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Colloidal Platinum–Copper Nanocrystal Alloy Catalysts Surpass Platinum in Low-Temperature Propene Combustion

丙烯 催化作用 铂金 化学 纳米晶 合金 无机化学 贵金属 化学工程 有机化学 工程类
作者
Nadia Tahsini,An-Chih Yang,Verena Streibel,Baraa Werghi,Emmett D. Goodman,Aisulu Aitbekova,Simon R. Bare,Yuejin Li,Frank Abild-Pedersen,Matteo Cargnello
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:144 (4): 1612-1621 被引量:17
标识
DOI:10.1021/jacs.1c10248
摘要

Low-temperature removal of noxious environmental emissions plays a critical role in minimizing the harmful effects of hydrocarbon fuels. Emission-control catalysts typically consist of large quantities of rare, noble metals (e.g., platinum and palladium), which are expensive and environmentally damaging metals to extract. Alloying with cheaper base metals offers the potential to boost catalytic activity while optimizing the use of noble metals. In this work, we show that PtxCu100-x catalysts prepared from colloidal nanocrystals are more active than the corresponding Pt catalysts for complete propene oxidation. By carefully controlling their composition while maintaining nanocrystal size, alloys with dilute Cu concentrations (15-30% atomic fraction) demonstrate promoted activity compared to pure Pt. Complete propene oxidation was observed at temperatures as low as 150 °C in the presence of steam, and five to ten times higher turnover frequencies were found compared to monometallic Pt catalysts. Through DFT studies and structural and catalytic characterization, the remarkable activity of dilute PtxCu100-x alloys was related to the tuning of the electronic structure of Pt to reach optimal binding energies of C* and O* intermediates. This work provides a general approach toward investigation of structure-property relationships of alloyed catalysts with efficient and optimized use of noble metals.
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