Abstract
Products of hydrogen cyanide (HCN) reactivity are suspected to play important roles in astrochemistry and, possibly, the origin of life. The composition, chemical structure, and mechanistic details for formation of products from HCN's self-reactions have, however, proven elusive for decades. Here, we elucidate base-catalyzed reaction mechanisms for the formation of diaminomaleonitrile and polyimine in liquid HCN using ab initio molecular dynamics simulations. Both materials are proposed as key intermediates for driving further chemical evolution. The formation of these materials is predicted to proceed at similar rates, thereby offering an explanation of how HCN's self-reactions can diversify quickly under kinetic control. Knowledge of these reaction routes provides a basis for rationalizing subsequent reactivity in astrochemical environments such as on Saturn's moon Titan, in the subsurface of comets, in exoplanet atmospheres, and on the early Earth.