4.8 Article

Facet-Controlled Synthesis of Platinum-Group-Metal Quaternary Alloys: The Case of Nanocubes and {100} Facets

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AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c12368

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  1. Georgia Institute of Technology
  2. National Science Foundation [ECCS-2025462]
  3. DOE Office of Science FWP [ERKCZ55-KC040304]

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This study presents a method for the facet-controlled synthesis of nanocrystals with an ultrathin shell made of a nearly equimolar RuRhPdPt quaternary alloy, showing greatly enhanced activity toward ethanol oxidation. The core-shell nanocubes demonstrate good thermal and electrochemical stability in terms of both geometrical shape and elemental composition, making them a promising candidate for various thermal and electrochemical reactions. The synthetic approach can potentially be extended to fabricate multimetallic catalysts with enhanced activities.
We report a robust method for the facet-controlled synthesis of nanocrystals with an ultrathin shell made of a nearly equimolar RuRhPdPt quaternary alloy. Our strategy involves the use of well-defined Rh cubic seeds, halide-free precursors, and a method for precisely controlling the reaction kinetics of different precursors. In the setting of dropwise addition, the precursors with different reactivities can be reduced at about the same pace for the generation of an alloy with a uniform and well-controlled composition. The core-shell nanocubes show greatly enhanced activity toward ethanol oxidation when benchmarked against Pd and Pt counterparts. Combining in situ and ex situ electron microscopy studies, we also demonstrate that the core-shell nanocubes possess good thermal and electrochemical stability in terms of both geometrical shape and elemental composition, with their cubic shape and alloy composition retained when annealing at 500 degrees C or after long-term electrochemical cycling. It is expected that the synthetic approach can be further extended to fabricate multimetallic catalysts with enhanced activities toward a variety of thermal and electrochemical reactions.

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