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Joint experimental and theoretical studies have confirmed that the boronyl group(BO)is a monovalent σradical with a robust B O triple bond,where BO/BO-are isovalent to CN/CN- and CO.On the basis of theBO/Au/H isolobal analogy,we have successfully produced and characterized a variety of gas-phase clusters withμ"-BO groups(n =1,2,3).These include terminal μ1-BO in linear B(BO)2-/0 and B2(BO)2-/-/0,triangularB(BO)3-/0,tetrahedral B(BO)4-,planar B3(BO)n-(n=1,2),B4(BO)n-(n=1-3),B10(BO)-and B12(BO)- and B12(BO)-,double-chain nanoribbon Bn(BO)2-/0 with πplusσdouble conjugation,and metal boronyl clusters Aun(BO)-and Aun(BO)(n =1-3)1,bridging μ2-BO in planar B2(BO)3- and B3(BO)3- and face-capping μ3-BO in octahedral B6(BO)7- species2.Interestingly,the perfectly planar boronyl boroxine D3hB3O3(BO)3with threeμ1-BO terminals represents a newmember of the “inorganic benzene” family,while the newly reported B3On-/0/+clusters(n = 2-4)3possess novel3c-2e ω-bonds and rhombic 4c-2e ο-bonds.Similar to BO,the BS group can also serve as effective terminal4andbridging groups.In short,parallel to CN,the μn-BO and μn-BS(n=1,2,3)groups enrich the chemistry of boronand open the area of boronyl chemistry.