摘要
氢气驱动的电化学CO_(2)捕集系统(hydrogen-driven electrochemical carbon capture system,HECCS)因低能耗和高选择性等特性受到广泛关注。HECCS中多离子耦合传输与电流密度、捕集浓度及温度等操作参数的定量关联是厘清其捕碳机制的关键。基于Maxwell-Stefan扩散方程,建立了HECCS系统捕碳过程中考虑多离子耦合传输的传质-电场耦合多物理场模型。研究表明,所建立模型可以有效地模拟HECCS系统中的多离子传输过程。通过对膜电极内p H分布、电解质电势及OH^(-)、HCO_(3)^(-)和CO_(3)^(2-)传输过程耦合特性的分析,厘清了不同操作参数下捕碳性能的速率限制步骤,获得了操作参数和关键控制因素对HECCS捕集通量和电子效率的影响规律。研究可为电化学CO_(2)捕集系统的性能提升和优化设计提供理论分析和计算依据。
Hydrogen-driven electrochemical carbon capture systems(HECCS)have been widely attracted attention due to their low energy consumption and high selectivity.Establishing a quantitative relationship between the multiple ions coupled transport mechanisms in HECCS and operating parameters such as current density,capture concentration,and temperature is the key to elucidating the underlying carbon capture mechanisms.Based on the Maxwell-Stefan diffusion equation,this paper establishes a mass transfer-electric field coupled multiphysics model for the carbon capture process in the HECCS system,taking into account multi-ion coupling transport.The results show that the proposed model can effectively simulate the multiple ions transport in the HECCS system.By analyzing the coupled behaviors of pH distribution,electrolyte potential,and the transport of OH^(-),HCO_(3)^(-)and CO_(2)^(3-)ions within the membrane electrode assembly,the rate-limiting steps under different operating conditions are identified.The influences of various operational parameters and key controlling factors on CO_(2)capture flux and faradaic efficiency are determined,clarifying the mechanisms by which operating conditions affect carbon capture performance.This work provides a theoretical and computational foundation for the performance improvement and optimal design of electrochemical CO_(2)capture system.
作者
李一白
刘世昌
王靖
刘永忠
LI Yibai;LIU Shichang;WANG Jing;LIU Yongzhong(Department of Chemical Engineering,Xi’an Jiaotong University,Xi’an 710049,Shaanxi,China;Engineering Research Center of New Energy System Engineering and Equipment,University of Shaanxi Province,Xi’an 710049,Shaanxi,China)
出处
《化工学报》
北大核心
2025年第11期5951-5964,共14页
CIESC Journal
基金
国家自然科学基金重点项目(22238006)和联合基金项目(U24B6016)
陕西省重点研发计划项目(2025CY-YBXM-183)
能源陕西实验室科技项目(ESLB202411)
中国博士后基金项目(2025M771171)。
