Abstract
Due to the large multi-elemental space desired for property screening and optimization, high-entropy alloys (HEAs) hold greater potential over conventional alloys for a range of applications, such as structural materials, energy conversion, and catalysis. However, the relationship between the HEA composition and its local structural/elemental configuration is not well understood, particularly in noble-metal-based HEA nanomaterials, hindering the design and development of nano-HEAs in energy conversion and catalysis applications. Herein, we determined precise atomic-level structural and elemental arrangements in model HEAs composed of RhPtPdFeCo and RuPtPdFeCo to unveil their local characteristics. Notably, by changing just one constituent element in the HEA (Rh to Ru), we found dramatic changes in the elemental arrangement from complete random mixing to a local single elemental ordering feature. Additionally, we demonstrate that the local ordering in RuPtPdFeCo can be further controlled by varying the Ru concentration, allowing us to toggle between local Ru clustering and distinct heterostructures in multicomponent systems. Overall, our study presents a practical approach for manipulating local atomic structures and elemental arrangements in noble-metal-based HEA systems, which could provide in-depth knowledge to mechanistically understand the functionality of noble-metal-based HEA nanomaterials in practical applications.
| Original language | English |
|---|---|
| Pages (from-to) | 2167-2173 |
| Number of pages | 7 |
| Journal | Journal of the American Chemical Society |
| Volume | 146 |
| Issue number | 3 |
| DOIs | |
| State | Published - Jan 24 2024 |
Funding
L.H. acknowledges support from the University of Maryland A. James Clark School of Engineering. Part of the Research was sponsored by the US DOE, Office of Science, Office of Basic Energy Sciences (BES), Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program. Technique development and data analysis were supported by US DOE Office of Science under Early Career award no. ERKCZ55. Microscopy experiments were performed by the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. B.L. and G.W. acknowledge the financial support for this research provided by the National Science Foundation (NSF) (grant no. DMR 1905572). This research was also supported in part by the University of Pittsburgh Center for Research Computing, RRID:SCR_022735, through the computer resources provided. Specifically, this work used the H2P cluster, which is supported by NSF award no. OAC-2117681.
| Funders | Funder number |
|---|---|
| Center for Nanophase Materials Sciences | |
| University of Maryland A. James Clark School of Engineering | |
| National Science Foundation | DMR 1905572 |
| U.S. Department of Energy | |
| Office of Science | ERKCZ55 |
| Basic Energy Sciences | |
| Oak Ridge National Laboratory | |
| University of Pittsburgh | OAC-2117681, SCR_022735 |