a zwitterion mechanism. The key physicochemical properties needed to interpret the data are the solubility and diffusivity of COS in the aqueous amine solution. These properties were estimated using the N2O analogy method. Experimental values of N2O solubility were correlated using an extended scaled-particle model, and the measured N2O diffusion coefficients were correlated using a modified Stokes-Einstein equation. Solution densities and viscosities were also measured and correlated in this work. On the basis of the zwitterion mechanism whose rate-limiting step was the deprotonation of a zwitterion, the Arrhenius relationship between the third-order rate constant and the temperature was well correlated with an absolute mean deviation of 0.3%. It could be thus concluded that the overall reaction rate was first-order in the COS concentration and second-order in the MEA concentration.

摘要

使用湿球吸收器,在温度范围为298 - 348K和胺浓度为5 - 20 wt%的条件下,研究了羰基硫与单乙醇胺(MEA)水溶液之间反应的动力学。实验数据采用两性离子机理解释。解释这些数据所需的关键物理化学性质是COS在胺水溶液中的溶解度和扩散系数。这些性质采用N₂O类比法估算。N₂O溶解度的实验值使用扩展的尺度粒子模型进行关联,测量的N₂O扩散系数使用修正的斯托克斯 - 爱因斯坦方程进行关联。本研究还测量并关联了溶液的密度和粘度。基于以两性离子去质子化为限速步骤的两性离子机理,三阶速率常数与温度之间的阿伦尼乌斯关系得到了很好的关联,绝对平均偏差为0.3%。因此可以得出结论,总反应速率对COS浓度为一级,对MEA浓度为二级。

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