Reconciling structure prediction of alloyed, ultrathin nanowires with spectroscopy

McGuire, Scott C.; Ebrahim, Amani M.; Hurley, Nathaniel; Zhang, Lihua; Frenkel, Anatoly I.; Wong, Stanislaus S.

doi:10.1039/D1SC00627D

Title: Reconciling structure prediction of alloyed, ultrathin nanowires with spectroscopy

Journal Article · Wed May 26 00:00:00 EDT 2021 · Chemical Science

DOI:https://doi.org/10.1039/D1SC00627D· OSTI ID:1780493

McGuire, Scott C. ^[1];

^[2]; Hurley, Nathaniel ^[1]; Zhang, Lihua ^[3];

^[4];

^[1]

Department of Chemistry, Stony Brook University, New York 11794-3400, USA
Department of Materials Science and Chemical Engineering, Stony Brook University, New York 11794-2275, USA
Center for Functional Nanomaterials, Brookhaven National Laboratory, New York 11973, USA
Department of Materials Science and Chemical Engineering, Stony Brook University, New York 11794-2275, USA, Chemistry Division

A number of complementary, synergistic advances are reported herein. First, we describe the ‘first-time’ synthesis of ultrathin Ru₂Co₁ nanowires (NWs) possessing average diameters of 2.3 ± 0.5 nm using a modified surfactant-mediated protocol. Second, we utilize a combination of quantitative EDS, EDS mapping (along with accompanying line-scan profiles), and EXAFS spectroscopy results to probe the local atomic structure of not only novel Ru₂Co₁ NWs but also ‘control’ samples of analogous ultrathin Ru₁Pt₁, Au₁Ag₁, Pd₁Pt₁, and Pd₁Pt₉ NWs. We demonstrate that ultrathin NWs possess an atomic-level geometry that is fundamentally dependent upon their intrinsic chemical composition. In the case of the PdPt NW series, EDS mapping data are consistent with the formation of a homogeneous alloy, a finding further corroborated by EXAFS analysis. By contrast, EXAFS analysis results for both Ru₁Pt₁ and Ru₂Co₁ imply the generation of homophilic structures in which there is a strong tendency for the clustering of ‘like’ atoms; associated EDS results for Ru₁Pt₁ convey the same conclusion, namely the production of a heterogeneous structure. Conversely, EDS mapping data for Ru₂Co₁ suggests a uniform distribution of both elements. In the singular case of Au₁Ag₁, EDS mapping results are suggestive of a homogeneous alloy, whereas EXAFS analysis pointed to Ag segregation at the surface and an Au-rich core, within the context of a core–shell structure. Overall, these cumulative outcomes indicate that only a combined consideration of both EDS and EXAFS results can provide for an accurate representation of the local atomic structure of ultrathin NW motifs.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: Joint Photon Sciences Institute (JPSI) graduate student fellowship; SC0012704; SC0012335; SC0012573; CHE-1807640

OSTI ID:: 1780493

Alternate ID(s):: OSTI ID: 1785943

Report Number(s):: BNL-221570-2021-JAAM; CSHCBM

Journal Information:: Chemical Science, Journal Name: Chemical Science Vol. 12 Journal Issue: 20; ISSN 2041-6520

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

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