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Abstract:
The Zintl concept is important in solid-state chemistry to explain how
some compounds that combine electropositive and main group elements can
be stable at formulas that at their simplest level do not make any
sense. The electronegative elements in such compounds form a polyatomic
electron-accepting molecule inside the solid, a 'polyanion', that fills
its available energy states with electrons from the electropositive
elements to obey fundamental electron-counting rules. Here we use this
concept to discover a large family of filled skutterudites based on the
group 9 transition metals Co, Rh, and Ir, the alkali, alkaline-earth,
and rare-earth elements, and Sb-4 polyanions. Forty-three new filled
skutterudites are reported, with 63 compositional variations-results
that can be extended to the synthesis of hundreds of additional new
compounds. Many interesting electronic and magnetic properties can be
expected in future studies of these new compounds.