(Keynote) Insight into Carbon Corrosion of Different Carbon Supports for Pt-Based Electrocatalysts for Polymer Electrolyte Fuel Cells from Interfacial Perspective

Abstract

A mechanistic understanding of carbon corrosion in polymer electrolyte fuel cells (PEFCs) is required to design catalyst layers that are durable. Electrochemical oxidation of carbon occurs during uncontrolled startup and shutdown events of PEFCs leading to multitude of degradation events, including loss of electrochemical surface area (ECSA), pore structure collapse, Pt detachment, loss in ionomer and others. To understand carbon corrosion physics and resulting degradation mechanisms a detailed electrochemical characterization is needed to probe interfaces between Pt-ionomer, carbon-ionomer and to measure transport properties and the ECSA in the catalyst layer. In this presentation we will provide an overview of carbon corrosion understanding and our approaches to quantify the sequence of events. In these studies, PEFCs were subjected to the Department of Energy carbon corrosion accelerated stress test (AST) protocol. Various electrochemical techniques were used to describe interfaces and morphology, as well as transport properties for the cells at different stages of the AST. ECSA measurements, polarization curves, CO-displacement/stripping to determine sulfonic acid group coverage in dry and wet conditions, electrochemical impedance spectroscopy, oxygen transport resistance measurements and other techniques were used. In addition, physical characterization methods at the beginning of life (BOL) and end of life (EOL) were used, such as micro x-ray fluorescence mapping, focused ion beam scanning electron microscopy, transmission electron microscopy, x-ray photoelectron spectroscopy and Raman spectroscopy. A combination of electrochemical and physicochemical methods revealed that amorphous carbon oxidizes first, after which Pt detach resulting in the loss of the ECSA, followed by severe structure collapse, resulting in a poor oxygen transport resistance. We extend the study to carbon supports that are more graphitized to alleviate some of the issues observed with amorphous carbon support.