Formic acid dehydrogenation reaction on high-performance Pd_xAu_1−x alloy nanoparticles prepared by the eco-friendly slow synthesis methodology

Abstract

Dehydrogenation of formic acid (FA) is considered to be an effective solution for efficient storage and transport of hydrogen. For decades, highly effective catalysts for this purpose have been widely investigated, but numerous challenges remain. Herein, the Pd_xAu_1−x (x = 0, 0.2, 0.4, 0.5, 0.6, 0.8, 1) alloys over the whole composition range were successfully prepared and used to catalyze FA hydrogen production efficiently near room temperature. Small PdAu nanoparticles (5–10 nm) were well-dispersed and supported on the activated carbon to form PdAu solid solution alloys via the eco-friendly slow synthesis methodology. The physicochemical properties of the PdAu alloys were comprehensively studied by utilizing various measurement methods, such as X-ray diffraction (XRD), N₂ adsorption–desorption, high angle annular dark field-scanning transmission electron microscope (HAADF-STEM), X-ray photoelectrons spectroscopy (XPS). Notably, owing to the strong metal-support interaction (SMSI) and electron transfer between active metal Au and Pd, the Pd_0.5Au_0.5 obtained exhibits a turnover frequency (TOF) value of up to 1648 h⁻¹ (313 K, n_Pd+Au/n_FA = 0.01, n_HCOOH/n_HCOONa = 1:3) with a high activity, selectivity, and reusability in the FA dehydrogenation.

Graphical abstract

Keywords

FA dehydrogenation / face-centred cubic structures / PdAu solid solution alloy nanoparticles / slow synthesis methodology / SMSI effect

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant Nos. 52176131 and 51888103), the Natural Science Foundation of Shaanxi Province, China (Grant Nos. 2021JLM-18, 2020JC-04, and 2023KXJ-228), the National Science and Technology Major Project of China (No. J2019-III-0018-0062), and Xi’an Jiaotong University Special Research Project for Basic Research Business Expenses (No. xzy022022043).

Competing interests

The authors declare that they have no competing interests.

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