Redox-active Group 13 molecules possess the unusual combination of concomitant redox and acid-base reactivity. These combined properties enable regeneration of a metal hydroxide complex in a cycle for conversion of CO2 into carbonate salts. Reaction of (IP(-))2Al(OH) (M = Al, Ga) with 1 atm of CO2 affords [(IP(-))2Al]2(μ(2)κ(1):κ(2)-OCO2). Subsequent reduction affords MgCO3 or CaCO3 and two equivalents of [(IP(2-))2Al](-), which can be reoxidized to (IP(-))2Al(OH) to close a cycle.