Revealing Reaction Mechanisms and Enabling Materials Discovery in Fluxes through Panoramic Synthesis

TL;DR

This paper shows how panoramic synthesis with in situ diffraction reveals reaction mechanisms in flux methods, enabling the discovery of new materials.

Contribution

The paper introduces panoramic synthesis as a method to uncover reaction mechanisms in flux reactions, enabling rational material design.

Findings

Panoramic synthesis using synchrotron X-ray and neutron diffraction reveals dissolution and intermediate phases in flux reactions.

The method enables the discovery of new materials, including complex metal chalcogenides and intermetallics.

Mechanistic insights from panoramic synthesis lead to a novel crystal growth method.

Abstract

Advancements in many modern technologies, including solar cells, batteries, light-emitting diodes, quantum information science, etc., depend on the continuous discovery of novel materials. Flux, or high-temperature solution, reactions have been widely exploited to synthesize materials such as complex metal oxides, chalcogenides, pnictides, and intermetallics. However, as with most solid-state syntheses, high-temperature flux methods function as a “black box,” offering little insight into solvated species, reaction mechanisms, intermediates, or nucleation processes. In this context, panoramic synthesis1 using in situ diffraction techniques is critical for monitoring the dissolution, intermediate phases, and final products in flux reactions. Therefore, through a deeper mechanistic understanding, this approach holds the key to the rational design of synthetic routes leading to new compositional spaces and targeted solid-state materials. We demonstrate that panoramic synthesis, empowered by both synchrotron X-ray and neutron diffraction, can reveal reaction mechanisms in two distinct chemical systems: metal chalcogenides synthesized using molten salts and intermetallics formed in metal fluxes. These mechanistic insights not only facilitate the discovery and design of new materials, even with complex systems featuring unique structures, but also instrumental in developing a novel method for crystal growth. Kanatzidis, M. G., Discovery-Synthesis, Design, and Prediction of Chalcogenide Phases. Inorganic Chemistry
2017,
56 (6), 3158-3173.