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. 2021 May 19:9:683450.
doi: 10.3389/fchem.2021.683450. eCollection 2021.

Facile Synthesis of Pd@PtM (M = Rh, Ni, Pd, Cu) Multimetallic Nanorings as Efficient Catalysts for Ethanol Oxidation Reaction

Xingqiao Wu  1 , Xiao Li  1 , Yucong Yan  1   2 , Sai Luo  1 , Jingbo Huang  1 , Junjie Li  1 , Deren Yang  1 , Hui Zhang  1   3
Affiliations

Facile Synthesis of Pd@PtM (M = Rh, Ni, Pd, Cu) Multimetallic Nanorings as Efficient Catalysts for Ethanol Oxidation Reaction

Xingqiao Wu et al. Front Chem. .

Abstract

Pt-based multimetallic nanorings with a hollow structure are attractive as advanced catalysts due to their fantastic structure feature. However, the general method for the synthesis of such unique nanostructures is still lack. Here we report the synthesis of Pd@PtM (M = Rh, Ni, Pd, Cu) multimetallic nanorings by selective epitaxial growth of Pt alloyed shells on the periphery of Pd nanoplates in combination with oxidative etching of partial Pd in the interior. In situ generation of CO and benzoic acid arising from interfacial catalytic reactions between Pd nanoplates and benzaldehyde are critical to achieve high-quality Pt-based multimetallic nanorings. Specifically, the in-situ generated CO promotes the formation of Pt alloyed shells and their epitaxial growth on Pd nanoplates. In addition, the as-formed benzoic acid and residual oxygen are responsible for selective oxidative etching of partial Pd in the interior. When evaluated as electrocatalysts, the Pd@PtRh nanorings exhibit remarkably enhanced activity and stability for ethanol oxidation reaction (EOR) compared to the Pd@PtRh nanoplates and commercial Pt/C due to their hollow nanostructures.

Keywords: electrocatalysis; epitaxial growth; interfacial catalytic reactions; multimetallic nanocrystals; nanorings.

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Conflict of interest statement

The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.

Figures

Figure 1
Figure 1
(A) TEM, (B) atomic-resolution HAADF-STEM, (C) EDX mapping images of the planar Pd@PtRh nanorings. (D) TEM, (E) HAADF-STEM, (F) EDX mapping images of the vertically upstanding Pd@PtRh nanorings.
Figure 2
Figure 2
TEM and HAADF-STEM-EDX mapping images for (A,D) Pd@PtNi nanorings, (B,E) Pd@PtPd nanorings, and (C,F) Pd@PtCu nanorings, respectively.
Figure 3
Figure 3
(A) GC-MS spectra of three residual solutions including the reaction solution of Pd@PtRh nanorings, nanoplates, and the standard sample containing (1) benzene, (2) toluene, (3) BAl, (4) BA, and (5) benzoic acid. (B) Possible reaction pathways for BAL under the solvothermal process in the presence of the Pd nanoplates. (C) Scheme for the epitaxial growth and in-situ etching of Pd@PtM (M = Rh, Ni, Cu, Pd) nanorings realized by interface catalytic reactions.
Figure 4
Figure 4
Electrochemical characterization of carbon supported Pd@PtRh nanorings, Pd@PtRh nanoplates, and Pt/C catalysts: (A) CV curves in 0.1 M HClO4 solution at a scan rate of 50 mV/s; (B,C) CV curves normalized with ECSAs and Pt mass, respectively, in a mixed solution containing 0.5 M H2SO4 and 0.5 M EtOH at a scan rate of 50 mV/s; (D) i-t curves at 0.9 V (vs. RHE) for 1000 s; (E) specific activities and ECSAs; (F) mass activities normalized with metals and Pt mass, respectively.
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