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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Topology optimization for the design of porous electrodes

Porous electrodes are an integral part of many electrochemical devices since they have high porosity to maximize electrochemical transport and high surface area to maximize activity. Traditional porous electrode materials are typically homogeneous, stochastic collections of small-scale particles and offer few opportunities to engineer higher performance. Fortunately, recent breakthroughs in advanced and additive manufacturing are yielding new methods to structure and pattern porous electrodes across length scales. These architected electrodes are emerging as a promising new technology to continue to drive improvement; however, it is still unclear which structures to employ and few tools are available to guide their design. Here we address this gap by applying topology optimization to the design of porous electrodes. We demonstrate our framework on two applications: a porous electrode driving a steady Faradaic reaction and a transiently operated electrode in a supercapacitor. We present computationally designed electrodes that minimize energy losses in a half-cell. For low-conductivity materials, the optimization algorithm creates electrode designs with a hierarchy of length scales. Further, the designed electrodes are found to outperform undesigned, homogeneous electrodes. Finally, we present three-dimensional porous electrode designs. We thus establish a topology optimization framework for designing porous electrodes.

25 ENERGY STORAGE↗
NASA NTRS1987

Effect of structure on current and potential distributions in porous electrode

Porous electrodes generally contain constricted macropores and localized micropores. The effects of the macropore constrictions on the resistance of a capillary were studied and an analytical model was developed for predicting the current distribution in a constricted macropore which directly includes constriction effects and does not require an empirical tortuosity parameter. The current and concentration distributions in localized micropores were also investigated and it was shown that the microporous area is fully accessible to charge and mass transfer processes. From these analyses it was concluded that the micropores primarily affect the kinetics of the interfacial processes by contributing to the interfacial area, while the macropores impose ohmic and mass transport limitations through the volume of the porous electrode.

Lanzi, Oscar↗
NASA NTRS1990

The impedance of a tubular electrode - A model for a porous electrode

A cylindrical tube is used as the basis for a two-dimensional mathematical model to calculate the impedance of a flooded porous electrode. The model incorporates charge-transfer, mass-transfer, and ohmic resistances to obtain the axial and radial dependencies of the concentration and potential profiles. A linearized Butler-Volmer kinetic expression for a simple redox reaction O + e yielding R is used, in conjuction with analytical expressions for the surface concentration and overpotential, to compute the open-circuit impedance. The results of the two-dimensional model, which omits double-layer charging, are compared with the results of a more standardly applied one-dimensional model in which radial variations are neglected, with and without double-layer charging. The simpler-to-apply one-dimensional model is found to be satisfactory when mass-transfer and ohmic resistances are small with respect to charge-transfer resistance. The omission of double-layer charging does not introduce error into the two-dimensional model in the frequency range in which capacitive-like effects are caused by mass-transfer limitations.

Viner, Andrew S.↗
NASA NTRS1991

Modelling of nickel-cadmium batteries using porous electrode theory

A porous electrode modeling technique is discussed which is considered a viable means for quantitatively predicting Ni-Cd cell performance. The authors describe the integration of the cell model into a battery model useful in the design and operation of aerospace applications. Test data from a sealed boilerplate cell are presented for constant current charge and discharge conditions. Performance predictions for similar cases have been performed, and a comparison to the boilerplate data is made. Areas for further development are also noted.

Timmerman, Paul J.↗
DOE OSTI2021

Quantifying Uncertainty in Tortuosity Estimates for Porous Electrodes

Measuring tortuosity in porous electrodes is important for understanding rate capability and optimizing design. Here, we describe an approach to determine electrode tortuosities and quantify the associated uncertainties by fitting a P2D model to discharge profiles from a standard rate capability test. A dimensionless current is identified as a design-of-experiment parameter that can be used to identify experiments that return confident estimates of tortuosity, even when other model parameters are not known with certainty. This approach is applied to analysis of L i x V 3 O 8 (LVO) electrodes and L i x N i 0.33 M n 0.33 C o 0.33 O 2 (NMC) electrodes. The details of the assumptions made in these measurements and their impact on the reported uncertainties are discussed. We also perform an uncertainty analysis on the standard method for quantifying tortuosity in the literature: electrochemical impedance spectroscopy collected under blocking electrolyte conditions. We find that confident estimates can be obtained using this approach even when uncertainties in equivalent circuit model parameters are considered.

