Water management is an important factor for optimizing polymer electrolyte fuel cells (PEFC) under high current density conditions as required for the automotive application. The characteristics of the local liquid saturation of the gas diffusion layer (GDL) is of particular interest. Here we report on the development of in-situ X-ray tomographic microscopy (XTM) with a pixel sizes in the order of 2 μm and sensitivity for carbon and liquid water for the quantitative analysis of liquid water in GDLs. In-situ XTM of PEFC is a major experimental challenge. A complete cell needs to be operated under realistic conditions in the constraint space of the small field of view on the beamline sample stage. Further phase segmentation of the images is required to successfully analyze the quantitative properties of the different phases. For this a workflow, applying differential images between dry and wet structures has been developed. Cells with Toray TGP-H-060 GDLs were analyzed in-situ. Droplets that appear on the GDL surface are connected to a significant water structure inside the GDL. Further the water cluster size distribution in the GDL shows that while small droplets (<100 pl) are numerous, most of the water is contained in few larger clusters.
Operating Polymer Electrolyte Fuel Cells (PEFC) under high current density conditions, causes significant losses related to liquid water saturation in the gas diffusion layer (GDL). The blockage of pores inside the material has a strong influence on its effective gas transport properties. Here we report on the combination of in-situ X-ray tomographic microscopy (XTM) of PEFC and the numerical determination of gas transport properties using Lattice Boltzmann and finite difference methods. The GDL domains (Toray TGP-H-060) of two identical cells, each with 11 mm 2 active area, were analyzed in sections of about 0.3 to 0.8 mm 2 size. Saturation levels between 0.1 and 0.4 were found, with higher saturation under the ribs. The saturated and the non-saturated states of the GDL samples were compared in order to quantify the dependence of gas phase permeability and effective relative diffusivity on liquid water saturation. Both these relative measures were found to follow power relationships of (1 − s) λ , where the exponent λ was approximately 3 for all cases except for the in-plane diffusivity where it was closer to 2.Performance of polymer electrolyte fuel cells (PEFC) at high current densities is limited by mass transport losses associated with the presence of liquid water in the porous structures. In the gas diffusion layers (GDL) this issue is particularly relevant.The porous GDL structure allows collecting current under the flow field channels and provides access for the gases under the ribs. 1 This requires a high permeability and relative diffusivity in the pore space and a high conductivity in the solid. GDLs, made from carbon fibers with diameters in the order of typically 6-8 μm, have porosities around 75% and the internal surface is treated with hydrophobing agents. The formation and transport of liquid water in the GDL is thus governed by its internal structure and surface properties, and the presence of liquid water in the pore space of the GDL influences its gas transport properties. At high current density and/or moderate temperature conditions, the oxygen transport in the cathode GDL is particularly affected, which may lead to significant overvoltages. 2,3The effective relative diffusivity of GDLs has been determined with sulphuric acid filled samples and an electrochemical method. 4,5 LaManna et al. 6 have obtained the effective relative diffusivity in a test cell by inducing mass transfer using a concentration gradient of water vapor. These methods however fail to produce saturation dependent results. Opposite to the experimental methods, effective medium theory was used to describe the diffusion through a porous medium consisting of packed spheres. 7 Later, numerical models yielded similar relations particularly for hydrophobic fibrous materials such as the GDL. Tomadakis and Sotirchos 8 used Monte-Carlo simulations in fiber structures and found that the effective relative diffusivity was strongly dependent on the fiber orientation. Nam and Kaviany 9 extended the work of Tomadakis and Sotirchos 8 and...
The basic dynamics of a prolate spheroidal particle suspended in shear flow is studied using lattice Boltzmann simulations. The spheroid motion is determined by the particle Reynolds number (${\mathit{Re}}_{p} $) and Stokes number ($\mathit{St}$), estimating the effects of fluid and particle inertia, respectively, compared with viscous forces on the particle. The particle Reynolds number is defined by ${\mathit{Re}}_{p} = 4G{a}^{2} / \nu $, where $G$ is the shear rate, $a$ is the length of the spheroid major semi-axis and $\nu $ is the kinematic viscosity. The Stokes number is defined as $\mathit{St}= \alpha \boldsymbol{\cdot} {\mathit{Re}}_{p} $, where $\alpha $ is the solid-to-fluid density ratio. Here, a neutrally buoyant prolate spheroidal particle ($\mathit{St}= {\mathit{Re}}_{p} $) of aspect ratio (major axis/minor axis) ${r}_{p} = 4$ is considered. The long-term rotational motion for different initial orientations and ${\mathit{Re}}_{p} $ is explained by the dominant inertial effect on the particle. The transitions between rotational states are subsequently studied in detail in terms of nonlinear dynamics. Fluid inertia is seen to cause several bifurcations typical for a nonlinear system with odd symmetry around a double zero eigenvalue. Particle inertia gives rise to centrifugal forces which drives the particle to rotate with the symmetry axis in the flow-gradient plane (tumbling). At high ${\mathit{Re}}_{p} $, the motion is constrained to this planar motion regardless of initial orientation. At a certain critical Reynolds number, ${\mathit{Re}}_{p} = {\mathit{Re}}_{c} $, a motionless (steady) state is created through an infinite-period saddle-node bifurcation and consequently the tumbling period near the transition is scaled as $\vert {\mathit{Re}}_{p} - {\mathit{Re}}_{c} {\vert }^{- 1/ 2} $. Analyses in this paper show that if a transition from tumbling to steady state occurs at ${\mathit{Re}}_{p} = {\mathit{Re}}_{c} $, then any parameter $\beta $ (e.g. confinement or particle spacing) that influences the value of ${\mathit{Re}}_{c} $, such that ${\mathit{Re}}_{p} = {\mathit{Re}}_{c} $ as $\beta = {\beta }_{c} $, will lead to a period that scales as $\vert \beta - {\beta }_{c} {\vert }^{- 1/ 2} $ and is independent of particle shape or any geometric aspect ratio in the flow.
Bio-based nanocellulose has been shown to possess impressive mechanical properties and simplicity for chemical modifications. The chemical properties are largely influenced by the surface area and functionality of the nanoscale materials. However, finding the typical cross-sections of nanocellulose, such as cellulose nanofibers (CNFs), has been a long-standing puzzle, where subtle changes in extraction methods seem to yield different shapes and dimensions. Here, we extracted CNFs from wood with two different oxidation methods and variations in degree of oxidation and high-pressure homogenization. The cross-sections of CNFs were characterized by small-angle X-ray scattering and wide-angle X-ray diffraction in dispersed and freeze-dried states, respectively, where the results were analyzed by assuming that the cross-sectional distribution was quantized with an 18-chain elementary microfibril, the building block of the cell wall. We find that the results agree well with a pseudosquare unit having a size of about 2.4 nm regardless of sample, while the aggregate level strongly depends on the extraction conditions. Furthermore, we find that aggregates have a preferred cohesion of phase boundaries parallel to the (110)-plane of the cellulose fibril, leading to a ribbon shape on average.
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