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 Fm3m phase of K2SiH6 and uncover two denser phases, space groups P3m1 and P6(3)mc at ambient pressure, by means of first-principles structure searches. We note that P3m1-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 degrees C with decomposition into KSi + K + H-2. 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.

Automated summary

K2SiH6 is a promising hydrogen storage material with high hydrogen density and appropriate dehydrogenation temperature. Other potential hydrogen storage materials have also been found, which require further investigation under high pressure.