Influence of Size-Induced Oxidation State of Platinum Nanoparticles on Selectivity and Activity in Catalytic Methanol Oxidation in the Gas Phase
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- Influence of Size-Induced Oxidation State of Platinum Nanoparticles on Selectivity and Activity in Catalytic Methanol Oxidation in the Gas Phase
- Wang, Hailiang; Wang, Yihai; Zhu, Zhongwei; Sapi, Andras; An, Kwangjin; Kennedy, Griffin; Michalak, William D.; Somorjai, Gabor A.
- Heterogeneous catalysis; methanol oxidation; Pt nanoparticles; size effect
- Issue Date
- AMER CHEMICAL SOC
- NANO LETTERS, v.13, no.6, pp.2976 - 2979
- Pt nanoparticles with various sizes of 1, 2, 4, and 6 nm were synthesized and studied as catalysts for gas-phase methanol oxidation reaction toward formaldehyde and carbon dioxide under ambient pressure (10 Torr of methanol, 50 Torr of oxygen, and 710 Torr of helium) at a low temperature of 60 °C. While the 2, 4, and 6 nm nanoparticles exhibited similar catalytic activity and selectivity, the 1 nm nanoparticles showed a significantly higher selectivity toward partial oxidation of methanol to formaldehyde, but a lower total turnover frequency. The observed size effect in catalysis was correlated to the size-dependent structure and oxidation state of the Pt nanoparticles. X-ray photoelectron spectroscopy and infrared vibrational spectroscopy using adsorbed CO as molecular probes revealed that the 1 nm nanoparticles were predominantly oxidized while the 2, 4, and 6 nm nanoparticles were largely metallic. Transmission electron microscopy imaging witnessed the transition from crystalline to quasicrystalline structure as the size of the Pt nanoparticles was reduced to 1 nm. The results highlighted the important impact of size-induced oxidation state of Pt nanoparticles on catalytic selectivity as well as activity in gas-phase methanol oxidation reactions. © 2013 American Chemical Society.
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