25 ENERGY STORAGE↗
DOE OSTI2021

Computational design of microarchitected porous electrodes for redox flow batteries

Porous electrodes are used as the core reactive component across electrochemical technologies. In flowing systems, controlling the fluid distribution, species transport, and reactive environment is critical to attaining high performance. However, conventional electrode materials like felts and papers provide few opportunities for precise engineering of the electrode and its microstructure. To address these limitations, architected electrodes composed of unit cells with spatially varying geometry determined via computational optimization are proposed. Resolved simulation is employed to develop a homogenized description of the constituent unit cells. These effective properties serve as inputs to a continuum model for the electrode when used in the negative half-cell of a vanadium redox flow battery. Porosity distributions minimizing power loss are then determined via computational design optimization to generate architected porosity electrodes. The architected electrodes are compared to bulk, uniform porosity electrodes and found to lead to increased power efficiency across operating flow rates and currents. The design methodology is further used to generate a scaled-up electrode with comparable power efficiency to the bench-scale systems. Finally, the variable porosity architecture and computational design methodology presented here thus offers a novel pathway for automatically generating spatially engineered electrode structures with improved power performance.

25 ENERGY STORAGE↗
NASA NTRS1987

Electrochemical impregnation of nickel hydroxide in porous electrodes

The electrochemical impregnation of nickel hydroxide in porous electrode was investigated both experimentally and theoretically. The loading level and plaque expansion were the most important parameters to be considered. The effects of applied current density, stirring, ratio of solution to electrode volume and pH were identified. A novel flow through electrochemical impregnation is proposed in which the electrolyte is forced through the porous nickel plaque. The thickening of the plaque can be reduced while maintaining high loading capacity. A mathematical model is presented which describes the transport of the nitrate, nickel and hydroxyl ions and the consecutive heterogeneous electrochemical reduction of nitrate and the homogeneous precipitation reaction of nickel hydroxide. The distributions of precipitation rate and active material within the porous electrode are obtained. A semiempirical model is also proposed which takes into account the plugging of the pores.

Ho, Kuo-Chuan↗
DOE OSTI2022

Continuum Modeling of Porous Electrodes for Electrochemical Synthesis

Electrochemical synthesis possesses substantial promise to utilize renewable energy sources to power the conversion of abundant feedstocks to value-added commodity chemicals and fuels. Of the potential system architectures for these processes, only systems employing 3-D structured porous electrodes have the capacity to achieve the high rates of conversion necessary for industrial scale. However, the phenomena and environments in these systems are not well understood and are challenging to probe experimentally. Fortunately, continuum modeling is well-suited to rationalize the observed behavior in electrochemical synthesis, as well as to ultimately provide recommendations for guiding the design of next-generation devices and components. In this review, we begin by presenting an historical review of modeling of porous electrode systems, with the aim of showing how past knowledge of macroscale modeling can contribute to the rising challenge of electrochemical synthesis. We then present a detailed overview of the governing physics and assumptions required to simulate porous electrode systems for electrochemical synthesis. Here, leveraging the developed understanding of porous-electrode theory, we survey and discuss the present literature reports on simulating multiscale phenomena in porous electrodes in order to demonstrate their relevance to understanding and improving the performance of devices for electrochemical synthesis. Lastly, we provide our perspectives regarding future directions in the development of models that can most accurately describe and predict the performance of such devices and discuss the best potential applications of future models.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Topology Optimization for Porous Electrodes

This code is for the topology optimization of porous electrodes. It was used to produce the results in Roy, T., Salazar de Troya, M.A., Worsley, M.A. and Beck, V.A., 2021. Topology optimization for the design of porous electrodes. arXiv preprint arXiv:2111.12059.

Roy, Thomas↗
DOE OSTI2022

Lattice Optimization for Porous Electrode

This code performs an optimization over the structure of a porous electrode formed from a lattice of unit cells. This is a steepest descent version of the code used in: V. A. Beck, J. J. Wong, C. F. Jekel, D. A. Tortorelli, S. E. Baker, E. B. Duoss and M. A. Worsley, Computational design of microarchitected porous electrodes for redox flow batteries, J. Power Sources, 2021, 512, 230453.

