Application of Hydrogenated Graphitic Supports in Electrocatalysts: Effects on Carbon Support Surface Chemistry, Nanoparticle Growth, and Electrocatalytic Activity.

One of the key technical challenges before the widespread adoption of proton exchange membrane fuel cells (PEMFCs) is increasing the durability of the platinum catalyst layer to meet a target of 8000 operating hours with only a 10% loss of performance. Carbon corrosion, one of the primary mechanisms of degradation in fuel cells, has attracted attention from researchers interested in solving the durability problem. As such, the development of catalyst supports to avoid this issue has been a focus in recent years, with interest in hydrophobic supports such as highly graphitized carbons. In this research, we propose a method to increase the durability of carbon supports by way of exploiting hydrogenated graphene's hydrophobic properties. By performing a Birch reduction on graphene nanoplatelets, we were able to synthesize hydrogenated graphene nanoplatelets which were used as support for hollow porous PtNi nanoparticles. The structure of these nanoparticle-carbon composites was characterized by transmission electron microscopy (TEM), energy dispersive spectroscopy coupled with scanning transmission electron microscopy (STEM-EDS), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS). We found that hydrogenation can strongly affect the morphology of nanoparticles formed as well as increase the electrochemical stability of the composites. Accelerated stress tests for 6000 cycles between 1.0 and 1.6 V vs RHE at 25 °C demonstrated that a hydrogenated support for PtNi increased the retained electrochemical surface from 36.8% to 61.9% when compared to the pristine graphene nanoplatelets. Moreover, the retained activity was increased from 26.6% to 53.0% by use of the hydrogenated carbon support. To confirm that hydrogenation enhanced durability, stress tests combined with Raman spectroscopy showed minimal change in the / ratio of the hydrogenated composite. Finally, identical location transmission electron microscopy (IL-TEM) was used to support the results of the electrochemical stress tests.