Abstract
Nanoparticles with high-index facets are intriguing because such facets can lend the structure useful functionality, including enhanced catalytic performance and wide-ranging optical tunability. Ligand-free solid-state syntheses of high index-facet nanoparticles, through an alloying-dealloying process with foreign volatile metals, are attractive owing to their materials generality and high yields. However, the role of foreign atoms in stabilizing the high-index facets and the dynamic nature of the transformation including the coarsening and facet regulation process are still poorly understood. Herein, the transformation of Pt salts to spherical seeds and then to tetrahexahedra, is studied in situ via gas-cell transmission electron microscopy. The dynamic behaviors of the alloying and dealloying process, which involves the coarsening of nanoparticles and consequent facet regulation stage are captured in the real time with a nanoscale spatial resolution. Based on additional direct evidence obtained using atom probe tomography and density functional theory calculations, the underlying mechanisms of the alloying-dealloying process are uncovered, which will facilitate broader explorations of high-index facet nanoparticle synthesis.
Original language | English (US) |
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Article number | 3790 |
Journal | Nature communications |
Volume | 14 |
Issue number | 1 |
DOIs | |
State | Published - Dec 2023 |
Funding
We thank Dr. J.K.H. Orbeck and Dr. S.H. Petrosko (Northwestern University) for professional editorial advice and Prof. David Seidman (Northwestern University) for helpful discussions. This material is based on work supported by the Sherman Fairchild Foundation Inc., and Kairos Ventures. K.K. is supported by National Research Foundation of Korea (NRF) Basic Science Research Program grant 2022R1A6A3A03059199. This work made use of the EPIC and NUFAB facility of Northwestern University\u2019s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-2025633), the International Institute for Nanotechnology (IIN), and Northwestern\u2019s MRSEC program (NSF DMR-1720139). Atom-probe tomography was performed at the Northwestern University Center for Atom-Probe Tomography (NUCAPT). The LEAP tomograph at NUCAPT was purchased and upgraded with grants from the NSF-MRI (DMR-0420532) and ONR-DURIP (N00014-0400798, N00014-0610539, N00014-0910781, N00014-1712870) programs. NUCAPT received support from the MRSEC program (NSF DMR-1720139), the SHyNE Resource (NSF ECCS-1542205), and the Initiative for Sustainability and Energy (ISEN) at Northwestern University. The thermal analysis made use of the IMSERC X-Ray Facility at Northwestern University, which has received support from the SHyNE Resource (NSF ECCS-2025633) and Northwestern University. B.S. gratefully acknowledges support from the IIN Postdoctoral Fellowship from the IIN at Northwestern University. We thank Dr. J.K.H. Orbeck and Dr. S.H. Petrosko (Northwestern University) for professional editorial advice\u00A0and Prof. David\u00A0Seidman (Northwestern University) for helpful discussions. This material is based on work supported by the Sherman Fairchild Foundation Inc., and Kairos Ventures. K.K. is supported by National Research Foundation of Korea (NRF) Basic Science Research Program grant 2022R1A6A3A03059199. This work made use of the EPIC and NUFAB facility of Northwestern University\u2019s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-2025633), the International Institute for Nanotechnology (IIN), and Northwestern\u2019s MRSEC program (NSF DMR-1720139). Atom-probe tomography was performed at the Northwestern University Center for Atom-Probe Tomography (NUCAPT). The LEAP tomograph at NUCAPT was purchased and upgraded with grants from the NSF-MRI (DMR-0420532) and ONR-DURIP (N00014-0400798, N00014-0610539, N00014-0910781, N00014-1712870) programs. NUCAPT received support from the MRSEC program (NSF DMR-1720139), the SHyNE Resource (NSF ECCS-1542205), and the Initiative for Sustainability and Energy (ISEN) at Northwestern University. The thermal analysis made use of the IMSERC X-Ray Facility at Northwestern University, which has received support from the SHyNE Resource (NSF ECCS-2025633) and Northwestern University. B.S. gratefully acknowledges support from the IIN Postdoctoral Fellowship from the IIN at Northwestern University.
ASJC Scopus subject areas
- General Chemistry
- General Biochemistry, Genetics and Molecular Biology
- General Physics and Astronomy