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


ABSTRACT: The Ni(P2N2)2 catalysts are among the most efficient non-noble-metal based molecular catalysts for H2 cycling. However, these catalysts are O2 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 H2 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 H2 is used by the catalyst to convert O2 to H2O, thereby providing the "active" layer with a barrier against O2. 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 H2 oxidation as well as O2 tolerance.

SUBMITTER: Oughli AA 

PROVIDER: S-EPMC5830441 | biostudies-literature | 2018 Feb

REPOSITORIES: biostudies-literature

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

Oughli Alaa A AA   Ruff Adrian A   Boralugodage Nilusha Priyadarshani NP   Rodríguez-Maciá Patricia P   Plumeré Nicolas N   Lubitz Wolfgang W   Shaw Wendy J WJ   Schuhmann Wolfgang W   Rüdiger Olaf O  

Nature communications 20180228 1


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  ...[more]

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