Observation of Iron Oxide to Nitride Conversion via Liquid Liquid Phase Separation in High pressure Borate Melt

Abstract

High pressure chemistry provides a powerful route to materials that are inaccessible or difficult to synthesize under ambient conditions. However, high pressure chemical reaction processes and mechanisms remain largely unexplored because of the challenges associated with in situ characterization under high pressure and high temperature, particularly within the deeply enclosed sample environment of a large volume press. Here, we employ the state of the art real time synchrotron X ray radiography to image a high pressure chemical reaction at 5.4 GPa and 1700 K within a large volume press. Using Fe2O3 and BN as precursors, we capture the complete dynamic metal oxide to nitride conversion and show that it differs fundamentally from conventional solid state diffusion controlled nitridation. Synchrotron X ray radiography clearly revealed that this conversion involves a two stage liquid liquid separation process (LLPS), including fluid nitrogen and fluid Fe N alloy. On the basis of these observations, we propose a nitrogen driven mechanism for LLPS in borate melts. Specifically, nitrogen reduces metal cations in the borate network, altering their coordination environments and triggering a substantial reorganization of the melt structure. This coordination induced restructuring destabilizes the borate melt and promotes the LLPS of fluid Fe N alloy. Our in-situ observations suggest a general pathway for high pressure metal oxide to nitride conversion. This study provides a direct visualization of a pres-sure-enabled chemical reaction that is inaccessible under ambient conditions, offering fundamental in-sight into how high pressure reshapes chemical reaction pathways and enables the synthesis of metal nitrides.