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Activity and durability of intermetallic PdZn electrocatalyst for ethanol oxidation reaction

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Abstract

Intermetallic or substitutional solid-solution PdZn alloy nanoparticle (NP)-loaded carbon black (i-PdZn/C, s-PdZn/C) was prepared by reducing equimolar palladium acetate and zinc acetate in ethanol dispersion of carbon black with sodium tetrahydroborate with and without the following heat-treatment in an autoclave. The Pd 3d and Zn 2p core-level spectra exhibited that the binding energy of Pd and Zn for i-PdZn/C shifted positively and negatively compared to that for metallic Pd and Zn sheets, respectively, suggesting a strong electronic interaction between Pd and Zn. In contrast, for s-PdZn/C, the binding energy for Pd shifted positively, but only a peak for ZnO was observed. In 1 M KOH aqueous solution at 20 ºC, the Zn content of s-PdZn/C was almost zero in 30 min, while i-PdZn/C held the Zn component of 75% at 20 ºC and 70% at 60 ºC after 30 min, indicating that i-PdZn/C was much more tolerant to alkaline medium than s-PdZn/C. Consequently, s-PdZn NPs were changed to porous Pd NPs, whereas i-PdZn NPs were changed to core–shell NPs whose surface was porous Pd. In the (1 M KOH + 1 M ethanol) aqueous solution at 20 ºC, i-PdZn/C and s-PdZn/C significantly enhanced the activity for ethanol oxidation reaction (EOR) compared to Pd NP-loaded carbon black (Pd/C). In the potentiostatic electrolysis at 0.7 V for 10,000 s, the deterioration of i-PdZn/C was effectively delayed compared to Pd/C and s-PdZn/C due to the electronic effect of the intermetallic PdZn core.

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Authors and Affiliations

  1. Department of Applied Chemistry, Graduate School of Engineering, Osaka Metropolitan University, Sakai, Osaka, 599-8531, Japan

    Nguyen Trung Kien, Kanaru Hashisake, Masanobu Chiku, Eiji Higuchi & Hiroshi Inoue

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  1. Nguyen Trung Kien
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  2. Kanaru Hashisake
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  3. Masanobu Chiku
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  4. Eiji Higuchi
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  5. Hiroshi Inoue
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Contributions

HI designed the research. NTK and KH performed the preparation of electrodes. NTK, KH and MC preformed and analyzed EDX, XRD, XPS and electrochemical experiments. EH performed TEM measurements and analysis. HI supervised the work. HI and NTK wrote the paper. NTK and KH prepared all figures. All authors have reviewed and agreed to the published version of the manuscript.

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Correspondence to Hiroshi Inoue.

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Kien, N.T., Hashisake, K., Chiku, M. et al. Activity and durability of intermetallic PdZn electrocatalyst for ethanol oxidation reaction. Res Chem Intermed 48, 3795–3810 (2022). https://doi.org/10.1007/s11164-022-04780-z

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