Binding the Power of Cycloaddition and Cross-Coupling in a Single Mechanism: an Unexpected Bending Journey to Radical Chemistry of Butadiynyl with Conjugated Dienes.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS（2025）
Univ Hawaii Manoa
Abstract
What if an experiment could combine the power of cycloaddition and cross-coupling with the in situ formation of an aromatic molecule in a single collision? Crossed molecular beam experiments augmented with electronic structure and statistical calculations provided compelling evidence on a novel radical route involving 1,3-butadiynyl (HCCCC; X2 & sum;+) radicals synthesizing (substituted) arylacetylenes in the gas phase upon reactions with 1,3-butadiene (CH2CHCHCH2; X1Ag) and 2-methyl-1,3-butadiene (isoprene; CH2C(CH3)CHCH2; X1A'). This elegant mechanism de facto merges two previously disconnected concepts of cross-coupling and cycloaddition-aromatization in a single collision event via the formation of two new C(sp2)-C(sp2) bonds and bending the 180 degrees moiety of the linear 1,3-butadiynyl radical out of the ordinary by 60 degrees to 120 degrees. In addition to its importance to fundamental organic chemistry, this unconventional mechanism links two previously separated routes of gas-phase molecular mass growth processes of polyacetylenes and polycyclic aromatic hydrocarbons (PAHs), respectively, in low-temperature environments such as in cold molecular clouds like the Taurus Molecular Cloud (TMC-1) and in hydrocarbon-rich atmospheres of planets and their moons such as Titan, which revises the established understanding of low-temperature molecular mass growth processes in the Universe.
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