Add time:09/06/2019 Source:sciencedirect.com
Formation of the linear chain ruthenium and osmium carbonyls by successive linkage of mononuclear [M(CO)4Cl2] units and by opening trinuclear clusters [M3(CO)12] and [FeM2(CO)12] (M = Ru, Os) with chlorine gas have been studied by computational DFT methods. Energetically the formation of dinuclear [M2(CO)8Cl2] from [M(CO)4Cl2] units is the most demanding step. The following chain growth by adding new mononuclear units proceeds more easily with nearly constant energy per step. Cluster opening by chlorine gas to obtain trinuclear [M3(CO)12Cl2] is a facile reaction for both ruthenium and osmium clusters as well as for mixed metal clusters. Mixed metal clusters [FeOs2(CO)12] and [FeRu2(CO)12] open preferably between iron–osmium or iron–ruthenium bonds producing linear trinuclear Fe–M–M-type of compound. In the case of mixed metal Os–Ru clusters, the cleavage of Os–Ru bond is not clearly preferred. Fragmentation of the cluster to shorter units cis(Cl)-[M(CO)4Cl2] or [M2(CO)8Cl2] with equatorial chlorides is highly favorable and competes with the cluster opening. No preferences on the bond type (Os–Ru, Os–Os, or Ru–Ru) that are broken can be found in the case of mixed metal Os–Ru clusters.
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