TY - JOUR
T1 - Molybdenum doping augments platinum–Copper Oxygen reduction Electrocatalyst
AU - Luo, Yun
AU - Kirchhoff, Björn
AU - Fantauzzi, Donato
AU - Calvillo, Laura
AU - Estudillo-Wong, Luis Alberto
AU - Granozzi, Gaetano
AU - Jacob, Timo
AU - Alonso-Vante, Nicolas
N1 - Publisher Copyright:
© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
PY - 2018/1
Y1 - 2018/1
N2 - Improving the efficiency of Pt-based oxygen reduction reaction (ORR) catalysts while also reducing costs remains an important challenge in energy research. To this end, we synthesized highly stable and active carbon-supported Mo-doped PtCu (Mo-PtCu/C) nanoparticles (NPs) from readily available precursors in a facile one-pot reaction. Mo-PtCu/C displays two-tofourfold- higher ORR half-cell kinetics than reference PtCu/C and Pt/C materials, a trend that was confirmed in proof-of-concept experiments by using a H2/O2 microlaminar fuel cell. This Mo-induced activity increase mirrors observations for Mo-PtNi/ C NPs and possibly suggests an emerging trend. Electrochemical- accelerated stability tests revealed that dealloying was greatly reduced in Mo-PtCu/C in contrast to the binary alloys PtCu/C and PtMo/C. Supporting DFT studies suggested that the exceptional stability of Mo-PtCu could be attributed to oxidative resistance of the Mo-doped atoms. Furthermore, our calculations revealed that oxygen could induce segregation of Mo to the catalytic surface, at which it effected beneficial changes to the surface oxygen adsorption energetics in the context of the Sabatier principle.
AB - Improving the efficiency of Pt-based oxygen reduction reaction (ORR) catalysts while also reducing costs remains an important challenge in energy research. To this end, we synthesized highly stable and active carbon-supported Mo-doped PtCu (Mo-PtCu/C) nanoparticles (NPs) from readily available precursors in a facile one-pot reaction. Mo-PtCu/C displays two-tofourfold- higher ORR half-cell kinetics than reference PtCu/C and Pt/C materials, a trend that was confirmed in proof-of-concept experiments by using a H2/O2 microlaminar fuel cell. This Mo-induced activity increase mirrors observations for Mo-PtNi/ C NPs and possibly suggests an emerging trend. Electrochemical- accelerated stability tests revealed that dealloying was greatly reduced in Mo-PtCu/C in contrast to the binary alloys PtCu/C and PtMo/C. Supporting DFT studies suggested that the exceptional stability of Mo-PtCu could be attributed to oxidative resistance of the Mo-doped atoms. Furthermore, our calculations revealed that oxygen could induce segregation of Mo to the catalytic surface, at which it effected beneficial changes to the surface oxygen adsorption energetics in the context of the Sabatier principle.
KW - Alloys
KW - Density functional theory
KW - Doping
KW - Molybdenum
KW - Nanoparticles
UR - http://www.scopus.com/inward/record.url?scp=85040466114&partnerID=8YFLogxK
U2 - 10.1002/cssc.201701822
DO - 10.1002/cssc.201701822
M3 - Artículo
C2 - 29112796
SN - 1864-5631
VL - 11
SP - 193
EP - 201
JO - ChemSusChem
JF - ChemSusChem
IS - 1
ER -