Sustainable solid-state synthesis of uniformly distributed PdAg alloy nanoparticles for electrocatalytic hydrogen oxidation and evolution

doi:10.1016/S1872-2067(20)63650-6

Abstract

Abstract:

New sustainable syntheses based on solid-state strategies have sparked enormous attention and provided novel routes for the synthesis of supported metallic alloy nanocatalysts (SMACs). Despite considerable recent progress in this field, most of the developed methods suffer from either complex operations or poorly controlled morphology, which seriously limits their practical applications. Here, we have developed a sustainable strategy for the synthesis of PdAg alloy nanoparticles (NPs) with an ultrafine size and good dispersion on various carbon matrices by directly grinding the precursors in an agate mortar at room temperature. Interestingly, no solvents or organic reagents are used in the synthesis procedure. This simple and green synthesis procedure provides alloy NPs with clean surfaces and thus an abundance of accessible active sites. Based on the combination of this property and the synergistic and alloy effects between Pd and Ag atoms, which endow the NPs with high intrinsic activity, the PdAg/C samples exhibit excellent activities as electrocatalysts for both the hydrogen oxidation and evolution reactions (HOR and HER) in a basic medium. Pd₉Ag₁/C showed the highest activity in the HOR with the largest j_0,m value of 26.5 A g_Pd^-1 and j_0,s value of 0.033 mA cm_Pd ^-2, as well as in the HER, with the lowest overpotential of 68 mV at 10 mA cm^-2. As this synthetic method can be easily adapted to other systems, the present scalable solid-state strategy may open opportunity for the general synthesis of a wide range of well-defined SMACs for diverse applications.

Key words: Solid-state synthesis, Supported metallic alloy nanoparticles, Electrocatalysis, Hydrogen oxidation reaction, Hydrogen evolution reaction

Caili Xu, Qian Chen, Rong Ding, Shengtian Huang, Yun Zhang, Guangyin Fan. Sustainable solid-state synthesis of uniformly distributed PdAg alloy nanoparticles for electrocatalytic hydrogen oxidation and evolution[J]. Chinese Journal of Catalysis, 2021, 42(2): 251-258.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63650-6

https://www.cjcatal.com/EN/Y2021/V42/I2/251

Figures/Tables 6

Fig. 1. Schematic illustration of the synthesis of PdAg/C.

Fig. 2. TEM images and particle size distributions of Pd/C (a, e), Pd9Ag1/C (b, f), Pd1Ag9/C (c, g), and Ag/C (d, h). Insets in a-d are the HRTEM images of the corresponding NPs.

Fig. 3. (a, b) TEM images of Pd5Ag5/C (Inset in b is the HRTEM image of the corresponding NPs); (c) Corresponding particle size distribution; STEM (d) and EDS mapping images (e-g) of Pd5Ag5/C: (e) C, (f) Pd, and (g) Ag.

Fig. 4. XRD patterns (a), XPS survey spectra (b), Ag 3d (c), and Pd 3d (d) XPS spectra of the as-prepared and reference samples.

Fig. 5. (a) HOR polarization curves in H2-saturated 0.1 M KOH; (b) Comparison of the current densities and Pd mass activities at an overpotential of 100 mV; (c) Tafel plots of the HOR/HER kinetic currents and corresponding fittings with the Butler-Volmer equation; (d) j0,s and j0,m values for Pd/C, Pd9Ag1/C, and Pd5Ag5/C; (e) Comparison of the exchange current density (j0,m and j0,s) of Pd9Ag1/C with those of other reported catalysts; (f) Polarization curves of Pd9Ag1/C before and after 1000 CV cycles.

Fig. 6. (a) Polarization curves of Pd/C, Pd9Ag1/C, Pd5Ag5/C, Pd1Ag9/C and Ag/C in 1.0 M KOH. (b) Comparison of the overpotential (@10 mA cm-2) of Pd9Ag1/C and previous Pd-based nanocatalysts. (c) Comparison of the TOF values, mass activity, and Tafel slopes of all the samples; (d) TOF per surface active site and (e) corresponding Tafel plots. (f) Polarization curves of Pd9Ag1/C before and after 1000 CV cycles.

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