Relating the composition of PtxRu100-x/C nanoparticles to their structural aspects and electrocatalytic activities in the methanol oxidation reaction

Fadlilatul Taufany; Chun Jern Pan; Feng Ju Lai; Hung Lung Chou; Loka Subramanyam Sarma; John Rick; Jhih Min Lin; Jyh Fu Lee; Mau Tsu Tang; Bing Joe Hwang

doi:10.1002/chem.201202473

Relating the composition of Pt_xRu_100-x/C nanoparticles to their structural aspects and electrocatalytic activities in the methanol oxidation reaction

Fadlilatul Taufany, Chun Jern Pan, Feng Ju Lai, Hung Lung Chou, Loka Subramanyam Sarma, John Rick, Jhih Min Lin, Jyh Fu Lee, Mau Tsu Tang, Bing Joe Hwang^*

^*Corresponding author for this work

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

12 Citations (Scopus)

Abstract

A controlled composition-based method - that is, the microwave-assisted ethylene glycol (MEG) method - was successfully developed to prepare bimetallic Pt_xRu_100-x/C nanoparticles (NPs) with different alloy compositions. This study highlights the impact of the variation in alloy composition of Pt_xRu_100-x/C NPs on their alloying extent (structure) and subsequently their catalytic activity towards the methanol oxidation reaction (MOR). The alloying extent of these Pt_xRu _100-x/C NPs has a strong influence on their Pt d-band vacancy and Pt electroactive surface area (Pt ECSA); this relationship was systematically evaluated by using X-ray absorption (XAS), scanning electron microscopy (SEM) coupled with energy dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM), density functional theory (DFT) calculations, and electrochemical analyses. The MOR activity depends on two effects that act in cooperation, namely, the number of active Pt sites and their activity. Here the number of active Pt sites is associated with the Pt ECSA value, whereas the Pt-site activity is associated with the alloying extent and Pt d-band vacancy (electronic) effects. Among the Pt_xRu_100-x/C NPs with various Pt:Ru atomic ratios (x=25, 50, and 75), the Pt₇₅Ru ₂₅/C NPs were shown to be superior in MOR activity on account of their favorable alloying extent, Pt d-band vacancy, and Pt ECSA. This short study brings new insight into probing the synergistic effect on the surface reactivity of the Pt_xRu_100-x/C NPs, and possibly other bimetallic Pt-based alloy NPs. Control and catalysis: This study reports a controlled composition-based synthesis and characterization of selected bimetallic Pt_xRu_100-x/C nanoparticles and simultaneously demonstrates their physiochemical properties - that is, their alloying extent and electronic structure - by focusing on the catalytic activity (see figure). A methanol oxidation reaction was used as a model system.

Original language	English
Pages (from-to)	905-915
Number of pages	11
Journal	Chemistry - A European Journal
Volume	19
Issue number	3
DOIs	https://doi.org/10.1002/chem.201202473
Publication status	Published - 14 Jan 2013

Keywords

alloys
electronic effects
oxidation
platinum
ruthenium

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10.1002/chem.201202473

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Taufany, F., Pan, C. J., Lai, F. J., Chou, H. L., Sarma, L. S., Rick, J., Lin, J. M., Lee, J. F., Tang, M. T., & Hwang, B. J. (2013). Relating the composition of Pt_xRu_100-x/C nanoparticles to their structural aspects and electrocatalytic activities in the methanol oxidation reaction. Chemistry - A European Journal, 19(3), 905-915. https://doi.org/10.1002/chem.201202473

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title = "Relating the composition of PtxRu100-x/C nanoparticles to their structural aspects and electrocatalytic activities in the methanol oxidation reaction",

abstract = "A controlled composition-based method - that is, the microwave-assisted ethylene glycol (MEG) method - was successfully developed to prepare bimetallic PtxRu100-x/C nanoparticles (NPs) with different alloy compositions. This study highlights the impact of the variation in alloy composition of PtxRu100-x/C NPs on their alloying extent (structure) and subsequently their catalytic activity towards the methanol oxidation reaction (MOR). The alloying extent of these PtxRu 100-x/C NPs has a strong influence on their Pt d-band vacancy and Pt electroactive surface area (Pt ECSA); this relationship was systematically evaluated by using X-ray absorption (XAS), scanning electron microscopy (SEM) coupled with energy dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM), density functional theory (DFT) calculations, and electrochemical analyses. The MOR activity depends on two effects that act in cooperation, namely, the number of active Pt sites and their activity. Here the number of active Pt sites is associated with the Pt ECSA value, whereas the Pt-site activity is associated with the alloying extent and Pt d-band vacancy (electronic) effects. Among the PtxRu100-x/C NPs with various Pt:Ru atomic ratios (x=25, 50, and 75), the Pt75Ru 25/C NPs were shown to be superior in MOR activity on account of their favorable alloying extent, Pt d-band vacancy, and Pt ECSA. This short study brings new insight into probing the synergistic effect on the surface reactivity of the PtxRu100-x/C NPs, and possibly other bimetallic Pt-based alloy NPs. Control and catalysis: This study reports a controlled composition-based synthesis and characterization of selected bimetallic PtxRu100-x/C nanoparticles and simultaneously demonstrates their physiochemical properties - that is, their alloying extent and electronic structure - by focusing on the catalytic activity (see figure). A methanol oxidation reaction was used as a model system.",

