CO2吸收过程中气相分压对Rayleigh对流传质特性的影响

doi:10.16085/j.issn.1000-6613.2023-0224

摘要/Abstract

摘要：

界面浓度梯度导致的Rayleigh对流现象能够显著提高CO₂吸收过程的传质速率，然而目前该过程的传质强化机制尚未清晰。为探究Rayleigh对流传质过程的强化机制，本文以水吸收CO₂过程为研究对象，基于粒子图像测速技术（PIV）和激光诱导荧光技术（LIF）实现了不同气相CO₂分压条件下界面对流的可视化与定量测量。实验发现，界面平均浓度在对流发生的临界时刻会瞬间下降并在有序的自组织结构形成后上升，最终的界面平均浓度会随着气相CO₂分压减小而减小；对流发生后，系统传质能力的提高分为两个阶段，涡量场在有序的自组织结构形成前起主导作用，有序的自组织结构形成后，系统传质能力的提高则是由涡量场与界面浓度共同作用的结果；有序的自组织结构形成后，不同系统的平均瞬时传质系数与平均涡量具有很强的相关性，表明浓度场与速度场相互作用形成的涡量场在对流传质强化过程中发挥着重要作用。

关键词: 二氧化碳捕集, Rayleigh对流, 传质, 激光诱导荧光, 粒子图像测速

Abstract:

Rayleigh convection phenomenon caused by interfacial concentration gradient can significantly improve the mass transfer rate of CO₂ absorption process, but the mechanism of mass transfer enhancement in this process is not clear at present. In order to explore the enhancement mechanism of Rayleigh convection mass transfer process, water absorbing CO₂ process was selected as the research object, and realized the visualization and quantitative measurement of interfacial convection based on particle image velocimetry (PIV) and laser induced fluorescence (LIF) technology under different CO₂ partial pressure conditions. It was found that the average interface concentration would drop instantaneously at the critical time of the convection and would rise after the formation of the ordered self-organization structure, the final average interface concentration would descend with the decrease of CO₂ partial pressure in gas phase. After convection, the mass transfer capacity enhancement of the system was divided into two stages, vorticity field played a leading role before the formation of the ordered self-organization structure, but after the formation of the ordered self-organization structure, the mass transfer capacity enhancement was the result of the joint action of vorticity field and interface concentration. After the formation of the ordered self-organization structure, the average instantaneous mass transfer coefficients of different systems had a strong correlation with the corresponding average vorticity, indicating that the vorticity field formed by the interaction of concentration field and velocity field played an important role in the process of convective mass transfer enhancement.

Key words: CO₂capture, Rayleigh convection, mass transfer, laser induced fluorescence, particle image velocimetry

中图分类号:

TQ021.4

张瑞凯, 张会书, 郑龙云, 曾爱武. CO₂吸收过程中气相分压对Rayleigh对流传质特性的影响[J]. 化工进展, 2024, 43(2): 913-924.

ZHANG Ruikai, ZHANG Huishu, ZHENG Longyun, ZENG Aiwu. Effect of gas partial pressure on Rayleigh convection mass transfer characteristics during CO₂ absorption[J]. Chemical Industry and Engineering Progress, 2024, 43(2): 913-924.

图/表 13

图1 实验装置1—N2气瓶；2—CO2气瓶；3，4，8—气体流量计；5，6—预饱和罐；7—气体混合器；9—比例-积分-微分（PID）温度控制器；10—气液传质装置；11—Nd:YAG激光器；12—光学镜组；13，14—CCD相机；15—计算机

图2 气液传质装置示意图

表1 不同气相CO2分压传质条件对应的Ra数

气相CO₂分压/kPa	Ra数
101	1.54×10⁹
72.1	1.10×10⁹
57.7	0.88×10⁹
43.3	0.66×10⁹
28.8	0.44×10⁹
14.4	0.22×10⁹

图3 荧光强度与CO2浓度关系曲线

表2 H2O-CO2体系在298.15K、101.325kPa下的物性参数

∆ρ_sat^[5,32-34]/kg·m^-3	∆σ_sat^[5]/N·m^-1	D^[35]/m²·s^-1	μ^[35]/Pa·s
0.40	-5×10^-5	1.97×10^-9	8.8×10^-4

图4 气相CO2分压p=101kPa条件下不同时刻的CO2浓度及速度分布

图5 不同气相CO2分压条件下t=300s时刻的CO2浓度及速度分布

图6 水吸收CO2过程中的界面浓度变化

图7 水吸收CO2过程中液相主体不同横截面上的平均浓度分布

图8 气相CO2分压p=101kPa条件下不同时刻的液相涡量分布

图9 不同气相CO2分压条件下的液相平均涡量

图10 不同气相CO2分压条件下的瞬时传质系数

图11 平均涡量与平均瞬时传质系数的耦合关系曲线

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CO₂吸收过程中气相分压对Rayleigh对流传质特性的影响

Effect of gas partial pressure on Rayleigh convection mass transfer characteristics during CO₂ absorption

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