Qu Yatian, Campbell Patrick G, Hemmatifar Ali, Knipe Jennifer M, Loeb Colin K, Reidy John J, Hubert Mckenzie A, Stadermann Michael, Santiago Juan G
Department of Mechanical Engineering, Stanford University , Stanford, California 94305, United States.
Lawrence Livermore National Laboratory , 7000 East Avenue, Livermore, California, United States.
J Phys Chem B. 2018 Jan 11;122(1):240-249. doi: 10.1021/acs.jpcb.7b09168. Epub 2018 Jan 2.
We present a study of the interplay among electric charging rate, capacitance, salt removal, and mass transport in "flow-through electrode" capacitive deionization (CDI) systems. We develop two models describing coupled transport and electro-adsorption/desorption which capture salt removal dynamics. The first model is a simplified, unsteady zero-dimensional volume-averaged model which identifies dimensionless parameters and figures of merits associated with cell performance. The second model is a higher fidelity area-averaged model which captures both spatial and temporal responses of charging. We further conducted an experimental study of these dynamics and considered two salt transport regimes: (1) advection-limited regime and (2) dispersion-limited regime. We use these data to validate models. The study shows that, in the advection-limited regime, differential charge efficiency determines the salt adsorption at the early stage of the deionization process. Subsequently, charging transitions to a quasi-steady state where salt removal rate is proportional to applied current scaled by the inlet flow rate. In the dispersion-dominated regime, differential charge efficiency, cell volume, and diffusion rates govern adsorption dynamics and flow rate has little effect. In both regimes, the interplay among mass transport rate, differential charge efficiency, cell capacitance, and (electric) charging current governs salt removal in flow-through electrode CDI.
我们展示了一项关于“流通式电极”电容去离子化(CDI)系统中充电速率、电容、盐分去除和传质之间相互作用的研究。我们开发了两个描述耦合传输和电吸附/解吸的模型,这些模型捕捉了盐分去除动力学。第一个模型是一个简化的、非稳态的零维体积平均模型,它确定了与电池性能相关的无量纲参数和品质因数。第二个模型是一个更高保真度的面积平均模型,它捕捉了充电的空间和时间响应。我们进一步对这些动力学进行了实验研究,并考虑了两种盐分传输机制:(1)平流限制机制和(2)扩散限制机制。我们使用这些数据来验证模型。研究表明,在平流限制机制下,差分电荷效率在去离子化过程的早期阶段决定了盐分吸附。随后,充电转变为准稳态,此时盐分去除率与由入口流速缩放的施加电流成正比。在扩散主导机制下,差分电荷效率、电池体积和扩散速率控制吸附动力学,流速影响很小。在这两种机制中,传质速率、差分电荷效率、电池电容和(电)充电电流之间的相互作用决定了流通式电极CDI中的盐分去除。