Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.101
Publication date: 16th December 2024
To realize the electrocatalytic nitrogen reduction reaction (NRR) numerous material systems have been experimentally investigated but their NRR activity and selectivity are far from satisfactory and thus very challenging. There is potential to approach this challenge with catalyst nanoengineering including facet-controlled growth, vacancy engineering, heteroatom doping and the fabrication of composite catalyst structures.[1] Gas phase synthesis routes like chemical vapor deposition (CVD) are promising as they allow the fabrication different materials including oxides, carbides, nitrides and sulfides on the nanoscale, while also offering the potential to tune the material properties by variation of the deposition parameters.
ZrN has been identified as a promising catalyst material for NRR,[2] as it owns electronic properties comparable to noble metals, while being cheap and abundant.
Since theoretical investigations suggest the highest selectivity and stability under typical electrochemical conditions of the (100) facets of rock salt structured ZrN,[3] we followed a metal organic chemical vapor deposition (MOCVD) approach to synthesize facet-controlled ZrN along the (100) plane. Through variation of the process parameters including the precursor choice, the substrate and the deposition temperature, crystalline ZrN (100) layers were grown on Si and glassy carbon substrates. Complementary analysis of the films by X-ray diffraction (XRD) , Rutherford backscattering spectrometry in combination with nuclear reaction analysis (RBS/NRA), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and transmission electron microscopy (TEM) were conducted to gain more insights into the catalyst material. Interestingly, ZrN rapidly oxidizes when exposed to ambient conditions and forms amorphous ZrOxNy species on the surface. This was further substantiated by ab initio molecular dynamics simulations (aiMD), while first proof of principle electrochemical experiments hint towards a potential activity of this material.[4] While further electrochemical experiments need to be conducted in an attempt to prove the genuine NRR of this material, alternative composite catalyst materials based on the reported MoS2/Ru[5] structure are currently developed by MOCVD approach.
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