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Isolation and Structural Elucidation of 15‐Nuclear Copper Dihydride Clusters: An Intermediate in the Formation of a Two‐Electron Copper Superatom

Kiran Kumarvarma Chakrahari, Jingping Liao, Rhone P. Brocha Silalahi, Tzu‐Hao Chiu, Jian‐Hong Liao, Xiaoping Wang, Samia Kahlal, Jean‐Yves Saillard, C. W. Liu

2020Small44 citationsDOIOpen Access PDF

Abstract

Abstract Highly reactive copper‐dihydride clusters, [Cu 15 (H) 2 (S 2 CNR 2 ) 6 (C 2 Ph) 6 ](PF 6 ) {R = n Bu ( 1 H ), n Pr ( 2 H ), i Bu ( 3 H )}, are isolated during the reaction of [Cu 28 H 15 {S 2 CN n Bu 2 } 12 ](PF 6 ) with ten equivalents of phenylacetylene. They are found to be intermediates in the formation of the earlier reported two‐electron superatom [Cu 13 (S 2 CNR 2 ) 6 (C 2 Ph) 4 ] + . Better yields are obtained by reacting dithiocarbamate sodium salts, [Cu(CH 3 CN) 4 ](PF 6 ), BH 4 − and phenylacetylene. The presence of two hydrides in the isolated clusters is confirmed by the synthesis and characterization of its deuteride analogue [Cu 15 (D) 2 (S 2 CNR 2 ) 6 (C 2 Ph) 6 ] + , and a single‐crystal neutron structure of 2 H . Structural characterization of 1 H reveals a new bicapped icosahedral copper(I) cage encapsulating a linear copper dihydride (CuH 2 ) − unit. Reaction of 3 H with Au(I) salts yields a highly luminescent [AuCu 12 (S 2 CN i Bu 2 ) 6 (C 2 Ph) 4 ] + cluster.

Topics & Concepts

PhenylacetyleneChemistryCopperCrystallographyIcosahedral symmetryCrystal structureOrganic chemistryCatalysisNanocluster Synthesis and ApplicationsInorganic Chemistry and MaterialsMagnetism in coordination complexes