Proceedings of September Meeting 2016 (NFM16)
Publication date: 14th June 2016
Redox-active support materials can help reduce the noble-metal loading of a solid chemical catalyst, while offering electronic catalyst-support interactions beneficial for catalyst stability. This is well known in heterogeneous gas-phase catalysis, but much less discussed for electrocatalysis at electrified liquid-solid interfaces. Here, we demonstrate experimental evidence for electronic catalyst-support interactions in electrochemical environments and study their role and contribution to the corrosion stability of catalyst/support couples. Electrochemically oxidized M (M = Ir or Ru) oxide nanoparticles, supported on high surface area carbons and oxides, were selected as model catalyst/support systems for the electrocatalytic oxygen evolution reaction (OER). First, the electronic, chemical, and structural state of the catalyst/support couple was compared using XANES, EXAFS, TEM and depth-resolved XPS. Unlike carbon-supported catalysts, the M/MOx/ATO system exhibited evidence of metal/metal-oxide support interactions (MMOSI) that stabilized the metal particles on ATO and resulted in sustained lower M (M = Ir or Ru) oxidation states. At the same time, the growth of higher-valent M oxide layers that compromise catalyst stability was suppressed. Then, the electrochemical stability and the charge-transfer kinetics of the electrocatalysts were evaluated under constant current and constant potential conditions, where the analysis of the metal dissolution confirmed that the ATO support mitigates Mz+ dissolution thanks to a stronger MMOSI effect. Our findings raise the possibility that MMOSI effects in electrochemistry - largely neglected in the past - may be more important for a detailed understanding of the durability of oxide-supported nanoparticle OER catalysts than previously thought.
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