We present a combined anion photoelectron spectroscopic and quantum chemical investigation on the structures and bonding properties of CPt2−/0 and CPt2H−/0. The experimental vertical detachment energies of CPt2 and CPt2H are measured to be 1.91 ± 0.08 and 3.54 ± 0.08 eV, respectively. CPt2 is identified as a C2v symmetric Pt—C—Pt bent structure, and CPt2 has a D∞h symmetric Pt—C—Pt linear structure. Both anionic and neutral CPt2H adopt a Pt—C—Pt—H chain-shaped structure, in which the ∠PtCPt and ∠CPtH bond angles of CPt2H are larger than those of CPt2H. The Pt—C bonds in CPt2−/0 and CPt2H−/0 exhibit covalent double bonding characters. The Pt=C bonds are much stronger than the C—H bond that may explain why the C atom CPt2H−/0 prefers to form Pt=C bonds rather than C—H bonds. It may also explain why platinum can insert into the C—H bond to activate the C—H bond as reported in the literature.

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