Bubbles in Porous Electrodes for Alkaline Water Electrolysis.

Porous electrodes with high specific surface areas have been commonly employed for alkaline water electrolysis. The gas bubbles generated in electrodes due to water electrolysis, however, can screen the reaction sites and hinder reactant transport, thereby deteriorating the performance of electrodes. Hence, an in-depth understanding of the behavior of bubbles in porous electrodes is of great importance. Nevertheless, since porous electrodes are opaque, direct observation of bubbles therein is still a challenge. In this work, we have successfully captured the behavior of bubbles in the pores at the side surfaces of nickel-based porous electrodes. Two types of porous electrodes are employed: the ones with straight pores along the gravitational direction and the ones with tortuous pores. In the porous electrodes with tortuous pores, the moving bubbles are prone to collide with the solid matrix, thereby leading to the accumulation of bubbles in the pores and hence bubble trapping. By contrast, in the porous electrodes with straight pores, bubbles are seldom trapped; and when two bubbles near the wall surfaces coalesce, the merged bubble can jump away from the wall surfaces, releasing more active surfaces for reaction. As a result, the porous electrodes with straight pores, although with lower specific surface areas, are superior to those with tortuous pores. The relationship among the pore structures of porous electrodes, bubble behavior, and electrode performance disclosed in this work provides deep insights into the design of porous electrodes.

Spontaneous Imbibition in Paper-Based Microfluidic Devices: Experiments and Numerical Simulations.

Microfluidic paper-based analytical devices (µPADs) have quickly been an excellent choice for point-of-care diagnostic platforms ever since they appeared. Because capillary force is the main driving force for the transport of analytes in µPADs, low spontaneous imbibition rates may limit the detection sensitivity. Therefore, quantitative understanding of internal spontaneous capillary flow progress is requisite for designing sensitive and accurate µPADs. In this work, experimental and numerical studies have been performed to investigate the capillary flow in a typical filter paper. We use light-transmitting imaging technology to study wetting saturation changes in the paper. Our experimental results show an obvious transition of a saturated wetting front into an unsaturated wetting front as the imbibition proceeds. We find that the single-phase Darcy model considerably overestimates the temporal wetting penetration depths. Alternatively, we use the Richards equation together with the two-phase flow material properties that are obtained from the image-based pore-network modeling of the filter paper. Moreover, we have considered a dynamic term in the capillary pressure due to strong wetting dynamics in spontaneous imbibition. As a result, the numerical predictions of spontaneous imbibition in the paper are significantly improved. Our studies provide insights into the development of a quantitative spontaneous imbibition model for µPADs applications.

Experimental Investigation of Hysteretic Dynamic Capillarity Effect in Unsaturated Flow.

The difference between average pressures of two immiscible fluids is commonly assumed to be the same as macroscopic capillary pressure, which is considered to be a function of saturation only. However, under transient conditions, a dependence of this pressure difference on the time rate of saturation change has been observed by many researchers. This is commonly referred to as dynamic capillarity effect. As a first-order approximation, the dynamic term is assumed to be linearly dependent on the time rate of change of saturation, through a material coefficient denoted by τ. In this study, a series of laboratory experiments were carried out to quantify the dynamic capillarity effect in an unsaturated sandy soil. Primary, main, and scanning drainage experiments, under both static and dynamic conditions, were performed on a sandy soil in a small cell. The value of the dynamic capillarity coefficient τ was calculated from the air-water pressure differences and average saturation values during static and dynamic drainage experiments. We found a dependence of τ on saturation, which showed a similar trend for all drainage conditions. However, at any given saturation, the value of τ for primary drainage was larger than the value for main drainage and that was in turn larger than the value for scanning drainage. Each data set was fit a simple log-linear equation, with different values of fitting parameters. This nonuniqueness of the relationship between τ and saturation and possible causes is discussed.

Relating Darcy-Scale Chemical Reaction Order to Pore-Scale Spatial Heterogeneity.

Due to spatial scaling effects, there is a discrepancy in mineral dissolution rates measured at different spatial scales. Many reasons for this spatial scaling effect can be given. We investigate one such reason, i.e., how pore-scale spatial heterogeneity in porous media affects overall mineral dissolution rates. Using the bundle-of-tubes model as an analogy for porous media, we show that the Darcy-scale reaction order increases as the statistical similarity between the pore sizes and the effective-surface-area ratio of the porous sample decreases. The analytical results quantify mineral spatial heterogeneity using the Darcy-scale reaction order and give a mechanistic explanation to the usage of reaction order in Darcy-scale modeling. The relation is used as a constitutive relation of reactive transport at the Darcy scale. We test the constitutive relation by simulating flow-through experiments. The proposed constitutive relation is able to model the solute breakthrough curve of the simulations. Our results imply that we can infer mineral spatial heterogeneity of a porous media using measured solute concentration over time in a flow-through dissolution experiment.