Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.054
Publication date: 18th July 2023
The extensive application of proton exchange membrane fuel cells (PEMFC) is conditioned by the limited supply and high cost of the Pt used in commercial PEMFC catalysts. To make PEMFC more widely available, new electrocatalysts with low Pt loading and high Pt efficiencies must be developed.
An important, but little explored aspect of this, is the interaction between the carbon support, proton conductive ionomer and catalyst. Catalyst support with optimal porosity is suggested to protect the Pt particles from direct ionomer poisoning but still provide the particles with good accessibility to the protons and oxygen.
In our project, carbon nanospheres with highly ordered mesoporous channels have been synthesised sustainably from biomass. Pt nanoparticles were deposited via polyol method onto the as synthesised mesoporous carbon sphere (MCS) and another two commercially widely used carbon substrates (porous Ketjenblack and non-porous Vulcan). Characterization of the catalysts were carried out with SEM/TEM, BET, XPS, XRD, revealing that the Pt nanoparticles are same in geometric and electronic structure while the difference of these catalysts solely arises from the different support porosity thus the different local environment of Pt NPs in the catalysts. All the Pt/C catalysts were tested under a gas diffusion half cell configuration for their oxygen reduction performance. Pt/MCS shows supreme performance where the Pt NPs sit inside the mesoporous channels of the carbon sphere.
To understand the outstanding activity of Pt/MCS, operando X-ray Absorption Spectroscopy was used to evaluate the ionomer coverage on the Pt surface by monitoring the Pt electronic structure change in the potential range of 0.1-1 V (vs RHE). Together with comprehensive nanostructure analysis via gas sorption, we proved that the oxygen reduction performance was boosted via the ideal interaction of Pt and Nafion ionomer, where direct contact in-between these two is eliminated without sacrificing the accessibility of Pt active sites. This will then guild the design strategy for future electrocatalysts development.
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