Galvanic Replacement-Driven Transformations of Atomically Intermixed Bimetallic Colloidal Nanocrystals: Effects of Compositional Stoichiometry and Structural Ordering

Li, Guangfang Grace; Sun, Mengqi; Villarreal, Esteban; Pandey, Shubham; Phillpot, Simon R.; Wang, Hui

doi:10.1021/acs.langmuir.8b00448

Galvanic Replacement-Driven Transformations of Atomically Intermixed Bimetallic Colloidal Nanocrystals: Effects of Compositional Stoichiometry and Structural Ordering

Journal Article · Thu Mar 22 00:00:00 EDT 2018 · Langmuir

DOI:https://doi.org/10.1021/acs.langmuir.8b00448· OSTI ID:1470524

Li, Guangfang Grace ^[1]; Sun, Mengqi ^[1]; Villarreal, Esteban ^[1]; Pandey, Shubham ^[2]; Phillpot, Simon R. ^[2]; ^[1]

Univ. of South Carolina, Columbia, SC (United States). Dept. of Chemistry and Biochemistry, Center for Hierarchical Waste Form Materials
Univ. of Florida, Gainesville, FL (United States). Dept. of Materials Science and Engineering

Galvanic replacement reactions dictated by deliberately designed nanoparticulate templates have emerged as a robust and versatile approach that controllably transforms solid monometallic nanocrystals into a diverse set of architecturally more sophisticated multimetallic hollow nanostructures. The galvanic atomic exchange at the nanoparticle/liquid interfaces induces a series of intriguing structure-transforming processes that interplay over multiple time and length scales. Using colloidal Au–Cu alloy and intermetallic nanoparticles as structurally and compositionally fine-tunable bimetallic sacrificial templates, we show that atomically intermixed bimetallic nanocrystals undergo galvanic replacement-driven structural transformations remarkably more complicated than those of their monometallic counterparts. Here, we interpret the versatile structure-transforming behaviors of the bimetallic nanocrystals in the context of a unified mechanistic picture that rigorously interprets the interplay of three key structure-evolutionary pathways: dealloying, Kirkendall diffusion, and Ostwald ripening. By deliberately tuning the compositional stoichiometry and atomic-level structural ordering of the Au–Cu bimetallic nanocrystals, we have been able to fine-maneuver the relative rates of dealloying and Kirkendall diffusion with respect to that of Ostwald ripening through which an entire family of architecturally distinct complex nanostructures are created in a selective and controllable manner upon galvanic replacement reactions. The insights gained from our systematic comparative studies form a central knowledge framework that allows us to fully understand how multiple classic effects and processes interplay within the confinement by a colloidal nanocrystal to synergistically guide the structural transformations of complex nanostructures at both the atomic and nanoparticulate levels.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Hierarchical Waste Form Materials (CHWM)

Sponsoring Organization:: Department of Education; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0016574

OSTI ID:: 1470524

Journal Information:: Langmuir, Journal Name: Langmuir Journal Issue: 14 Vol. 34; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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