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Strain-Enhanced Metallic Intermixing in Shape-Controlled Multilayered Core–Shell Nanostructures: Toward Shaped Intermetallics
Authors:Benjamin P Williams  Dr Allison P Young  Ilektra Andoni  Dr Yong Han  Wei-Shang Lo  Matthew Golden  Jane Yang  Lian-Ming Lyu  Prof Dr Chun-Hong Kuo  Prof Dr James W Evans  Prof Dr Wenyu Huang  Prof Dr Chia-Kuang Tsung
Institution:1. Department of Chemistry, Merkert Chemistry Center, Boston College, 2609 Beacon Street, Chestnut Hill, MA, 02467 USA

These authors contributed equally to this work.;2. Department of Chemistry, Merkert Chemistry Center, Boston College, 2609 Beacon Street, Chestnut Hill, MA, 02467 USA;3. Ames Laboratory—USDOE and Department of Physics & Astronomy, Iowa State University, Ames, IA, 50011 USA;4. Department of Materials Science and Engineering, National Tsing Hua University, Hsinchu, 30013 Taiwan;5. Institute of Chemistry, Academia Sinica, No. 128, Section 2, Academia Rd, Nangang District, Taipei City, 115 Taiwan;6. Ames Laboratory—USDOE and Department of Chemistry, Iowa State University, Ames, IA, 50011 USA

Abstract:Controlling the surface composition of shaped bimetallic nanoparticles could offer precise tunability of geometric and electronic surface structure for new nanocatalysts. To achieve this goal, a platform for studying the intermixing process in a shaped nanoparticle was designed, using multilayered Pd-Ni-Pt core–shell nanocubes as precursors. Under mild conditions, the intermixing between Ni and Pt could be tuned by changing layer thickness and number, triggering intermixing while preserving nanoparticle shape. Intermixing of the two metals is monitored using transmission electron microscopy. The surface structure evolution is characterized using electrochemical methanol oxidation. DFT calculations suggest that the low-temperature mixing is enhanced by shorter diffusion lengths and strain introduced by the layered structure. The platform and insights presented are an advance toward the realization of shape-controlled multimetallic nanoparticles tailored to each potential application.
Keywords:multilayered core–shell nanostructures  shaped intermetallic nanoparticles  strain-enhanced metallic intermixing
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