Dynamics of Pd Dopant Atoms inside Au Nanoclusters during Catalytic CO Oxidation
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In: Journal of Physical Chemistry C, Vol. 124.2020, No. 43, 20.10.2020, p. 23626-23636.
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TY - JOUR
T1 - Dynamics of Pd Dopant Atoms inside Au Nanoclusters during Catalytic CO Oxidation
AU - García, Clara
AU - Truttmann, Vera
AU - Lopez, Irene
AU - Haunold, Thomas
AU - Marini, Carlo
AU - Rameshan, Christoph
AU - Pittenauer, Ernst
AU - Kregsamer, Peter
AU - Dobrezberger, Klaus
AU - Stöger-Pollach, Michael
AU - Barrabés, Noelia
AU - Rupprechter, Günther
N1 - Publisher Copyright: © 2020 American Chemical Society.
PY - 2020/10/20
Y1 - 2020/10/20
N2 - Doping gold nanoclusters with palladium has been reported to increase their catalytic activity and stability. PdAu24 nanoclusters, with the Pd dopant atom located at the center of the Au cluster core, were supported on titania and applied in catalytic CO oxidation, showing significantly higher activity than supported monometallic Au25 nanoclusters. After pretreatment, operando DRIFTS spectroscopy detected CO adsorbed on Pd during CO oxidation, indicating migration of the Pd dopant atom from the Au cluster core to the cluster surface. Increasing the number of Pd dopant atoms in the Au structure led to incorporation of Pd mostly in the S-(M-S)n protecting staples, as evidenced by in situ XAFS. A combination of oxidative and reductive thermal pretreatment resulted in the formation of isolated Pd surface sites within the Au surface. The combined analysis of in situ XAFS, operando DRIFTS, and ex situ XPS thus revealed the structural evolution of bimetallic PdAu nanoclusters, yielding a Pd single-site catalyst of 2.7 nm average particle size with improved CO oxidation activity.
AB - Doping gold nanoclusters with palladium has been reported to increase their catalytic activity and stability. PdAu24 nanoclusters, with the Pd dopant atom located at the center of the Au cluster core, were supported on titania and applied in catalytic CO oxidation, showing significantly higher activity than supported monometallic Au25 nanoclusters. After pretreatment, operando DRIFTS spectroscopy detected CO adsorbed on Pd during CO oxidation, indicating migration of the Pd dopant atom from the Au cluster core to the cluster surface. Increasing the number of Pd dopant atoms in the Au structure led to incorporation of Pd mostly in the S-(M-S)n protecting staples, as evidenced by in situ XAFS. A combination of oxidative and reductive thermal pretreatment resulted in the formation of isolated Pd surface sites within the Au surface. The combined analysis of in situ XAFS, operando DRIFTS, and ex situ XPS thus revealed the structural evolution of bimetallic PdAu nanoclusters, yielding a Pd single-site catalyst of 2.7 nm average particle size with improved CO oxidation activity.
UR - http://www.scopus.com/inward/record.url?scp=85096060229&partnerID=8YFLogxK
U2 - 10.1021/acs.jpcc.0c05735
DO - 10.1021/acs.jpcc.0c05735
M3 - Article
AN - SCOPUS:85096060229
VL - 124.2020
SP - 23626
EP - 23636
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
SN - 1932-7447
IS - 43
ER -
