Hydrogen Generation from Water Splitting by 3H₂O + Pd₁₃ → 3H₂ + Pd₁₃O₃ Reaction

Abstract

palladium (Pd) has been considered as one of such advanced reaction catalysts due to their stable structures and a large number of surface-active sites for maximizing atomic utilization efficiencies. Since hydrogen (H 2 ) is a nice pollution-free energy source, the H 2 generation from water (H 2 O) has attracted too much attention. Clusters catalyzing the H 2 O splitting reaction is a promising way to produce H 2 . The precious transition metal palladium (Pd) clusters have been considered as one of such advanced reaction catalysts due to their stable structures and many surfaceactive sites for maximizing atomic utilization efficiencies. Liang et al. [1] studied the dissociation of H 2 O on the Pd 4 and Pd 7 cluster, and found that H 2 O can be split into H 2 +O, OH+H, and O+H+H, and then H 2 +O and OH+H into O+H+H. For palladium, a variety of experimental and theoretical studies addressed properties of Pd surfaces, supported Pd clusters and Pd clusters in the gas phase. [2][3][4][5] The first-principles method has been applied to studies of the adsorption and decomposition of H 2 O on various surfaces and sizes of Pd clusters in the gas phase. [9][10][11][12] The active position of the icosahedron is more due to its special icosahedral structure, also known as the magic number structure in cluster physics. Zhao et al. [13] have studied that the adsorption and dissociation of H 2 O on the Al 13 cluster by density functional theory (DFT). Denis et al. [14] have reported that the process of hydrogen production on the Fe n + (n = 6-15) cluster in experimentally and shown the intrinsic reaction coordinate (IRC) of water dissociated into OH+H by two energy barriers on icosahedra Fe 13 + in theoretically. Benítez et al. [15] theoretically studied the adsorption of CO on neutral and charged Pd 13 clusters by DFT. The adsorption and dissociation of H 2 on the Pd n (n = 4, 6, 13, 19, 55) clusters have also been studied using DFT by Liu et al. [16] The study on the hydrogen storage in the cuboctahedra Pd 13 H n clusters with n = 1, 6, 8, and 14 has also been reported. [17] Experimentally, the far-IR part of the spectra gives evidence for the presence of partly dissociated water on Fe 13 + and Co 13 + are studied, [14,18] and they claim that Fe 13 + clusters readily acquire dissociation pathways at room temperature by DFT calculations. [14] In 2020 years, a prominent hydrogen evolution reaction of a single water molecule on vanadium clusters V n + (3 ≤ n ≤ 30) is observed in the reaction of cationic vanadium clusters with water at room temperature by Zhang et al., and a significant H 2 release is observed for n ≥ 3, deduced from reaction products observed in the mass spectra, V 13 + cluster is The Pd clusters are widely concerned because of their outstanding catalytic capacity. Here such a candidate of Pd 13 cluster with the icosahedron symmetry and multiple active sites is shown. The first-principles calculations reveal that this cluster can maximally catalyze the water-splitting reaction to generate three H 2 from three H ...