Structural diversity and hydrogen storage properties in the system K-Si-H

KSiH₃ exhibits 4.1 wt% experimental hydrogen storage capacity and shows reversibility under moderate conditions, which provides fresh impetus to the search for other complex hydrides in the K-Si-H system. Here, we reproduce the stable Fm3̄m phase of K₂SiH₆ and uncover two denser phases, space groups P3̄m1 and P6₃mc at ambient pressure, by means of first-principles structure searches. We note that P3̄m1-K₂SiH₆ has a high hydrogen content of 5.4 wt% and a volumetric density of 88.3 g L⁻¹. Further calculations suggest a favorable dehydrogenation temperature T_des of −20.1/55.8 °C with decomposition into KSi + K + H₂. The higher hydrogen density and appropriate dehydrogenation temperature indicate that K₂SiH₆ is a promising hydrogen storage material, and our results provide helpful and clear guidance for further experimental studies. We found three further potential hydrogen storage materials stable at high pressure: K₂SiH₈, KSiH₇ and KSiH₈. These results suggest the need for further investigations into hydrogen storage materials among such ternary hydrides at high pressure.