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Tuning the electronic structure of Ag-Pd alloys to enhance performance for alkaline oxygen reduction.

ABSTRACT: Alloying is a powerful tool that can improve the electrocatalytic performance and viability of diverse electrochemical renewable energy technologies. Herein, we enhance the activity of Pd-based electrocatalysts via Ag-Pd alloying while simultaneously lowering precious metal content in a broad-range compositional study focusing on highly comparable Ag-Pd thin films synthesized systematically via electron-beam physical vapor co-deposition. Cyclic voltammetry in 0.1?M KOH shows enhancements across a wide range of alloys; even slight alloying with Ag (e.g. Ag_0.1Pd_0.9) leads to intrinsic activity enhancements up to 5-fold at 0.9?V vs. RHE compared to pure Pd. Based on density functional theory and x-ray absorption, we hypothesize that these enhancements arise mainly from ligand effects that optimize adsorbate-metal binding energies with enhanced Ag-Pd hybridization. This work shows the versatility of coupled experimental-theoretical methods in designing materials with specific and tunable properties and aids the development of highly active electrocatalysts with decreased precious-metal content.

SUBMITTER: Zamora Zeledon JA

PROVIDER: S-EPMC7840808 | biostudies-literature | 2021 Jan

REPOSITORIES: biostudies-literature

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Tuning the electronic structure of Ag-Pd alloys to enhance performance for alkaline oxygen reduction.

Zamora Zeledón José A JA Stevens Michaela Burke MB Gunasooriya G T Kasun Kalhara GTKK Gallo Alessandro A Landers Alan T AT Kreider Melissa E ME Hahn Christopher C Nørskov Jens K JK Jaramillo Thomas F TF

Nature communications 20210127 1

Alloying is a powerful tool that can improve the electrocatalytic performance and viability of diverse electrochemical renewable energy technologies. Herein, we enhance the activity of Pd-based electrocatalysts via Ag-Pd alloying while simultaneously lowering precious metal content in a broad-range compositional study focusing on highly comparable Ag-Pd thin films synthesized systematically via electron-beam physical vapor co-deposition. Cyclic voltammetry in 0.1 M KOH shows enhancements across ...[more]

PMID: 33504815

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Project description:Fly ash (FA)-supported bimetallic nanoparticles (PdxAgy/FA) with varying Pd:Ag ratios were prepared by coprecipitation of Pd and Ag involving in situ reduction of Pd(II) and Ag(I) salts in aqueous medium. All the supported nanoparticles were thoroughly characterized with the aid of powder X-ray diffraction (PXRD), X-ray photoelectron spectroscopy (XPS), electron microscopy (field emission scanning electron microscopy (FE-SEM) and transmission electron microscopy (TEM)), and elemental analyses, which include inductively coupled plasma-optical emission spectroscopy (ICP-OES) and energy-dispersive X-ray spectroscopy (EDS). A gradual broadening and shifting of PXRD peaks, ascribable to Ag, to higher angles with an increase in the Pd:Ag ratio affirms the alloying of interface between Pd and Ag nanoparticles. The coexistence of Pd and Ag was further confirmed by EDS elemental mapping as well as by the presence of bimetallic lattices on the FA surface, as evident from the high-resolution TEM analysis. The dependency of crystallite size and average size of bimetallic nanoparticles on Ag loading (mol %) was elucidated with the help of a combination of PXRD and TEM studies. Based on XPS analysis, the charge transfer phenomenon between contacting Pd-Ag sites could be evident from the shifting of 3d core electron binding energy for both Pd and Ag compared with monometallic Pd and Ag nanoparticles. Following a pseudo-first-order reaction kinetics, all the nanocatalysts were able to efficiently reduce 4-nitrophenol into 4-aminophenol in aqueous NaBH4. The superior catalytic performance of the bimetallic nanocatalysts (PdxAgy/FA) over their monometallic (Pd100/FA and Ag100/FA) analogues has been demonstrated. Moreover, the tunable synergistic effect of the bimetallic systems has been explored in detail by varying the Pd:Ag mol ratio in a systematic manner which in turn allowed us to achieve an optimum reaction rate (k = 1.050 min-1) for the nitrophenol reduction using a Pd25Ag75/FA system. Most importantly, all the bimetallic nanocatalysts explored here exhibited excellent normalized rate constants (K ≈ 6000-15,000 min-1 mmol-1) compared with other supported bimetallic Pd-Ag nanocatalysts reported in the literature.

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Tuning the electronic structure of Ag-Pd alloys to enhance performance for alkaline oxygen reduction.

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Tuning the electronic structure of Ag-Pd alloys to enhance performance for alkaline oxygen reduction.

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