Computational design of microarchitected porous electrodes for redox flow batteries

Beck, Victor A.; Wong, Jonathan J.; Jekel, Charles F.; Tortorelli, Daniel A.; Baker, Sarah E.; Duoss, Eric B.; Worsley, Marcus A.

doi:10.1016/j.jpowsour.2021.230453

Cited by 36 publications

(37 citation statements)

References 72 publications

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“…We note that as the electrode thickness increases, the overall fitting quality decreases at low flow rates, which is in agreement with the findings of Milshtein et al 23 We hypothesize that this is due to non-uniform flow distribution associated with the structural anisotropy of each weave, which, in turn, amplifies the deviation from the isotropic assumptions within the original model derivation. Efforts to remedy the microscale topological variations in macrohomogenous models is an active area of research 35,36 but is beyond the scope of this work.…”

Section: Bulk Electrode Fluid Dynamics and Electrochemistrymentioning

confidence: 99%

The Effect of Fibrous Tows and Weave Pattern on Carbon Cloths as Electrodes in Redox Flow Batteries

Tenny

Chiang

Brushett

2022

Preprint

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The electrochemical and fluid dynamic performance of redox flow batteries is strongly influenced by the microstructure of the porous electrodes. Carbon cloths are a potential candidate whose hierarchical structure affects length scales associated with electrolyte flow; however, few studies have investigated the electrochemical behavior spanning from the fibrous tow to the bulk weave pattern. Here, we explore commercially activated weave patterns (plain, 8-harness satin, 2×2 basket) in an aqueous environment while quantifying reactive transport for individual tows and simulating fiber bundle electrochemical activity through multiphysics modeling. We then evaluate each woven electrode in a redox flow cell, measuring the pressure loss, polarization, and galvanostatic cycling behavior before comparing the mass-transfer relationships. We find the weave pattern strongly correlates with flow cell pressure drop, while the carbon fibers per tow influence electrochemistry and mass-transport scaling. Collectively, these results offer new insights into how advanced carbon cloths structures impact flow cell performance.

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Section: Bulk Electrode Fluid Dynamics and Electrochemistrymentioning

confidence: 99%

The Effect of Fibrous Tows and Weave Pattern on Carbon Cloths as Electrodes in Redox Flow Batteries

Tenny

Chiang

Brushett

2022

Preprint

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“…[18][19][20][21] Similarly, efforts have been made to tune the electrode microstructure to increase the volumetric surface area and facilitate access to electrocatalytic sites. 22,15,[23][24][25][26][27] The anisotropic porous structure of RFB electrodes convolutes mathematical treatments of reactiontransport phenomena and thus frustrates the use of standardized electroanalytical methods. Specifically, conventional applied electroanalytical techniques leverage planar, impermeable electrode surfaces in quiescent or well-controlled hydrodynamic conditions for simplified reaction-transport behavior that enables routine extraction of rate constants.…”

Section: Introductionmentioning

confidence: 99%

Synthesis and Characterization of Dense Carbon Films as Model Surfaces to Estimate Electron Transfer Kinetics on Redox Flow Battery Electrodes

Wan

Ismail

Quinn

et al. 2022

Preprint

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Redox flow batteries (RFBs) are a promising electrochemical technology for the efficient and reliable delivery of electricity, providing opportunities to integrate intermittent renewable resources and to support unreliable and/or aging grid infrastructure. Within the RFB, porous carbonaceous electrodes facilitate the electrochemical reactions, distribute the flowing electrolyte, and conduct electrons. Understanding electrode reaction kinetics is crucial for improving RFB performance and lowering costs. However, assessing reaction kinetics on porous electrodes is challenging as their complex structure frustrates canonical electroanalytical techniques used to quantify performance descriptors. Here, we outline a strategy to estimate electron transfer kinetics on planar electrode materials of similar surface chemistry to those used in RFBs. First, we describe a bottom-up synthetic process to produce flat, dense carbon films to enable evaluation of electron transfer kinetics using traditional electrochemical approaches. Next, we characterize physicochemical properties of the films using a suite of spectroscopic methods, confirming that their surface characteristics align with those of widely-used porous electrodes. Last, we study the electrochemical performance of the films in a custom-designed cell architecture, extracting intrinsic heterogeneous kinetic rate constants for two iron-based redox couples in aqueous electrolytes using standard electrochemical methods (i.e., cyclic voltammetry, electrochemical impedance spectroscopy). We anticipate that the synthetic methods and experimental protocols described here are applicable to a range of electrocatalysts and redox couples.

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“…The integration of optimization tools within electrochemical numerical frameworks has been recently deployed to support the numerical identification of fitting parameters and find optimal operational conditions (33,(37)(38)(39), as well as to support the design of cell components (40)(41)(42)(43). Recently, Choi et al utilized a GA in combination with a two-dimensional model of an all-vanadium flow battery to identify the fluid parameters using a fitness function involving the mean square error of the voltage between the experimental and simulated data.…”

Section: Introductionmentioning

confidence: 99%

Starting from the bottom: Coupling a genetic algorithm and pore network model for porous electrode design

Gorp

Heijden

Sadeghi

et al. 2022

Preprint

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The microstructure of porous electrodes determines multiple performance-defining properties, such as the available reactive surface area, mass transfer rates, hydraulic resistance, and electronic conductivity. Thus, optimizing the electrode architecture is a powerful approach to enhance the performance and cost-competitiveness of electrochemical technologies. To this goal, the deployment of computational modeling has improved the fundamental understanding of reactive transport in porous electrodes; however, to date, it has mostly been used to simulate existing sets of materials. To expand our current arsenal of materials, we need to build computational frameworks that are predictive and can explore a large geometrical design space while being physically robust. Here, we present a novel approach for the optimization of porous electrode microstructure from the bottom-up that couples a genetic algorithm with a chemistry-agnostic electrochemical pore network model. In this first demonstration, we focus on optimizing redox flow battery electrodes. The genetic algorithm manipulates the pore and throat size distributions of an artificially generated microstructure with fixed pore positions by selecting the best-performing networks, based on the hydraulic and electrochemical performance computed by the model. For the studied VO2+/VO2+ electrolyte, we find an increase in the fitness of 75% compared to the initial configuration. The algorithm improves the fluid distribution by the formation of a bimodal pore size distribution containing preferential longitudinal flow pathways, resulting in a decrease of 73% for the required pumping power. Furthermore, the optimization yielded an 47% increase in surface area resulting in an electrochemical performance improvement of 42%. Our results show the potential of using genetic algorithms combined with pore network models to optimize porous electrode microstructures for a wide range of electrolyte composition and operation conditions.

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Computational design of microarchitected porous electrodes for redox flow batteries

Cited by 36 publications

References 72 publications

The Effect of Fibrous Tows and Weave Pattern on Carbon Cloths as Electrodes in Redox Flow Batteries

The Effect of Fibrous Tows and Weave Pattern on Carbon Cloths as Electrodes in Redox Flow Batteries

Synthesis and Characterization of Dense Carbon Films as Model Surfaces to Estimate Electron Transfer Kinetics on Redox Flow Battery Electrodes

Starting from the bottom: Coupling a genetic algorithm and pore network model for porous electrode design

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