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

Qiaofeng Yao, Yan Feng, Victor Fung, Yong Yu, Jiang De-en (), Jun Yang () and Jianping Xie ()
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Qiaofeng Yao: National University of Singapore
Yan Feng: National University of Singapore
Victor Fung: University of California
Yong Yu: National University of Singapore
Jiang De-en: University of California
Jun Yang: Institute of Process Engineering, Chinese Academy of Sciences
Jianping Xie: National University of Singapore

Nature Communications, 2017, vol. 8, issue 1, 1-11

Abstract: Abstract 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.

Date: 2017
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DOI: 10.1038/s41467-017-01736-5

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