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X-ray diffraction reveals that the molecular structures of the tris(pyrazolyl)hydroborato and tris(2-pyridylthio)methyl lithium compounds, [TpBut,R]Li (R=H, Me) and [κ 4 -Tptm]Li, respectively exhibit three-coordinate trigonal pyramidal and four-coordinate trigonal monopyramidal coordination geometries, both of which are uncommon for lithium. Accordingly, [TpBut]Li and [TpBut,Me]Li bind additional...