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Matanovic, Ivana; Maurya, Sandip; Park, Eun Joo; Jeon, Jong Yeob; Bae, Chulsung; Kim, Yu Seung
Chemistry of materials, 06/2019, Letnik: 31, Številka: 11Journal Article
The performance of anion exchange membrane fuel cells (AEMFCs) employing Pt or PtRu electrocatalyst and ionomers with different polyaromatic backbones is correlated with the density functional theory (DFT)-calculated adsorption energies of the ionomer fragments on the metal surfaces. The performance of the AEMFCs tested in this work significantly changes depending on the backbone structure of polyaromatic ionomer or the type of the catalyst used at the anode. For the same anode catalyst, the performance decreases in the order poly(fluorene) > poly(p-biphenyl alkylene) > poly(terphenyl alkylene)s, which is in excellent agreement with the decrease in the DFT-calculated interaction energies between the catalyst surface and the corresponding ionomer fragment. Namely, DFT-calculated adsorption energies decrease in the order: p-terphenyl ≥ m-terphenyl > biphenyl > diphenyl ether > benzene ≥ o-terphenyl > 9,9-dimethyl fluorene. The trend in the adsorption energies is explained on the basis of the structural and conformational features of the ionomer fragments. Namely, strong adsorption of the polyaromatic ionomer fragments correlates with the number of benzene rings with a low rotational barrier that can bind parallel to the metal surfaces, leading to strong interaction and hybridization of the aromatic π-orbitals with metal electronic states. The results of this work suggest, therefore, that the interaction between the ionomer and electrocatalyst should be taken into account when designing high-performing ionomers even before considering other factors such as hydroxide conductivity, gas permeability, and water uptake of the ionomeric binder.
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