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

Phys Chem Chem Phys. 2022 Jun 1;24(21):13033-13039. doi: 10.1039/d2cp00298a.

Abstract

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 Fmm phase of K2SiH6 and uncover two denser phases, space groups Pm1 and P63mc at ambient pressure, by means of first-principles structure searches. We note that Pm1-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 Tdes 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.