Supercritical flow synthesis of PtPdFe alloyed nanoparticles with enhanced lowerature activity and thermal stability for propene oxidation under lean exhaust gas conditions

Hugo Silva, Patricia Hernandez-Fernandez, Ane K. Baden, Henrik L. Hellstern, Anton Kovyakh, Erik Wisaeus, Thomas Smitshuysen, Ib Chorkendorff, Leif H. Christensen, Debasish Chakraborty , Christian Kallesøe*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

Supercritical flow technology was used for the one step production of PtPd and PtPdFe nanoparticles supported on high surface area γ-Al2O3. Fe addition to PtPd nanoparticles enhanced the propene oxidation activity of the fresh catalysts. For instance, the turnover frequency of a catalyst with 0.12 wt% Fe was 0.06 s-1 at 120 °C, three times higher than the analogous PtPd catalyst. Fe was also incorporated as a substitute element for the PtPd precious metal content ((PtPd)x-yFey, x = 0.75 wt% and y = 0-0.25 wt%), and a relationship between the activity for propene oxidation and the ratio of Fe to PtPd was found. The optimum ratio in terms of activity was found for the (PtPd)0.65Fe0.10/γ-Al2O3 catalyst, allowing precious metal savings of 19% when compared to the PtPd/γ-Al2O3 commercial reference catalyst. Additionally, the T50 (temperature of half conversion) for propene oxidation was lowered by 10 °C under fresh conditions and 20 °C, after hydrothermal aging (750 °C/3h, 10% O2, 10% H2O). Synchrotron X-ray powder diffraction showed that Fe incorporation causes contraction of the PtPd lattice, implying that the PtPdFe alloy formation is responsible for the improved propene oxidation activity. Even after aging, the lattice remained contracted suggesting that the alloyed nanoparticles are stable under the harsh operating conditions of catalytic converters. The lattice contraction effect can be associated with the propene oxidation kinetics, leading to a weaker binding of oxygen on the PtPdFe nanoparticle surface, which can induce a higher surface reaction rate.
Original languageEnglish
JournalCatalysis Science and Technology
Volume9
Issue number23
Pages (from-to)6691-6699
Number of pages9
ISSN2044-4753
DOIs
Publication statusPublished - 2019

Cite this

Silva, Hugo ; Hernandez-Fernandez, Patricia ; Baden, Ane K. ; Hellstern, Henrik L. ; Kovyakh, Anton ; Wisaeus, Erik ; Smitshuysen, Thomas ; Chorkendorff, Ib ; Christensen, Leif H. ; Chakraborty , Debasish ; Kallesøe, Christian. / Supercritical flow synthesis of PtPdFe alloyed nanoparticles with enhanced lowerature activity and thermal stability for propene oxidation under lean exhaust gas conditions. In: Catalysis Science and Technology. 2019 ; Vol. 9, No. 23. pp. 6691-6699.
@article{3e8ba27883344b23bb6e3e7253beb3ee,
title = "Supercritical flow synthesis of PtPdFe alloyed nanoparticles with enhanced lowerature activity and thermal stability for propene oxidation under lean exhaust gas conditions",
abstract = "Supercritical flow technology was used for the one step production of PtPd and PtPdFe nanoparticles supported on high surface area γ-Al2O3. Fe addition to PtPd nanoparticles enhanced the propene oxidation activity of the fresh catalysts. For instance, the turnover frequency of a catalyst with 0.12 wt{\%} Fe was 0.06 s-1 at 120 °C, three times higher than the analogous PtPd catalyst. Fe was also incorporated as a substitute element for the PtPd precious metal content ((PtPd)x-yFey, x = 0.75 wt{\%} and y = 0-0.25 wt{\%}), and a relationship between the activity for propene oxidation and the ratio of Fe to PtPd was found. The optimum ratio in terms of activity was found for the (PtPd)0.65Fe0.10/γ-Al2O3 catalyst, allowing precious metal savings of 19{\%} when compared to the PtPd/γ-Al2O3 commercial reference catalyst. Additionally, the T50 (temperature of half conversion) for propene oxidation was lowered by 10 °C under fresh conditions and 20 °C, after hydrothermal aging (750 °C/3h, 10{\%} O2, 10{\%} H2O). Synchrotron X-ray powder diffraction showed that Fe incorporation causes contraction of the PtPd lattice, implying that the PtPdFe alloy formation is responsible for the improved propene oxidation activity. Even after aging, the lattice remained contracted suggesting that the alloyed nanoparticles are stable under the harsh operating conditions of catalytic converters. The lattice contraction effect can be associated with the propene oxidation kinetics, leading to a weaker binding of oxygen on the PtPdFe nanoparticle surface, which can induce a higher surface reaction rate.",
author = "Hugo Silva and Patricia Hernandez-Fernandez and Baden, {Ane K.} and Hellstern, {Henrik L.} and Anton Kovyakh and Erik Wisaeus and Thomas Smitshuysen and Ib Chorkendorff and Christensen, {Leif H.} and Debasish Chakraborty and Christian Kalles{\o}e",
year = "2019",
doi = "10.1039/c9cy00634f",
language = "English",
volume = "9",
pages = "6691--6699",
journal = "Catalysis Science & Technology",
issn = "2044-4753",
publisher = "Royal Society of Chemistry",
number = "23",