keywords = "alloys, electronic effects, oxidation, platinum, ruthenium",

author = "Fadlilatul Taufany and Pan, {Chun Jern} and Lai, {Feng Ju} and Chou, {Hung Lung} and Sarma, {Loka Subramanyam} and John Rick and Lin, {Jhih Min} and Lee, {Jyh Fu} and Tang, {Mau Tsu} and Hwang, {Bing Joe}",

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AU - Taufany, Fadlilatul

AU - Pan, Chun Jern

AU - Lai, Feng Ju

AU - Chou, Hung Lung

AU - Sarma, Loka Subramanyam

AU - Rick, John

AU - Lin, Jhih Min

AU - Lee, Jyh Fu

AU - Tang, Mau Tsu

AU - Hwang, Bing Joe

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N2 - A controlled composition-based method - that is, the microwave-assisted ethylene glycol (MEG) method - was successfully developed to prepare bimetallic PtxRu100-x/C nanoparticles (NPs) with different alloy compositions. This study highlights the impact of the variation in alloy composition of PtxRu100-x/C NPs on their alloying extent (structure) and subsequently their catalytic activity towards the methanol oxidation reaction (MOR). The alloying extent of these PtxRu 100-x/C NPs has a strong influence on their Pt d-band vacancy and Pt electroactive surface area (Pt ECSA); this relationship was systematically evaluated by using X-ray absorption (XAS), scanning electron microscopy (SEM) coupled with energy dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM), density functional theory (DFT) calculations, and electrochemical analyses. The MOR activity depends on two effects that act in cooperation, namely, the number of active Pt sites and their activity. Here the number of active Pt sites is associated with the Pt ECSA value, whereas the Pt-site activity is associated with the alloying extent and Pt d-band vacancy (electronic) effects. Among the PtxRu100-x/C NPs with various Pt:Ru atomic ratios (x=25, 50, and 75), the Pt75Ru 25/C NPs were shown to be superior in MOR activity on account of their favorable alloying extent, Pt d-band vacancy, and Pt ECSA. This short study brings new insight into probing the synergistic effect on the surface reactivity of the PtxRu100-x/C NPs, and possibly other bimetallic Pt-based alloy NPs. Control and catalysis: This study reports a controlled composition-based synthesis and characterization of selected bimetallic PtxRu100-x/C nanoparticles and simultaneously demonstrates their physiochemical properties - that is, their alloying extent and electronic structure - by focusing on the catalytic activity (see figure). A methanol oxidation reaction was used as a model system.

AB - A controlled composition-based method - that is, the microwave-assisted ethylene glycol (MEG) method - was successfully developed to prepare bimetallic PtxRu100-x/C nanoparticles (NPs) with different alloy compositions. This study highlights the impact of the variation in alloy composition of PtxRu100-x/C NPs on their alloying extent (structure) and subsequently their catalytic activity towards the methanol oxidation reaction (MOR). The alloying extent of these PtxRu 100-x/C NPs has a strong influence on their Pt d-band vacancy and Pt electroactive surface area (Pt ECSA); this relationship was systematically evaluated by using X-ray absorption (XAS), scanning electron microscopy (SEM) coupled with energy dispersive X-ray spectroscopy (EDX), transmission electron microscopy (TEM), density functional theory (DFT) calculations, and electrochemical analyses. The MOR activity depends on two effects that act in cooperation, namely, the number of active Pt sites and their activity. Here the number of active Pt sites is associated with the Pt ECSA value, whereas the Pt-site activity is associated with the alloying extent and Pt d-band vacancy (electronic) effects. Among the PtxRu100-x/C NPs with various Pt:Ru atomic ratios (x=25, 50, and 75), the Pt75Ru 25/C NPs were shown to be superior in MOR activity on account of their favorable alloying extent, Pt d-band vacancy, and Pt ECSA. This short study brings new insight into probing the synergistic effect on the surface reactivity of the PtxRu100-x/C NPs, and possibly other bimetallic Pt-based alloy NPs. Control and catalysis: This study reports a controlled composition-based synthesis and characterization of selected bimetallic PtxRu100-x/C nanoparticles and simultaneously demonstrates their physiochemical properties - that is, their alloying extent and electronic structure - by focusing on the catalytic activity (see figure). A methanol oxidation reaction was used as a model system.

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Relating the composition of Pt_xRu_100-x/C nanoparticles to their structural aspects and electrocatalytic activities in the methanol oxidation reaction

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