期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202216376
关键词
Electrochemistry; Non-Random Nucleation; Oxidation-Reduction Cycles; Place Exchange; Platinum
By analyzing the distribution of nuclei-distance, it is found that a rare and non-random nucleation process occurs in chemical surface systems. This process involves the formation of special, preferential nucleation sites via a precursor, eventually leading to a semi-ordered Pt-oxide structure. This precursor mechanism may also explain the formation of nano-islands on other surfaces/reactions.
Many chemical surface systems develop ordered nano-islands during repeated reaction and restoration. Platinum is used in electrochemical energy applications, like fuel cells and electrolysers, although it is scarce, expensive, and degrades. During oxidation-reduction cycles, simulating device operation, nucleation and growth of nano-islands occurs that eventually enhances the dissolution. Preventing nucleation would be the most effective solution. However, little is known about the atomic details of the nucleation; a process almost impossible to observe. Here, we analyze the nuclei-distance distribution mapping out the underlying atomic mechanism: a rarely observed, non-random nucleation takes place. Special, preferential nucleation sites that a priori do not exist, develop initially via a precursor and eventually form a semi-ordered Pt-oxide structure. This precursor mechanism seems to be general, possibly explaining also the nano-island formation on other surfaces/reactions.
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