Nanocomposite Concept for Electrochemical In Situ Preparation of Pt-Au Alloy Nanoparticles for Formic Acid Oxidation
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Nanocomposite Concept for Electrochemical In Situ Preparation of Pt-Au Alloy Nanoparticles for Formic Acid Oxidation. / Du, Jia; Quinson, Jonathan; Zhang, Damin; Wang, Baiyu; Wiberg, Gustav K. H.; Pittkowski, Rebecca K.; Schroeder, Johanna; Simonsen, Soren B.; Kirkensgaard, Jacob J. K.; Li, Yao; Reichenberger, Sven; Barcikowski, Stephan; Jensen, Kirsten M. o.; Arenz, Matthias.
In: JACS Au, Vol. 2, No. 7, 2022, p. 1757-1768.Research output: Contribution to journal › Journal article › Research › peer-review
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TY - JOUR
T1 - Nanocomposite Concept for Electrochemical In Situ Preparation of Pt-Au Alloy Nanoparticles for Formic Acid Oxidation
AU - Du, Jia
AU - Quinson, Jonathan
AU - Zhang, Damin
AU - Wang, Baiyu
AU - Wiberg, Gustav K. H.
AU - Pittkowski, Rebecca K.
AU - Schroeder, Johanna
AU - Simonsen, Soren B.
AU - Kirkensgaard, Jacob J. K.
AU - Li, Yao
AU - Reichenberger, Sven
AU - Barcikowski, Stephan
AU - Jensen, Kirsten M. o.
AU - Arenz, Matthias
PY - 2022
Y1 - 2022
N2 - Herein, we report a straightforward approach for the in situ preparation of Pt-Au alloy nanoparticles from Pt + xAu/C nano -composites using monometallic colloidal nanoparticles as starting blocks. Four different compositions with fixed Pt content and varying Pt to Au mass ratios from 1:1 up to 1:7 were prepared as formic acid oxidation reaction (FAOR) catalysts. The study was carried out in a gas diffusion electrode (GDE) setup. It is shown that the presence of Au in the nanocomposites substantially improves the FAOR activity with respect to pure Pt/C, which serves as a reference. The nanocomposite with a mass ratio of 1:5 between Pt and Au displays the best performance during potentiodynamic tests, with the electro-oxidation rates, overpotential, and poisoning resistance being improved simultaneously. By comparison, too low or too high Au contributions in the nanocomposites lead to an unbalanced performance in the FAOR. The combination of operando small-angle X-ray scattering (SAXS), scanning transmission electron microscopy (STEM) elemental mapping, and wide-angle X-ray scattering (WAXS) reveals that for the nanocomposite with a 1:5 mass ratio, a conversion between Pt and Au from separate nanoparticles to alloy nanoparticles occurs during continuous potential cycling in formic acid. By comparison, the nanocomposites with lower Au contents, for example, 1:2, exhibit less in situ alloying, and the concomitant performance improvement is less pronounced. On applying identical location transmission electron microscopy (IL-TEM), it is revealed that the in situ alloying is due to Pt dissolution and re-deposition onto Au as well as Pt migration and coalescence with Au nanoparticles.
AB - Herein, we report a straightforward approach for the in situ preparation of Pt-Au alloy nanoparticles from Pt + xAu/C nano -composites using monometallic colloidal nanoparticles as starting blocks. Four different compositions with fixed Pt content and varying Pt to Au mass ratios from 1:1 up to 1:7 were prepared as formic acid oxidation reaction (FAOR) catalysts. The study was carried out in a gas diffusion electrode (GDE) setup. It is shown that the presence of Au in the nanocomposites substantially improves the FAOR activity with respect to pure Pt/C, which serves as a reference. The nanocomposite with a mass ratio of 1:5 between Pt and Au displays the best performance during potentiodynamic tests, with the electro-oxidation rates, overpotential, and poisoning resistance being improved simultaneously. By comparison, too low or too high Au contributions in the nanocomposites lead to an unbalanced performance in the FAOR. The combination of operando small-angle X-ray scattering (SAXS), scanning transmission electron microscopy (STEM) elemental mapping, and wide-angle X-ray scattering (WAXS) reveals that for the nanocomposite with a 1:5 mass ratio, a conversion between Pt and Au from separate nanoparticles to alloy nanoparticles occurs during continuous potential cycling in formic acid. By comparison, the nanocomposites with lower Au contents, for example, 1:2, exhibit less in situ alloying, and the concomitant performance improvement is less pronounced. On applying identical location transmission electron microscopy (IL-TEM), it is revealed that the in situ alloying is due to Pt dissolution and re-deposition onto Au as well as Pt migration and coalescence with Au nanoparticles.
KW - nanocomposite electrocatalysts
KW - formic acid oxidation reaction
KW - gas diffusion electrode setup
KW - small-angle X-ray scattering
KW - in situ alloying
KW - ELECTROCATALYTIC ACTIVITY
KW - CELL
KW - ELECTROOXIDATION
KW - REDUCTION
KW - CATALYSTS
KW - NANOSTRUCTURES
U2 - 10.1021/jacsau.2c00335
DO - 10.1021/jacsau.2c00335
M3 - Journal article
C2 - 35911453
VL - 2
SP - 1757
EP - 1768
JO - JACS Au
JF - JACS Au
SN - 2691-3704
IS - 7
ER -
ID: 315759311