Wong, JonathanJ↗
DOE OSTI2024

Quantitative local state of charge mapping by operando electrochemical fluorescence microscopy in porous electrodes

We introduce operando quantitative electrochemical fluorescence state of charge mapping (QEFSM), a non-invasive technique to study operating electrochemical systems along with a new design of optically transparent microfluidic redox flow cells compatible with the most demanding optical requirements. QEFSM allows quantitative mappings of the concentration of a particular oxidation state of a redox-active species within a porous electrode during its operation. In this study, we used confocal microscopy to map the fluorescence signal of the reduced form of 2,7-anthraquinone disulfonate (AQDS) in a set of multistep-chronoamperometry experiments. Calibrating these images and incorporating an analytical model of quinhydrone heterodimer formation with no free parameters, and accounting for the emission of each species involved, we determined the local molecular concentration and the state of charge (SOC) fields within a commercial porous electrode during operation. With this method, electrochemical conversion and species advection, reaction and diffusion can be monitored at heretofore unprecedented transverse and axial resolution (1 μm and 25 μm, respectively) at frame rates of 0.5 Hz, opening new routes to understanding local electrochemical processes in porous electrodes. Here, we observed pore-scale SOC inhomogeneities appearing when the fraction of electroactive species converted in a single pass through the electrode becomes large.

42 ENGINEERING↗
NASA NTRS1990

Characterization of reaction kinetics in a porous electrode

A continuum-model approach, analogous to porous electrode theory, was applied to a thin-layer cell of rectangular and cylindrical geometry. A reversible redox couple is assumed, and the local reaction current density is related to the potential through the formula of Hubbard and Anson for a uniformily accessible thin-layer cell. The placement of the reference electrode is also accounted for in the analysis. Primary emphasis is placed on the effect of the solution-phase ohmic potential drop on the voltammogram characteristics. Correlation equations for the peak-potential displacement from E(sup 0 prime) and the peak current are presented in terms of two dimensionless parameters.

Fedkiw, Peter S.↗
DOE OSTI2021

Lithium vanadium oxide (Li 1.1 V 3 O 8 ) thick porous electrodes with high rate capacity: utilization and evolution upon extended cycling elucidated via operando energy dispersive X-ray diffraction and continuum simulation

The phase distribution of lithiated LVO in thick (~500 μm) porous electrodes (TPEs) designed to facilitate both ion and electron transport was determined using synchrotron-based operando energy dispersive X-ray diffraction (EDXRD). Probing 3 positions in the TPE while cycling at a 1C rate revealed a homogeneous phase transition across the thickness of the electrode at the 1st and 95th cycles. Additionally, continuum modelling indicated uniform lithiation across the TPE in agreement with the EDXRD results and ascribed decreasing accessible active material to be the cause of loss in delivered capacity between the 1st and 95th cycles. The model was supported by the observation of significant particle fracture by SEM consistent with loss of electrical contact. Overall, the combination of operando EDXRD, continuum modeling, and ex situ measurements enabled a deeper understanding of lithium vanadium oxide transport properties under high rate extended cycling within a thick highly porous electrode architecture.

25 ENERGY STORAGE↗
DOE OSTI2024

Topology optimization for the full-cell design of porous electrodes in electrochemical energy storage devices

In this paper, we introduce a density-based topology optimization framework to design porous electrodes for maximum energy storage. We simulate the full cell with a model that incorporates electronic potential, ionic potential, and electrolyte concentration. The system consists of three materials, namely pure liquid electrolyte and the porous solids of the anode and cathode, for which we determine the optimal placement. We use separate electronic potentials to model each electrode, which allows interdigitated designs. As a result, a penalization is required to ensure that the anode and cathode do not touch, i.e., causing a short circuit. We compare multiple 2D designs generated for different fixed conditions, e.g. material properties. A 3D design with complex channel and interlocked structure is also created. All optimized designs are far superior to the traditional monolithic electrode design with respect to energy storage metrics. We observe up to a 750% increase in energy storage for cases with slow effective ionic diffusion within the porous electrode.

25 ENERGY STORAGE↗