In silico model development and optimization of in vitro lung cell population growth.

Tissue engineering predominantly relies on trial and error in vitro and ex vivo experiments to develop protocols and bioreactors to generate functional tissues. As an alternative, in silico methods have the potential to significantly reduce the timelines and costs of experimental programs for tissue engineering. In this paper, we propose a methodology to formulate, select, calibrate, and test mathematical models to predict cell population growth as a function of the biochemical environment and to design optimal experimental protocols for model inference of in silico model parameters. We systematically combine methods from the experimental design, mathematical statistics, and optimization literature to develop unique and explainable mathematical models for cell population dynamics. The proposed methodology is applied to the development of this first published model for a population of the airway-relevant bronchio-alveolar epithelial (BEAS-2B) cell line as a function of the concentration of metabolic-related biochemical substrates. The resulting model is a system of ordinary differential equations that predict the temporal dynamics of BEAS-2B cell populations as a function of the initial seeded cell population and the glucose, oxygen, and lactate concentrations in the growth media, using seven parameters rigorously inferred from optimally designed in vitro experiments.

Investigating the Influence of Treatments on Carbon Felts for Vanadium Redox Flow Batteries.

Vanadium redox flow battery (VRFB) electrodes face challenges related to their long-term operation. We investigated different electrode treatments mimicking the aging processes during operation, including thermal activation, aging, soaking, and storing. Several characterization techniques were used to deepen the understanding of the treatment of carbon felts. Synchrotron X-ray imaging, electrochemical impedance spectroscopy (EIS) with the distribution of relaxation times analysis, and dynamic vapor sorption (DVS) revealed differences between the wettability of felts. The bulk saturation after electrolyte injection into the carbon felts significantly differed from 8 % to 96 %. DVS revealed differences in the sorption/desorption behavior of carbon felt ranging from a slight change of 0.8 wt % to over 100 wt %. Additionally, the interactions between the water vapor and the sample change from type V to type H2. After treatment, morphology changes were observed by atomic force microscopy and scanning electron microscopy. Cyclic voltammetry and EIS were used to probe the electrochemical performance, revealing different catalytic activities and transport-related impedances for the treated samples. These investigations are crucial for understanding the effects of treatments on the performance and optimizing materials for long-term operation.

Simultaneous multimaterial operando tomography of electrochemical devices.

The performance of electrochemical energy devices, such as fuel cells and batteries, is dictated by intricate physiochemical processes within. To better understand and rationally engineer these processes, we need robust operando characterization tools that detect and distinguish multiple interacting components/interfaces in high contrast. Here, we uniquely combine dual-modality tomography (simultaneous neutron and x-ray tomography) and advanced image processing (iterative reconstruction and metal artifact reduction) for high-contrast multimaterial imaging, with signal and contrast enhancements of up to 10 and 48 times, respectively, compared to conventional single-modality imaging. Targeted development and application of these methods to electrochemical devices allow us to resolve operando distributions of six interacting fuel cell components (including void space) with the highest reported pairwise contrast for simultaneous yet decoupled spatiotemporal characterization of component morphology and hydration. Such high-contrast tomography ushers in key gold standards for operando electrochemical characterization, with broader applicability to numerous multimaterial systems.

Revealing the Multifaceted Impacts of Electrode Modifications for Vanadium Redox Flow Battery Electrodes.

Carbon electrodes are one of the key components of vanadium redox flow batteries (VRFBs), and their wetting behavior, electrochemical performance, and tendency to side reactions are crucial for cell efficiency. Herein, we demonstrate three different types of electrode modifications: poly(o-toluidine) (POT), Vulcan XC 72R, and an iron-doped carbon-nitrogen base material (Fe-N-C + carbon nanotube (CNT)). By combining synchrotron X-ray imaging with traditional characterization approaches, we give thorough insights into changes caused by each modification in terms of the electrochemical performance in both half-cell reactions, wettability and permeability, and tendency toward the hydrogen evolution side reaction. The limiting performance of POT and Vulcan XC 72R could mainly be ascribed to hindered electrolyte transport through the electrode. Fe-N-C + CNT displayed promising potential in the positive half-cell with improved electrochemical performance and wetting behavior but catalyzed the hydrogen evolution side reaction in the negative half-cell.

Cell Inertia: Predicting Cell Distributions in Lung Vasculature to Optimize Re-endothelialization.

We created a transient computational fluid dynamics model featuring a particle deposition probability function that incorporates inertia to quantify the transport and deposition of cells in mouse lung vasculature for the re-endothelialization of the acellular organ. Our novel inertial algorithm demonstrated a 73% reduction in cell seeding efficiency error compared to two established particle deposition algorithms when validated with experiments based on common clinical practices. We enhanced the uniformity of cell distributions in the lung vasculature by increasing the injection flow rate from 3.81 ml/min to 9.40 ml/min. As a result, the cell seeding efficiency increased in both the numerical and experimental results by 42 and 66%, respectively.

