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Chalcogenides (Q = S, Se, Te), one of the most important family of materialsin solid-state chemistry, differ from oxides by their ability to formcovalently-bonded (Qn)2- oligomers. Each chalcogen atom within such entityfulfills the octet rule by sharing electrons with other chalcogen atoms butsome antibonding levels are vacant. This makes these oligomers particularlysuited for redox reactions in solid state, namely towards elemental metals witha low redox potential that may be oxidized. We recently used this strategy todesign, at low temperature and in an orientated manner, materials with 2Dinfinite layers through the topochemical insertion of copper into preformedprecursors containing (S2)2- and/or (Se2)2- dimers (i.e. La2O2S2, Ba2F2S2 andLaSe2). Herein we extend the validity of the concept to the redox activity of(S2)2- and (S3)2- oligomers towards 3d transition metal elements (Cu, Ni, Fe)and highlight the strong relationship between the structures of the precursors,BaS2 and BaS3, and the products, BaCu2S2, BaCu4S3, BaNiS2 and BaFe2S3. Clearly,beyond the natural interest for the chemical reactivity of oligomers togenerate compounds, this soft chemistry route may conduct to the rationalconception of materials with a predicted crystal structure.

Unexplored reactivity of (Sn)2- Oligomers with transition metals in low-temperature solid-state reactions