}

Supercritical flow synthesis of PtPdFe alloyed nanoparticles with enhanced lowerature activity and thermal stability for propene oxidation under lean exhaust gas conditions. / Silva, Hugo; Hernandez-Fernandez, Patricia; Baden, Ane K.; Hellstern, Henrik L.; Kovyakh, Anton; Wisaeus, Erik; Smitshuysen, Thomas; Chorkendorff, Ib; Christensen, Leif H.; Chakraborty , Debasish; Kallesøe, Christian.

In: Catalysis Science and Technology, Vol. 9, No. 23, 2019, p. 6691-6699.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Supercritical flow synthesis of PtPdFe alloyed nanoparticles with enhanced lowerature activity and thermal stability for propene oxidation under lean exhaust gas conditions

AU - Silva, Hugo

AU - Hernandez-Fernandez, Patricia

AU - Baden, Ane K.

AU - Hellstern, Henrik L.

AU - Kovyakh, Anton

AU - Wisaeus, Erik

AU - Smitshuysen, Thomas

AU - Chorkendorff, Ib

AU - Christensen, Leif H.

AU - Chakraborty , Debasish

AU - Kallesøe, Christian

PY - 2019

Y1 - 2019

N2 - Supercritical flow technology was used for the one step production of PtPd and PtPdFe nanoparticles supported on high surface area γ-Al2O3. Fe addition to PtPd nanoparticles enhanced the propene oxidation activity of the fresh catalysts. For instance, the turnover frequency of a catalyst with 0.12 wt% Fe was 0.06 s-1 at 120 °C, three times higher than the analogous PtPd catalyst. Fe was also incorporated as a substitute element for the PtPd precious metal content ((PtPd)x-yFey, x = 0.75 wt% and y = 0-0.25 wt%), and a relationship between the activity for propene oxidation and the ratio of Fe to PtPd was found. The optimum ratio in terms of activity was found for the (PtPd)0.65Fe0.10/γ-Al2O3 catalyst, allowing precious metal savings of 19% when compared to the PtPd/γ-Al2O3 commercial reference catalyst. Additionally, the T50 (temperature of half conversion) for propene oxidation was lowered by 10 °C under fresh conditions and 20 °C, after hydrothermal aging (750 °C/3h, 10% O2, 10% H2O). Synchrotron X-ray powder diffraction showed that Fe incorporation causes contraction of the PtPd lattice, implying that the PtPdFe alloy formation is responsible for the improved propene oxidation activity. Even after aging, the lattice remained contracted suggesting that the alloyed nanoparticles are stable under the harsh operating conditions of catalytic converters. The lattice contraction effect can be associated with the propene oxidation kinetics, leading to a weaker binding of oxygen on the PtPdFe nanoparticle surface, which can induce a higher surface reaction rate.

AB - Supercritical flow technology was used for the one step production of PtPd and PtPdFe nanoparticles supported on high surface area γ-Al2O3. Fe addition to PtPd nanoparticles enhanced the propene oxidation activity of the fresh catalysts. For instance, the turnover frequency of a catalyst with 0.12 wt% Fe was 0.06 s-1 at 120 °C, three times higher than the analogous PtPd catalyst. Fe was also incorporated as a substitute element for the PtPd precious metal content ((PtPd)x-yFey, x = 0.75 wt% and y = 0-0.25 wt%), and a relationship between the activity for propene oxidation and the ratio of Fe to PtPd was found. The optimum ratio in terms of activity was found for the (PtPd)0.65Fe0.10/γ-Al2O3 catalyst, allowing precious metal savings of 19% when compared to the PtPd/γ-Al2O3 commercial reference catalyst. Additionally, the T50 (temperature of half conversion) for propene oxidation was lowered by 10 °C under fresh conditions and 20 °C, after hydrothermal aging (750 °C/3h, 10% O2, 10% H2O). Synchrotron X-ray powder diffraction showed that Fe incorporation causes contraction of the PtPd lattice, implying that the PtPdFe alloy formation is responsible for the improved propene oxidation activity. Even after aging, the lattice remained contracted suggesting that the alloyed nanoparticles are stable under the harsh operating conditions of catalytic converters. The lattice contraction effect can be associated with the propene oxidation kinetics, leading to a weaker binding of oxygen on the PtPdFe nanoparticle surface, which can induce a higher surface reaction rate.

U2 - 10.1039/c9cy00634f

DO - 10.1039/c9cy00634f

M3 - Journal article

VL - 9

SP - 6691

EP - 6699

JO - Catalysis Science & Technology

JF - Catalysis Science & Technology

SN - 2044-4753

IS - 23

ER -