4.8 Article

Phase-Controlled Synthesis of Pd-Sn Nanocrystal Catalysts of Defined Size and Shape

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 44, Pages 51876-51885

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c04801

Keywords

intermetallic; nanocatalysts; bimetallic nanoparticles; alloy; shape control

Funding

  1. Indiana University
  2. U.S. DOE BES Award [DESC0018961]
  3. NSF CRIF [CHE-1048613, DMR MRI 1126394]
  4. IU Electron Microscopy Center
  5. NSF [DGE-1342962]

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The study successfully synthesized phase-controlled Pd-Sn nanoparticles using a one-pot method, which exhibited good catalytic activity, with Pd2Sn quasi-spheres and nanorhombohedra showing the most outstanding performance.
Bimetallic Pd-based nanoparticles (NPs) are of interest as electrocatalysts for formic acid electrooxidation (FAEO) because of their higher initial catalytic activity and CO tolerance when compared to Pt. Intermetallic NPs (i-NPs) with specific geometric and electronic structures generally exhibit superior catalytic activity, selectivity, and durability when compared to their disordered (random alloy) counterparts; however, the colloidal synthesis of i-NPs remains a challenge. Here, a one-pot method was demonstrated as a facile route to obtain monodisperse Pd-Sn NPs with phase control, including intermetallic hexagonal Pd3Sn2 (P6(3)/mmc), intermetallic orthorhombic Pd2Sn (Pnma), and alloy cubic Pd3Sn (FCC, Fm (3) over barm) as size-controlled NPs with quasi-spherical shapes. Initial metal precursor ratios and reaction temperature were critical parameters to achieving phase control. Also, slight modifications of synthetic conditions resulted in either Pd2Sn nanorhombohedra or nanorods with tunable aspect ratios. A systematic evaluation of the Pd-Sn NPs for FAEO showed that most presented higher specific activities when compared to commercial Pd/C, in which Pd2Sn quasi-spheres and nanorhombohedra showed the highest catalytic activity for FAEO. These results highlight the benefits of phase-controlled Pd-based nanocatalysts with defined nanocrystal size and shape, with use of trioctylphospine (TOP) and oleic acid (OA) central to shape and size control.

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