Unprecedented Prediction of a B 160 Cluster Stuffed by Dual-Icosahedron B 12 .

Serving as the premise to understand bulk allotropes, boron clusters have been intriguing experimentalists and theoreticians to study their geometries and chemical bonding. Here, we designed a complete core-shell B cluster stuffed by two B cores, which is energetically preferable over the bilayer structure of the same size. The unprecedented peanutlike structure with symmetry has superior stability and exhibits superatomic electronic configuration and spherical aromaticity. Our theoretical work not only proposed the core-shell structure of dual icosahedrons for the first time but also indicated the multi-B core-shell structural pattern in boron particles, bridging to boron crystalline structures.