Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
DOI: https://doi.org/10.29363/nanoge.nfm.2022.006
Publication date: 11th July 2022
Transition metal phosphides (TMP) are a promising materials family that has been studied extensively. Still, synthesizing complex and ternary phosphides in a reproducible manner is a challenge, due to the various available oxidation states and crystallographic phases. The various reactivities of the precursors and phase segregation often produce structure of diverse morphologies and compositions. For elucidating the intrinsic properties of these structures as catalysts, such synthetic control is crucial. Here, I will describe a few methods to produce complex ternary structures and their electro-catalytic activity towards hydrogen evolution (HER), oxygen evolution (OER) and alcohol oxidation.
Specifically, I will present a comparative study that illustrates the catalytic activity of three Ni-P phases towards hydrogen production through electrochemical water reduction as well as hydrogen retrieval by hydrolysis of hydrogen storage materials (ammonia-borane and NaBH4). I will show that Ni12P5 was recognized as a suitable platform for the electrochemical production of γ-NiOOH—a particularly active phase—because of its matching crystallographic structure. An additional incorporation of tungsten by doping produces surface roughness, increases the electrochemical surface area (ESCA), and reduces the energy barrier for electron-coupled water dissociation (the Volmer step for the formation of Hads). We explored the three different phases of nickel phosphide also for the electro-oxidation of methanol, ethanol, isopropanol, ethylene glycol, and glycerol. Ni12P5 exhibits excellent activity (210 mA cm-2 at 1.72 V vs RHE), durability, and mass activity (~4.2 A mg-1), outperforming the state-of-the-art catalysts. The high selectivity of the reaction and the large suppression of further oxidation to CO2 are a marker of a preferred bidentate adsorption configuration that conveys a specific O–H activation reaction path. The catalysts show excellent activity towards alcohol oxidation and durability, likely thanks to the mild conditions required for the process, which allow the formation of a regenerating thin active layer of oxidized nickel.
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