Dual properties of a hydrogen oxidation Ni-catalyst entrapped within a polymer promote self-defense against oxygen.

Oughli, Alaa A; Ruff, Adrian; Boralugodage, Nilusha Priyadarshani; Rodríguez-Maciá, Patricia; Plumeré, Nicolas; Lubitz, Wolfgang; Shaw, Wendy J; Schuhmann, Wolfgang et al. · Nat Commun · 2018

basic_science · Level V

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Abstract

The Ni(P<sub>2</sub>N<sub>2</sub>)<sub>2</sub> catalysts are among the most efficient non-noble-metal based molecular catalysts for H<sub>2</sub> cycling. However, these catalysts are O<sub>2</sub> sensitive and lack long term stability under operating conditions. Here, we show that in a redox silent polymer matrix the catalyst is dispersed into two functionally different reaction layers. Close to the electrode surface is the "active" layer where the catalyst oxidizes H<sub>2</sub> and exchanges electrons with the electrode generating a current. At the outer film boundary, insulation of the catalyst from the electrode forms a "protection" layer in which H<sub>2</sub> is used by the catalyst to convert O<sub>2</sub> to H<sub>2</sub>O, thereby providing the "active" layer with a barrier against O<sub>2</sub>. This simple but efficient polymer-based electrode design solves one of the biggest limitations of these otherwise very efficient catalysts enhancing its stability for catalytic H<sub>2</sub> oxidation as well as O<sub>2</sub> tolerance.