Simple Replacement Reaction for the Preparation of Ternary Fe1鈥?i>xPtRux Nanocrystals with Superior Catalytic Activity in Methanol Oxidation Reaction

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• 作者：Di-Yan Wang ; Hung-Lung Chou ; Yen-Chen Lin ; Feng-Ju Lai ; Ching-Hsiang Chen ; Jyh-Fu Lee ; Bing-Joe Hwang ; Chia-Chun Chen
• 刊名：The Journal of the American Chemical Society
• 出版年：2012
• 出版时间：June 20, 2012
• 年：2012
• 卷：134
• 期：24
• 页码：10011-10020
• 全文大小：567K
• 年卷期：v.134,no.24(June 20, 2012)
• ISSN：1520-5126

文摘

The finding of new metal alloyed nanocrystals (NCs) with high catalytic activity and low cost to replace PtRu NCs is a critical step toward the commercialization of fuel cells. In this work, a simple cation replacement reaction was utilized to synthesize a new type of ternary Fe_1鈥?i>xPtRu_x NCs from binary FePt NCs. The detailed structural transformation from binary FePt NCs to ternary Fe_1鈥?i>xPtRu_x NCs was analyzed by X-ray absorption spectroscopy (XAS). Ternary Fe₃₅Pt₄₀Ru₂₅, Fe₃₁Pt₄₀Ru₂₉, and Fe₁₇Pt₄₀Ru₄₃ NCs exhibit superior catalytic ability to withstand CO poisoning in methanol oxidation reaction (MOR) than do binary NCs (FePt and J-M PtRu). Also, the Fe₃₁Pt₄₀Ru₂₉ NCs had the highest alloying extent and the lowest onset potential among the ternary NCs. Furthermore, the origin for the superior CO resistance of ternary Fe_1鈥?i>xPtRu_x NCs was investigated by determining the adsorption energy of CO on the NCs鈥?surfaces and the charge transfer from Fe/Ru to Pt using a simulation based on density functional theory. The simulation results suggested that by introducing a new metal into binary PtRu/PtFe NCs, the anti-CO poisoning ability of ternary Fe_1鈥?i>xPtRu_x NCs was greatly enhanced because the bonding of CO鈥揚t on the NCs鈥?surface was weakened. Overall, our experimental and simulation results have indicated a simple route for the discovery of new metal alloyed catalysts with superior anti-CO poisoning ability and low usage of Pt and Ru for fuel cell applications.