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All‐Metallic Zn=Zn Double‐π Bonded Octahedral Zn 2 M 4 (M=Li, Na) Clusters with Negative Oxidation State of Zinc
Author(s) -
Liu Xingman,
Zhang Min,
Wu Shuixing,
Zhong Ronglin,
Liu Yingying,
Arif Ali Muhammad,
Geng Yun,
Su Zhongmin
Publication year - 2020
Publication title -
chemphyschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.016
H-Index - 140
eISSN - 1439-7641
pISSN - 1439-4235
DOI - 10.1002/cphc.201901051
Subject(s) - delocalized electron , chemistry , crystallography , octahedron , atom (system on chip) , oxidation state , zinc , metal , molecular orbital , atomic orbital , alkali metal , inorganic chemistry , electron , molecule , crystal structure , physics , organic chemistry , quantum mechanics , computer science , embedded system
Zn=Zn double bonded‐especially double‐π bonded‐systems are scarce due to strong Coulomb repulsion caused by the Zn atom's internally crowded d electrons and very high energy of the virtual π orbitals in Zn 2 fragments. It is also rare for Zn atoms to exhibit negative oxidation states within reported Zn−Zn bonded complexes. Herein, we report Zn=Zn double‐π bonded octahedral clusters Zn 2 M 4 (M=Li, Na) bridged by four alkali metal ligands, in which the central Zn atom is in a negative oxidation state. Especially in D 4h −Zn 2 Na 4 , the natural population analysis shows that the charge of the Zn atom reaches up to −0.89 | e | (−1.11 | e | for AIM charge). Although this cooperation inevitably increases the repulsion between two Zn atoms, the introduction of the s 1 ‐type ligands results in occupation of degenerated π orbitals and the electrons being delocalized over the whole octahedral framework as well, in turn stabilizing the octahedral molecular structure. This study demonstrates that maintaining the degeneracy of the π orbitals and introducing electrons from equatorial plane are effective means to construct double‐π bonds between transitional metals.

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