Vessel network extraction and analysis of mouse pulmonary vasculature via X-ray micro-computed tomographic imaging.

In this work, non-invasive high-spatial resolution three-dimensional (3D) X-ray micro-computed tomography (µCT) of healthy mouse lung vasculature is performed. Methodologies are presented for filtering, segmenting, and skeletonizing the collected 3D images. Novel methods for the removal of spurious branch artefacts from the skeletonized 3D image are introduced, and these novel methods involve a combination of distance transform gradients, diameter-length ratios, and the fast marching method (FMM). These new techniques of spurious branch removal result in the consistent removal of spurious branches without compromising the connectivity of the pulmonary circuit. Analysis of the filtered, skeletonized, and segmented 3D images is performed using a newly developed Vessel Network Extraction algorithm to fully characterize the morphology of the mouse pulmonary circuit. The removal of spurious branches from the skeletonized image results in an accurate representation of the pulmonary circuit with significantly less variability in vessel diameter and vessel length in each generation. The branching morphology of a full pulmonary circuit is characterized by the mean diameter per generation and number of vessels per generation. The methods presented in this paper lead to a significant improvement in the characterization of 3D vasculature imaging, allow for automatic separation of arteries and veins, and for the characterization of generations containing capillaries and intrapulmonary arteriovenous anastomoses (IPAVA).

Degradation Characteristics of Electrospun Gas Diffusion Layers with Custom Pore Structures for Polymer Electrolyte Membrane Fuel Cells.

Electrospinning has been demonstrated to be a versatile technique for producing hydrophobic gas diffusion layers (GDLs) with customized pore structures for the enhanced performance of polymer electrolyte membrane (PEM) fuel cells. However, the degradation characteristics of custom hydrophobic electrospun GDLs (eGDLs) have not yet been explored. Here, for the first time, we investigate the degradation characteristics of custom hydrophobic eGDLs via an ex situ accelerated degradation protocol using H2O2. The surface contact angle of degraded eGDLs (44 ± 12°) was lower than that of pristine eGDLs (137 ± 6°). The loss of hydrophobicity was attributed to the degradation (via hydrolysis) of the fluorinated monolayers (formed via a direct fluorination treatment) on the electrospun carbon fiber surfaces as evidenced by the reduction in surface fluorine content. Degradation of the surface monolayers affected fuel cell performance under multiple operating conditions. At 100% relative humidity (RH), the loss of monolayers led to higher liquid water content and lower cell voltages compared to the pristine eGDL. At 50% RH, the degraded eGDL led to lower cell voltages due to the lower electrical conductivity of the degraded materials. The lower electrical conductivity was attributed to the oxidation of carbon fibers upon loss of the monolayers. Our results indicate the importance of designing robust hydrophobic surface treatments for the advancement of customized GDLs for effective long-term fuel cell operation.

Boosting Membrane Hydration for High Current Densities in Membrane Electrode Assembly CO2 Electrolysis.

Despite the advantages of CO2 electrolyzers, efficiency losses due to mass and ionic transport across the membrane electrode assembly (MEA) are critical bottlenecks for commercial-scale implementation. In this study, more efficient electrolysis of CO2 was achieved by increasing cation exchange membrane (CEM) hydration via the humidification of the CO2 reactant inlet stream. A high current density of 755 mA/cm2 was reached by humidifying the reactant CO2 in a MEA electrolyzer cell featuring a CEM. The power density was reduced by up to 30% when the fully humidified reactant CO2 was introduced while operating at a current density of 575 mA/cm2. We reduced the ohmic losses of the electrolyzer by fourfold at 575 mA/cm2 by fully humidifying the reactant CO2. A semiempirical CEM water uptake model was developed and used to attribute the improved performance to 11% increases in membrane water uptake and ionic conductivity. Our CEM water uptake model showed that the increase in ohmic losses and the limitation of ionic transport were the result of significant dehydration at the central region of the CEM and the anode gas diffusion electrode-CEM interface region, which exhibited a 2.5% drop in water uptake.

Bubble Formation in the Electrolyte Triggers Voltage Instability in CO2 Electrolyzers.

The electrochemical reduction of CO2 is promising for mitigating anthropogenic greenhouse gas emissions; however, voltage instabilities currently inhibit reaching high current densities that are prerequisite for commercialization. Here, for the first time, we elucidate that product gaseous bubble accumulation on the electrode/electrolyte interface is the direct cause of the voltage instability in CO2 electrolyzers. Although bubble formation in water electrolyzers has been extensively studied, we identified that voltage instability caused by bubble formation is unique to CO2 electrolyzers. The appearance of syngas bubbles within the electrolyte at the gas diffusion electrode (GDE)-electrolyte chamber interface (i.e. ∼10% bubble coverage of the GDE surface) was accompanied by voltage oscillations of 60 mV. The presence of syngas in the electrolyte chamber physically inhibited two-phase reaction interfaces, thereby resulting in unstable cell performance. The strategic incorporation of our insights on bubble growth behavior and voltage instability is vital for designing commercially relevant CO2 electrolyzers.

