Nanoscale study of reactive transport in catalyst layer of proton exchange membrane fuel cells with precious and non-precious catalysts using lattice Boltzmann method

TL;DR

This study uses lattice Boltzmann simulations to analyze nanoscale transport phenomena in proton exchange membrane fuel cell catalyst layers, revealing how pore structure and catalyst type influence reactant transport and reaction rates.

Contribution

It introduces a novel nanoscale reconstruction and simulation approach to evaluate transport properties and reactive transport in catalyst layers with different catalysts.

Findings

Nonuniform ionomer distribution increases tortuosity and reduces diffusivity.

Knudsen diffusion significantly impacts oxygen transport.

Non-precious catalysts have higher reactive surface but lower reaction rates.

Abstract

High-resolution porous structures of catalyst layer (CL) with multicomponent in proton exchange membrane fuel cells are reconstructed using a reconstruction method called quartet structure generation set. Characterization analyses of nanoscale structures are implemented including pore size distribution, specific area and phase connectivity. Pore-scale simulation methods based on the lattice Boltzmann method are developed and used to predict the macroscopic transport properties including effective diffusivity and proton conductivity. Nonuniform distributions of ionomer in CL generates more tortuous pathway for reactant transport and greatly reduces the effective diffusivity. Tortuosity of CL is much higher than conventional Bruggeman equation adopted. Knudsen diffusion plays a significant role in oxygen diffusion and significantly reduces the effective diffusivity. Reactive transport inside the CL is also investigated. Although the reactive surface area of non-precious metal catalyst (NPMC) CL is much higher than that of Pt CL, the oxygen reaction rate is quite lower in NPMC CL compared with that in Pt CL, due to much lower reaction rate. Micropores (a few nanometers) in NPMC CL although can increase reactive sites, contribute little to enhance the mass transport. Mesopores (few tens of nanometers) or macropores are required to increase the mass transport rate.