Analytical modelling of CO<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" altimg="si26.svg"><mml:msub><mml:mrow/><mml:mn>2</mml:mn></mml:msub></mml:math> reduction in gas-diffusion electrode catalyst layers

Blake, Joseph W.; Padding, JT Johan; Haverkort, J.W.

doi:10.1016/j.electacta.2021.138987

Cited by 42 publications

(41 citation statements)

References 49 publications

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“…Mathematical modeling is an effective and promising method for the investigation of transport phenomena , and reaction kinetics. − In this work, we report a novel mathematical model for a three-phase oxidase enzymatic reaction system based on glucose oxidase (GOx), a model enzyme. A steady-state isothermal 2D model was developed to describe interphase (gas dissolution) and intraphase (species diffusion) mass transfer and enzyme catalysis reaction.…”

Section: Introductionmentioning

confidence: 99%

Mathematical Model for a Three-Phase Enzymatic Reaction System

Zou

Wang

Xiao

et al. 2023

Ind. Eng. Chem. Res.

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The enzymatic reaction system with a solid−liquid−gas three-phase interface microenvironment allows oxygen to be directly supplied to the oxidase catalytic reaction from the gas phase, effectively improving enzyme kinetics as compared with the conventional two-phase system. For this new system, a mathematical model is developed in this work to describe the enzymatic reaction coupled with interphase mass transfer, by which the influences of three-phase interfacial microenvironment on reaction kinetics can be systematically and quantitatively explored. The numerical simulations reveal that the flux of oxygen transport across the interface between the gas phase and the enzyme layer dominantly determines the H 2 O 2 production rate. The porous substrate possessing larger porosity and smaller pores, when coated with a thick and concentrated enzyme layer, can potentially lead to higher oxygen supply and hence a higher H 2 O 2 production rate. Moreover, regardless of the pore diameter, the H 2 O 2 production rate remains constant after the porosity is greater than 0.8, and if the enzyme concentration is not less than 5 mol m −3 , the H 2 O 2 production rate no longer changes after the thickness of the enzyme layer is greater than 0.5 μm. This work offers a powerful in silico tool for the investigation of the three-phase enzymatic reaction system. The quantitative results and mechanistic findings will lead to optimized design of this promising system.

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Section: Introductionmentioning

confidence: 99%

Mathematical Model for a Three-Phase Enzymatic Reaction System

Zou

Wang

Xiao

et al. 2023

Ind. Eng. Chem. Res.

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“…Tan et al [16] --Constant bulk concentration Constant CO 2 concentration at three-phase boundary Blake et al [32] -Electroneutrality Transport correlation with constant bulk concentration…”

Section: Ohm's Law Normal Flow Normal Flowmentioning

confidence: 99%

“…The penetration of liquid electrolyte into the CL is not accounted for in the model from Kas et al However, an electrolyte layer in the CL adds up an additional resistance to the mass transport of CO 2 from the gas phase to the catalytic active sites, which will impact the reduction rate. [4,31] In a recent publication, Blake et al [32] published both a numerical and an analytical model that approximate the cathodic CL environment. The models show good agreement with experimental data from Verma et al [18] and allow to study the influence of geometrical changes of the CL and electrolyte flow on the energetics and the liquid species concentration within the CL.…”

Section: Not Mentioned Two-dimensional Flow Channelmentioning

confidence: 99%

“…In a recent publication, Blake et al [ 32 ] published both a numerical and an analytical model that approximate the cathodic CL environment. The models show good agreement with experimental data from Verma et al [ 18 ] and allow to study the influence of geometrical changes of the CL and electrolyte flow on the energetics and the liquid species concentration within the CL.…”

Section: Introductionmentioning

confidence: 99%

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Simulation‐based guidance for improving CO2${\rm CO}_{2}$ reduction on silver gas diffusion electrodes

Heßelmann

Bräsel

Keller

et al. 2022

Electrochemical Science Adv

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The reduction of CO2${\rm CO}_{2}$ in an electrochemical reactor using electrical energy is a promising approach to implement a more sustainable carbon economy and to replace fossil fuels with renewable carbon sources. Conventionally used solid plate electrodes are limited by poor mass transport of the reactants. Gas diffusion electrodes (GDEs) can overcome this limitation and have gained industrial relevance during the last decades. A comprehensive understanding of transport and conversion phenomena within such porous electrodes is not yet well developed. Here, we report a one‐dimensional steady state model of the GDE to investigate the influence of relevant operational parameters and GDE properties on CO2${\rm CO}_{2}$ reduction. The results indicate the importance of controlling the local reaction environment, that is, the reactant concentration and the pH value, by tuning the electrolyte and gas composition, and flow rate as well as the catalyst layer properties.

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“…27 Recently, effectiveness factor analysis has also been utilized in gas diffusion electrodes for CO2 reduction to model agglomerates 28 and as part of the development of an analytical model of the catalyst layer. 29 Effectiveness factors have been applied to thermo-electrochemical cells, 30 particulate bed electrodes, 31,32 electrocatalysis in metal-organic frameworks, 33 and in oxygen reduction reactions. 34 The array of applications and incorporation across multiple modeling length scales highlights the ubiquity of the Thiele modulus / effectiveness factor approach.…”

Section: Introductionmentioning

confidence: 99%

Methods—A Potential–Dependent Thiele Modulus to Quantify the Effectiveness of Porous Electrocatalysts

Brushett

Wan

Greco

et al. 2021

J. Electrochem. Soc.

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Electrochemical reactors often employ high surface area electrocatalysts to accelerate volumetric reaction rates and increase productivity. While electrocatalysts can alleviate kinetic overpotentials, diffusional resistances at the pore-scale often prevent full catalyst utilization. The effect of intraparticle diffusion on the overall reaction rate can be quantified through an effectiveness factor expression governed by the Thiele modulus parameter. This analytical approach is integral to the development of catalytic structures for thermochemical processes and has previously been extended to electrochemical processes by accounting for the relationship between reaction kinetics and electrode overpotential. In this paper, we illustrate the method by deriving the expression for the potential-dependent Thiele modulus and using it to quantify the effectiveness factor for porous electrocatalytic structures. Specifically, we demonstrate the application of this mathematical framework to spherical microparticles as a function of applied overpotential across catalyst properties and reactant characteristics. The relative effects of kinetics and mass transport are related to overall reaction rates, revealing markedly lower catalyst utilization at increasing overpotential. Subsequently, we generalize the analysis to different catalyst shapes and provide guidance on the design of porous catalytic materials for use in electrochemical reactors.

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Analytical modelling of CO2 reduction in gas-diffusion electrode catalyst layers

Cited by 42 publications

References 49 publications

Mathematical Model for a Three-Phase Enzymatic Reaction System

Mathematical Model for a Three-Phase Enzymatic Reaction System

Simulation‐based guidance for improving CO2${\rm CO}_{2}$ reduction on silver gas diffusion electrodes

Methods—A Potential–Dependent Thiele Modulus to Quantify the Effectiveness of Porous Electrocatalysts

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