TY - JOUR
T1 - Dual properties of a hydrogen oxidation Ni-catalyst entrapped within a polymer promote self-defense against oxygen /639/638/77/886 /639/638/161/893 /639/638/675 /120 /128 /140/131 article
AU - Oughli, Alaa A.
AU - Ruff, Adrian
AU - Boralugodage, Nilusha Priyadarshani
AU - Rodríguez-Maciá, Patricia
AU - Plumeré, Nicolas
AU - Lubitz, Wolfgang
AU - Shaw, Wendy J.
AU - Schuhmann, Wolfgang
AU - Rüdiger, Olaf
N1 - Publisher Copyright:
© 2018 The Author(s).
PY - 2018/12/1
Y1 - 2018/12/1
N2 - The Ni(P 2 N 2 ) 2 catalysts are among the most efficient non-noble-metal based molecular catalysts for H 2 cycling. However, these catalysts are O 2 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 2 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 2 is used by the catalyst to convert O 2 to H 2 O, thereby providing the "active" layer with a barrier against O 2 . 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 2 oxidation as well as O 2 tolerance.
AB - The Ni(P 2 N 2 ) 2 catalysts are among the most efficient non-noble-metal based molecular catalysts for H 2 cycling. However, these catalysts are O 2 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 2 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 2 is used by the catalyst to convert O 2 to H 2 O, thereby providing the "active" layer with a barrier against O 2 . 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 2 oxidation as well as O 2 tolerance.
UR - http://www.scopus.com/inward/record.url?scp=85042732002&partnerID=8YFLogxK
U2 - 10.1038/s41467-018-03011-7
DO - 10.1038/s41467-018-03011-7
M3 - Article
C2 - 29491416
AN - SCOPUS:85042732002
SN - 2041-1723
VL - 9
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 864
ER -