Atomic-scale modeling of C/N kinetic stability descriptors for PGM-free electrocatalysts at finite temperatures

Hafiz, Hasnain; Zelenay, Piotr; Holby, Edward F.

doi:10.1016/j.apcatb.2023.123158

Title: Atomic-scale modeling of C/N kinetic stability descriptors for PGM-free electrocatalysts at finite temperatures

Journal Article · Tue Aug 08 00:00:00 UTC 2023 · Applied Catalysis. B, Environmental

DOI: https://doi.org/10.1016/j.apcatb.2023.123158 · OSTI ID:1995153

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Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

The durability of platinum group metal-free (PGM-free) electrocatalysts is a major barrier to their usage in polymer electrolyte fuel cell cathodes. C and N removal from active sites may play an important role in the catalyst’s ability to maintain high activity. While C degradation mechanisms are kinetically controlled, previous studies have focused on thermodynamic descriptors. In this work, we develop a temperature-dependent kinetic descriptor of C and N stability using an electron beam-damage model. Our approach considers the electron beam energy threshold (EBET) describing the knock-on displacement of C and N atoms as a stability descriptor for atomic structures. The stability of different sites is calculated to be different showing this approach can discriminate between similar sites with varied configurations. Additionally, we provide important insight regarding TEM beam damage of proposed active sites. We calculate 60 keV electrons can damage some proposed active site structures even at room temperature.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1995153

Report Number(s):: LA-UR--23-23023

Journal Information:: Applied Catalysis. B, Environmental, Journal Name: Applied Catalysis. B, Environmental Vol. 339; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Atomic-scale modeling of C/N kinetic stability descriptors for PGM-free electrocatalysts at finite temperatures

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