Discovery of chalcogenides structures and compositions using mixed fluxes

Area of Science:

• Solid-state chemistry and materials science.
• Inorganic synthesis and discovery.

Background:

• Modern technology requires continuous materials discovery.
• Designing synthesis routes for new solid-state materials necessitates understanding reactivity.
• Advances in synthesis science are crucial for accelerating materials discovery.

Purpose of the Study:

• To present a highly effective methodology for the rational discovery of solid-state materials.
• To demonstrate a technique using high-temperature solutions or fluxes with tunable solubility.
• To facilitate product selection by projecting the free-energy landscape into synthetic variables.

Main Methods:

• Utilized high-temperature solutions/fluxes with tunable solubility for materials synthesis.
• Employed mixed alkali hydroxide/halide (AOH/AX) fluxes for chalcogenide system synthesis.
• Systematically varied temperature and flux ratios to discover new compounds.

Main Results:

• Synthesized 30 unreported compounds or compositions in the A(Ba)-Cu-Q(O) system (Q=S, Se; A=Na, K, Rb).
• Discovered more than ten unique structural types.
• Observed a decrease in structural dimensionality with increasing reactant solubility and temperature.

Conclusions:

• The presented methodology enables rational discovery of inorganic solids.
• This approach effectively accelerates the discovery of novel materials.
• Tunable solubility in high-temperature fluxes is a key factor in controlling synthesis outcomes.