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The functionalization of the arsenic transfer reagent [Cp″ 2 Zr(η 1:1 -As 4 )] ( 1 ) focuses on modifying its properties and enabling a broader scope of reactivity. The coordination behavior of 1 towards different Lewis-acidic transition metal complexes and main group compounds is investigated by experimental and computational studies. Depending on the steric requirements of the Lewis acids and the reaction temperature, a variety of new complexes with different coordination modes and coordination numbers could be synthesized. Depending on the Lewis acid (LA) used, a mono-substitution in [Cp″ 2 Zr(µ,η 1:1:1:1 -As 4 )(LA)] (LA = Fe(CO) 4 ( 4 ); B(C 6 F 5 ) 3 ( 7 )) and [Cp″ 2 Zr(µ,η 3:1:1 -As 4 )(Fe(CO) 3 )] ( 5 ) or a di-substitution [Cp″ 2 Zr(µ 3 ,η 1:1:1:1 -As 4 )(LA) 2 ] (LA = W(CO) 5 ( 2 ); CpMn(CO) 2 ( 3 ); AlR 3 ( 6 , R = Me, Et,  i  Bu)) are monitored. In contrast to other coordination products, 5 shows an η 3 coordination in which the butterfly As 4 ligand is rearranged to a cyclo -As 4 ligand. The reported complexes are rationalized in terms of inverse coordination.

Coordination Behavior of [Cp″2Zr(µ1:1-As4)] towards Lewis Acids