Abstract
The ability to alloy different elements is critical for property tuning and materials discovery. However, general alloying at the nanoscale remains extremely challenging due to strong immiscibility and easy oxidation, particularly for early transition metals that are highly reactive. Here, we report nanoscale alloying using a high-temperature- and high-entropy-based strategy (T∗ΔSmix) to significantly expand the possible alloys and include early transition metals. While high-temperature synthesis favors alloy formation and metal reduction, the high-entropy compositional design is critical to further extending the alloying to strongly repelling combinations (e.g., Au-W) and easily oxidized elements (e.g., Zr). In particular, we explicitly characterized a record 15-element nanoalloy, which showed a solid-solution structure featuring localized strain and lattice distortions as a result of extreme mixing. Our study significantly broadens available compositions of nanoalloys and provides clear guidelines by utilizing the less-explored entropic chemistry.
| Original language | English |
|---|---|
| Pages (from-to) | 2340-2353 |
| Number of pages | 14 |
| Journal | Matter |
| Volume | 4 |
| Issue number | 7 |
| DOIs | |
| State | Published - Jul 7 2021 |
Funding
This work at the University of Maryland is supported by the National Science Foundation (NSF) Scalable Nano-manufacturing project no. 1635221. R.S.-Y.'s and Z.H.'s microscopy efforts were supported by NSF award no. DMR-1809439. L.A.H. and B.H.S. were supported by the Toyota Research Institute . S.E.Z. is supported by STROBE , an NSF Science and Technology Center under grant no. DMR 1548924 . Work at the Molecular Foundry was supported by the Office of Science , Office of Basic Energy Sciences of the US Department of Energy (DOE) under contract no. DE-AC02-05CH11231. This work used resources of the Advanced Photon Source, an Office of Science User Facility operated for the US DOE Office of Science by Argonne National Laboratory and was supported by the US DOE under contract no. DE-AC02- 06CH11357 and the Canadian Light Source and its funding partners. Part of the microscopy work was conducted at the Center for Nanophase Materials Science, which is a US DOE Office of Science User Facility. NIST disclaimer: Certain commercial products or equipment are described in this paper to specify adequately the experimental procedure. In no case does such identification imply recommendation or endorsement by the National Institute of Standards and Technology, nor does it imply that it is necessarily the best available for the purpose. This work at the University of Maryland is supported by the National Science Foundation (NSF) Scalable Nano-manufacturing project no. 1635221. R.S.-Y.'s and Z.H.'s microscopy efforts were supported by NSF award no. DMR-1809439. L.A.H. and B.H.S. were supported by the Toyota Research Institute. S.E.Z. is supported by STROBE, an NSF Science and Technology Center under grant no. DMR 1548924. Work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences of the US Department of Energy (DOE) under contract no. DE-AC02-05CH11231. This work used resources of the Advanced Photon Source, an Office of Science User Facility operated for the US DOE Office of Science by Argonne National Laboratory and was supported by the US DOE under contract no. DE-AC02- 06CH11357 and the Canadian Light Source and its funding partners. Part of the microscopy work was conducted at the Center for Nanophase Materials Science, which is a US DOE Office of Science User Facility. NIST disclaimer: Certain commercial products or equipment are described in this paper to specify adequately the experimental procedure. In no case does such identification imply recommendation or endorsement by the National Institute of Standards and Technology, nor does it imply that it is necessarily the best available for the purpose. Conceptualization, L.H. and Y.Y.; Methodology, Y.Y. J.G. T.L. Q.D. and M.J.; Investigation, Y.Y. Z.H. R.S.-Y. L.A.H. S.E.Z. B.H.S. C.O. A.M.M. D.M. Z.F. P.Z. M.C. Y.M. and J.L.; Writing ? original draft, L.H. and Y.Y.; Writing ? review & editing, all authors; Supervision, L.H. L.H. is a co-founder of HighT-Tech and a member of its scientific advisory board. All research reported in this paper was performed at the University of Maryland or by collaborators and is the intellectual property of the University of Maryland, not HighT-Tech. HighT-Tech has an exclusive license from the University of Maryland for the commercialization of this type of technology.
| Funders | Funder number |
|---|---|
| National Science Foundation | DMR-1809439, 1635221, DMR 1548924 |
| U.S. Department of Energy | DE-AC02-05CH11231, DE-AC02- 06CH11357 |
| National Institute of Standards and Technology | |
| Office of Science | |
| Basic Energy Sciences | |
| Argonne National Laboratory | |
| University of Maryland | |
| Toyota Research Institute |
Keywords
- Ellingham diagram
- MAP2: Benchmark
- entropy-driven alloying
- high-entropy alloys
- high-temperature synthesis
- nanoparticles