Rapid Computation of Mass Activities of Nanostructured Platinum Electrocatalysts for the Oxygen Reduction Reaction

Reduction of the Pt loading for the oxygen reduction reaction is a major challenge towards profitable fuel cell applications [1]. The development of three-dimensional (3D) Pt nanoparticle catalysts with enhanced catalytic mass activity addresses this problem [2]. Nonetheless, the investigation of novel 3D nanoparticle catalyst structures is highly limited by the complexity of experimental synthesis and large computation times in atomistic density functional theory (DFT) approaches. In the present work, we introduce a computational model which strongly speeds up the catalytic activity calculation of 3D Pt nanoparticle catalysts. Remarkably, this computational model evaluates the topological nanoparticle catalyst structure based on experimental and DFT data from literature while the model dispenses with expensive DFT calculations during runtime. The applicability of our computational model has been successfully proven on experimental data. Regarding the effect of nanoparticle sizes on the catalytic activity [3,4], the present study elucidates potential activity enhancement for specific ranges of nanoparticle sizes. Most prominently, rapid activity classification within our computational model enables extensive screening for promising novel 3D Pt nanoparticle catalyst shapes. References: [1] I. Erfye, L. Stephens and J. Rossmeisl, Science, 354(63), 9–11, 2016. [2] F. Calle-Vallejo, M. D. Pohl, D. Reinisch, D. Loffreda, P. Sautet and A. S. Bandarenka, Chem. Sci., 8(3), 2283–2289, 2017. [3] M. Shao, A. Peles and K. Shoemaker, Nano Letters, 11(9), 3714–3719, 2011. [4] F. J. Perez-Alonso, D. N. McCarthy, A. Nierhoff, P. Hernandez-Fernandez, C. Strebel, I. E. Stephens, J. H. Nielsen and I. Chorkendorff, Angewandte Chemie - International Edition, 51(19), 4641–4643, 2012     «

Reduction of the Pt loading for the oxygen reduction reaction is a major challenge towards profitable fuel cell applications [1]. The development of three-dimensional (3D) Pt nanoparticle catalysts with enhanced catalytic mass activity addresses this problem [2]. Nonetheless, the investigation of novel 3D nanoparticle catalyst structures is highly limited by the complexity of experimental synthesis and large computation times in atomistic density functional theory (DFT) approaches. In the presen...     »