期刊
ACS CATALYSIS
卷 6, 期 8, 页码 5530-5534出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.6b00557
关键词
ORR activity; fuel cells; platinum alloy; nanoparticle stability; intermetallic ordering; kinetic Monte Carlo; dealloying; in situ ICP-MS
资金
- Slovenian Research Agency within NATO Science for Peace Project [EAP.SFPP98492-DURAPEM]
The positive effect of intermetallic ordering of platinum alloy nanoparticles on oxygen reduction reaction (ORR) activity has been well established. What is still missing is an understanding of selective leaching of the less noble metal from the ordered structure and its correlation to long-term ORR performance. Using a combination of kinetic Monte Carlo simulations and advanced characterization techniques, we provide unprecedented insight into dealloying of intermetallic PtCu3 nanoparticles a well-known binary alloy. Comparison of ordered and disordered samples with identical initial compositions and particle size distributions reveals an unexpected correlation: whereas the copper dealloying rates in the ordered and disordered counterparts are almost the same, in the ordered structure Pt atoms are surrounded by 15-30% more Cu atoms throughout all the stages of acid leaching. This more convenient Pt-Cu coordination explains the statistically significant increase of 23-37% in ORR activity of the ordered structure at all stages of alloy degradation.
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