Synchrotron X-ray Radiography and Tomography of Vanadium Redox Flow Batteries-Cell Design, Electrolyte Flow Geometry, and Gas Bubble Formation.

The wetting behavior and affinity to side reactions of carbon-based electrodes in vanadium redox flow batteries (VRFBs) are highly dependent on the physical and chemical surface structures of the material, as well as on the cell design itself. To investigate these properties, a new cell design was proposed to facilitate synchrotron X-ray imaging. Three different flow geometries were studied to understand the impact on the flow dynamics, and the formation of hydrogen bubbles. By electrolyte injection experiments, it was shown that the maximum saturation of carbon felt was achieved by a flat flow field after the first injection and by a serpentine flow field after continuous flow. Furthermore, the average saturation of the carbon felt was correlated to the cyclic voltammetry current response, and the hydrogen gas evolution was visualized in 3D by X-ray tomography. The capabilities of this cell design and experiments were outlined, which are essential for the evaluation and optimization of cell components of VRFBs.

Reconciling temperature-dependent factors affecting mass transport losses in polymer electrolyte membrane electrolyzers.

In this work, we investigated the impact of temperature on two-phase transport in low temperature (LT)-polymer electrolyte membrane (PEM) electrolyzer anode flow channels via in operando neutron imaging and observed a decrease in mass transport overpotential with increasing temperature. We observed an increase in anode oxygen gas content with increasing temperature, which was counter-intu.itive to the trends in mass transport overpotential. We attributed this counterintuitive decrease in mass transport overpotential to the enhanced reactant distribution in the flow channels as a result of the temperature increase, determined via a one-dimensional analytical model. We further determined that gas accumulation and fluid property changes are competing, temperature-dependent contributors to mass transport overpotential; however, liquid water viscosity changes led to the dominate enhancement of reactant water distributions in the anode. We present this temperature-dependent mass transport overpotential as a great opportunity for further increasing the voltage efficiency of PEM electrolyzers.

Calibrating the X-ray attenuation of liquid water and correcting sample movement artefacts during in operando synchrotron X-ray radiographic imaging of polymer electrolyte membrane fuel cells.

Synchrotron X-ray radiography, due to its high temporal and spatial resolutions, provides a valuable means for understanding the in operando water transport behaviour in polymer electrolyte membrane fuel cells. The purpose of this study is to address the specific artefact of imaging sample movement, which poses a significant challenge to synchrotron-based imaging for fuel cell diagnostics. Specifically, the impact of the micrometer-scale movement of the sample was determined, and a correction methodology was developed. At a photon energy level of 20 keV, a maximum movement of 7.5 µm resulted in a false water thickness of 0.93 cm (9% higher than the maximum amount of water that the experimental apparatus could physically contain). This artefact was corrected by image translations based on the relationship between the false water thickness value and the distance moved by the sample. The implementation of this correction method led to a significant reduction in false water thickness (to ∼0.04 cm). Furthermore, to account for inaccuracies in pixel intensities due to the scattering effect and higher harmonics, a calibration technique was introduced for the liquid water X-ray attenuation coefficient, which was found to be 0.657 ± 0.023 cm(-1) at 20 keV. The work presented in this paper provides valuable tools for artefact compensation and accuracy improvements for dynamic synchrotron X-ray imaging of fuel cells.

Dynamic pore network model of surface heterogeneity in brine-filled porous media for carbon sequestration.

Trapping of carbon in deep underground brine-filled reservoirs is a promising approach for the reduction of atmospheric greenhouse gas emissions. However, estimation of the amount of carbon dioxide (CO(2)) that can be captured in a given reservoir and the long-term storage stability remain a challenge. One difficulty lies in the estimation of local capillary pressure effects that arise from mineral surface heterogeneity inherent in underground geological formations. As a preliminary step to address this issue, we have performed dynamic pore network modelling (PNM) simulations of two-phase immiscible flow in two-dimensional structured porous media with contact angle heterogeneity under typical reservoir conditions. We begin by characterizing the network with a single, uniform contact angle. We then present saturation patterns for networks with homogeneous and heterogeneous contact angles distributions, based on two common reservoir minerals: quartz and mica, both of which have been well-characterized experimentally for their brine-CO(2) contact angles. At lower flow rates, we found moderately higher saturations for the heterogeneous networks than for the homogeneous ones. To characterize the fingering patterns, we have introduced R as the ratio of filled throats to the total network saturation. Based on this measure, the heterogeneous networks demonstrated thicker fingering patterns than the homogeneous networks. The computed saturation patterns demonstrate the importance of considering surface heterogeneity in pore-scale modelling of deep saline aquifers.