Precise control of alloying sites of bimetallic nanoclusters via surface motif exchange reaction

Yao, Qiaofeng; Feng, Yan; Fung, Victor; Yu, Yong; Jiang, De-en; Yang, Jun; Xie, Jianping

doi:10.1038/s41467-017-01736-5

Precise control of alloying sites of bimetallic nanoclusters via surface motif exchange reaction

Journal Article · Thu Nov 16 04:00:00 EST 2017 · Nature Communications

DOI:https://doi.org/10.1038/s41467-017-01736-5· OSTI ID:1489404

^[1]; Feng, Yan ^[2]; Fung, Victor ^[3]; ^[1]; Jiang, De-en ^[3]; Yang, Jun ^[4]; ^[1]

National Univ. of Singapore (Singapore). Dept. of Chemical and Biomolecular Engineering
National Univ. of Singapore (Singapore). Dept. of Chemical and Biomolecular Engineering; Chinese Academy of Sciences (CAS), Beijing (China). State Key Lab. of Multiphase Complex Systems
Univ. of California, Riverside, CA (United States). Dept. of Chemistry
Chinese Academy of Sciences (CAS), Beijing (China). State Key Lab. of Multiphase Complex Systems

Here, precise control of alloying sites has long been a challenging pursuit, yet little has been achieved for the atomic-level manipulation of metallic nanomaterials. Here we describe utilization of a surface motif exchange (SME) reaction to selectively replace the surface motifs of parent [Ag₄₄(SR)₃₀]^4– (SR = thiolate) nanoparticles (NPs), leading to bimetallic NPs with well-defined molecular formula and atomically-controlled alloying sites in protecting shell. A systematic mass (and tandem mass) spectrometry analysis suggests that the SME reaction is an atomically precise displacement of SR–Ag(I)–SR-protecting modules of Ag NPs by the incoming SR–Au(I)–SR modules, giving rise to a core-shell [Ag₃₂@Au₁₂(SR)₃₀]^4–. Theoretical calculation suggests that the thermodynamically less favorable core-shell Ag@Au nanostructure is kinetically stabilized by the intermediate Ag₂₀ shell, preventing inward diffusion of the surface Au atoms. The delicate SME reaction opens a door to precisely control the alloying sites in the protecting shell of bimetallic NPs with broad utility.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1489404

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 8; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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