Abstract
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 °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.
| Original language | English |
|---|---|
| Pages (from-to) | 2553-2560 |
| Number of pages | 8 |
| Journal | Journal of the American Chemical Society |
| Volume | 145 |
| Issue number | 4 |
| DOIs | |
| State | Published - Feb 1 2023 |
Funding
This work was supported by start-up funds from the Georgia Institute of Technology. The electron microscopy, XRD, and XPS analyses were conducted at the Georgia Tech Institute for Electronics and Nanotechnology, a member of the National Nanotechnology Coordinated Infrastructure (NNCI), which is supported by the National Science Foundation (ECCS-2025462). EDX spectroscopy analysis was performed at Oak Ridge National Laboratory’s (ORNL) Center for Nanophase Materials Sciences (CNMS), which is a DOE Office of Science User Facility, and it was supported by an Early Career project supported by DOE Office of Science FWP #ERKCZ55–KC040304. This work was supported by start-up funds from the Georgia Institute of Technology. The electron microscopy, XRD, and XPS analyses were conducted at the Georgia Tech Institute for Electronics and Nanotechnology, a member of the National Nanotechnology Coordinated Infrastructure (NNCI), which is supported by the National Science Foundation (ECCS-2025462). EDX spectroscopy analysis was performed at Oak Ridge National Laboratory’s (ORNL) Center for Nanophase Materials Sciences (CNMS), which is a DOE Office of Science User Facility, and it was supported by an Early Career project supported by DOE Office of Science FWP #ERKCZ55-KC040304.