The role of Pt-FexOy interfacial sites for CO oxidation

Insoo Ro; Isaias B. Aragao; Joseph P. Chada; Yifei Liu; Keishla R. Rivera-Dones; Madelyn R. Ball; Daniela Zanchet; James A. Dumesic; George W. Huber

doi:10.1016/j.jcat.2017.11.021

Dept. of Chemical and Biomolecular Engineering

Research output: Contribution to journal › Article › peer-review

50 Scopus citations

Abstract

Supported Pt catalysts with different Fe/Pt atomic ratios were synthesized using controlled surface reactions to deposit (cyclohexadiene) iron tricarbonyl onto Pt/SiO₂ to create Pt-Fe_xO_y interfacial sites. X-ray photoelectron spectroscopy measurements show that Pt and Fe species exist as metallic Pt and Fe oxides phases, respectively, after treatment in H₂ at 573 K, whereas Fe becomes more oxidized under reaction conditions for CO oxidation at 313 K (CO:O₂ = 1:1). The addition of Fe increases the turnover frequency of Pt₁Fe_x/SiO₂ at 313 K and atmospheric pressure by up to two orders of magnitude compared to Pt/SiO₂. The reaction order with respect to the O₂ partial pressure suggests that O₂ adsorption on the surface is likely to be a rate controlling step for both Pt/SiO₂ and Pt₁Fe_0.2/SiO₂. The enhanced activity over Pt₁Fe_x/SiO₂ catalysts compared to Pt/SiO₂ can be associated with a lower energy barrier for O₂ adsorption and activation over Pt-Fe_xO_y interfacial sites.

Original language	English
Pages (from-to)	19-26
Number of pages	8
Journal	Journal of Catalysis
Volume	358
DOIs	https://doi.org/10.1016/j.jcat.2017.11.021
State	Published - Feb 2018

Keywords

Active site
Bimetallic catalyst
CO oxidation
Controlled surface reactions (CSR)
Interfacial sites

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10.1016/j.jcat.2017.11.021

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title = "The role of Pt-FexOy interfacial sites for CO oxidation",

abstract = "Supported Pt catalysts with different Fe/Pt atomic ratios were synthesized using controlled surface reactions to deposit (cyclohexadiene) iron tricarbonyl onto Pt/SiO2 to create Pt-FexOy interfacial sites. X-ray photoelectron spectroscopy measurements show that Pt and Fe species exist as metallic Pt and Fe oxides phases, respectively, after treatment in H2 at 573 K, whereas Fe becomes more oxidized under reaction conditions for CO oxidation at 313 K (CO:O2 = 1:1). The addition of Fe increases the turnover frequency of Pt1Fex/SiO2 at 313 K and atmospheric pressure by up to two orders of magnitude compared to Pt/SiO2. The reaction order with respect to the O2 partial pressure suggests that O2 adsorption on the surface is likely to be a rate controlling step for both Pt/SiO2 and Pt1Fe0.2/SiO2. The enhanced activity over Pt1Fex/SiO2 catalysts compared to Pt/SiO2 can be associated with a lower energy barrier for O2 adsorption and activation over Pt-FexOy interfacial sites.",

keywords = "Active site, Bimetallic catalyst, CO oxidation, Controlled surface reactions (CSR), Interfacial sites",

author = "Insoo Ro and Aragao, \{Isaias B.\} and Chada, \{Joseph P.\} and Yifei Liu and Rivera-Dones, \{Keishla R.\} and Ball, \{Madelyn R.\} and Daniela Zanchet and Dumesic, \{James A.\} and Huber, \{George W.\}",

note = "Publisher Copyright: {\textcopyright} 2017 Elsevier Inc.",

year = "2018",

month = feb,

doi = "10.1016/j.jcat.2017.11.021",

language = "English",

volume = "358",

pages = "19--26",

journal = "Journal of Catalysis",

issn = "0021-9517",

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T1 - The role of Pt-FexOy interfacial sites for CO oxidation

AU - Ro, Insoo

AU - Aragao, Isaias B.

AU - Chada, Joseph P.

AU - Liu, Yifei

AU - Rivera-Dones, Keishla R.

AU - Ball, Madelyn R.

AU - Zanchet, Daniela

AU - Dumesic, James A.

AU - Huber, George W.

PY - 2018/2

Y1 - 2018/2

N2 - Supported Pt catalysts with different Fe/Pt atomic ratios were synthesized using controlled surface reactions to deposit (cyclohexadiene) iron tricarbonyl onto Pt/SiO2 to create Pt-FexOy interfacial sites. X-ray photoelectron spectroscopy measurements show that Pt and Fe species exist as metallic Pt and Fe oxides phases, respectively, after treatment in H2 at 573 K, whereas Fe becomes more oxidized under reaction conditions for CO oxidation at 313 K (CO:O2 = 1:1). The addition of Fe increases the turnover frequency of Pt1Fex/SiO2 at 313 K and atmospheric pressure by up to two orders of magnitude compared to Pt/SiO2. The reaction order with respect to the O2 partial pressure suggests that O2 adsorption on the surface is likely to be a rate controlling step for both Pt/SiO2 and Pt1Fe0.2/SiO2. The enhanced activity over Pt1Fex/SiO2 catalysts compared to Pt/SiO2 can be associated with a lower energy barrier for O2 adsorption and activation over Pt-FexOy interfacial sites.

AB - Supported Pt catalysts with different Fe/Pt atomic ratios were synthesized using controlled surface reactions to deposit (cyclohexadiene) iron tricarbonyl onto Pt/SiO2 to create Pt-FexOy interfacial sites. X-ray photoelectron spectroscopy measurements show that Pt and Fe species exist as metallic Pt and Fe oxides phases, respectively, after treatment in H2 at 573 K, whereas Fe becomes more oxidized under reaction conditions for CO oxidation at 313 K (CO:O2 = 1:1). The addition of Fe increases the turnover frequency of Pt1Fex/SiO2 at 313 K and atmospheric pressure by up to two orders of magnitude compared to Pt/SiO2. The reaction order with respect to the O2 partial pressure suggests that O2 adsorption on the surface is likely to be a rate controlling step for both Pt/SiO2 and Pt1Fe0.2/SiO2. The enhanced activity over Pt1Fex/SiO2 catalysts compared to Pt/SiO2 can be associated with a lower energy barrier for O2 adsorption and activation over Pt-FexOy interfacial sites.

KW - Active site

KW - Bimetallic catalyst

KW - CO oxidation

KW - Controlled surface reactions (CSR)

KW - Interfacial sites

UR - https://www.scopus.com/pages/publications/85037668214

U2 - 10.1016/j.jcat.2017.11.021

DO - 10.1016/j.jcat.2017.11.021

M3 - Article

AN - SCOPUS:85037668214

SN - 0021-9517

VL - 358

SP - 19

EP - 26

JO - Journal of Catalysis

JF - Journal of Catalysis

ER -

The role of Pt-Fe_xO_y interfacial sites for CO oxidation

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