Zirconium hydrogen phosphate, ZrH₅(PO₄)₃, is an advanced material that has attracted significant attention in chemistry and materials science due to its unique structural and chemical properties[1]. As part of the zirconium phosphate family, this compound features a robust crystalline framework characterized by zirconium atoms coordinated to phosphate groups. Its high hydrogen content and acidic functional groups make it particularly appealing for applications in ion exchange, catalysis, and energy storage [1].

A key property of ZrH₅(PO₄)₃ is its ability to facilitate proton conduction, which is critical for fuel cells and other electrochemical devices[2]. Additionally, its thermal stability and chemical resistance enhance its versatility, enabling effective performance in harsh operating conditions. Combined with its potential for tunable behavior through chemical modifications [such as other metals (Sc, Cs,..) for Zr][1], these attributes make ZrH₅(PO₄)₃ a promising candidate for sustainable and efficient technologies, particularly in ammonia synthesis under mild conditions.

Ammonia synthesis traditionally relies on the Haber-Bosch process, a method that revolutionized agriculture and industry in the early 20th century. However, this process demands extreme operating conditions — high temperature and pressure — and employs catalysts based on ruthenium or iron, resulting in significant environmental impacts. This underscores the urgent need for greener, more sustainable alternatives.

The present study aims to investigate the efficiency of proton transfer in ZrH₅(PO₄)₃ for ammonia synthesis at room temperature using advanced computational techniques, including ab initio molecular dynamics (AIMD) simulations, density functional theory (DFT) calculations and phonon dispersion calculations. To validate theoretical results against experimental data, the hydrogen positions within the structure were first determined. Three structural configurations were analyzed: one with space group R-3, another with space group R-3c, and a structure with the lowest energy identified from AIMD simulations. Comparing the properties of these structures provides a promising starting point for selecting the optimal configuration to evaluate the mechanism of proton transfer under different conditions for ammonia synthesis, in combination with various catalysts.