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Functionalized ionic liquids (ILs) show great potential in the application of fuel gas desulfurization. Herein, we report the synthesis and function of two new 1,1,3,3-tetramethylguanidine-based ILs (TMG-based ILs), 1,1,3,3-tetramethylguanidine methoxyacetate ([TMG]­[MOAc]) and 1,1,3,3-tetramethylguanidine ethoxyacetate ([TMG]­[EOAc]). As contrast, two traditional TMG-based ILs, 1,1,3,3-tetramethylguanidine tetrafluoroborate ([TMG]­[BF4]) and 1,1,3,3-tetramethylguanidine acetate ([TMG]­[Ac]) were synthesized. [TMG]­[EOAc] exhibited the highest SO2 capacity (10.33 mol·kg–1 ILs), during which the solubility of SO2 in the ILs was investigated with a reaction equilibrium thermodynamic model (RETM). Remarkably, the absorbed SO2 transformed into cyclic sulfite esters with high yields (up to 99%) in [TMG]­[MOAc] without a traditional desorption process. Thanks to its good stability, the cycloaddition reaction is fully revisable in [TMG]­[MOAc] in five cycling measurements. These coupled applications and molecular insights demonstrate a new type of functional material for SO2 capture and its value-added conversion and also provide a new strategy to deal with harmful gas in the most convenient way.

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