In-situ X-ray imaging of reduction-nitridation in ferric oxide under high Pressure

The investigation of high-pressure chemical reaction dynamics has long been constrained by the absence of effective in-situ characterization methods. Here we performed the state-of-the-art synchrotron radiation in-situ X-ray imaging based on large-volume press (LVP) technology to uncover the crucial information on the dynamics of the underlying phenomena of the formation of iron-based spherical product in the high-pressure solid-state metathesis reaction (HSM). We successfully give access to the entire reduction-nitridation process of ferric oxide under the reaction conditions. By analyzing the variation of image intensity (Im) with temperature, two critical stages have been revealed, the formation of nitrogen-containing molten borate Fe[BO]+N[BO] melt and the phase separation of iron nitrides from molten borate. The experimental observation provides direct evidence for the existence of nitrogen-containing molten borate under high pressure, and the formation of molten borate plays a crucial role as a transport medium for nonmetallic ion exchange with metal elements. The M[BO]+N[BO] melt (M=other metals) represents a general pathway for the synthesis of metal nitrides under high pressure. The combination of LVP high-pressure experimental technology with X-ray radioscopy has resulted in a leap in the understanding of reaction dynamics and has opened new paths in the fields of high-pressure chemistry.