Sulfur Migration Enhanced Proton-Coupled Electron Transfer for Efficient CO 2 Desorption with Core-Shelled C@Mn 3 O 4 .

Transforming hazardous species into active sites by ingenious material design was a promising and positive strategy to improve catalytic reactions in industrial applications. To synergistically address the issue of sluggish CO 2 desorption kinetics and SO 2 -poisoning solvent of amine scrubbing, we propose a novel method for preparing a high-performance core-shell C@Mn 3 O 4 catalyst for heterogeneous sulfur migration and in situ reconstruction to active -SO 3 H groups, and thus inducing an enhanced proton-coupled electron transfer (PCET) effect for CO 2 desorption. As anticipated, the rate of CO 2 desorption increases significantly, by 255%, when SO 2 is introduced. On a bench scale, dynamic CO 2 capture experiments reveal that the catalytic regeneration heat duty of SO 2 -poisoned solvent experiences a 32% reduction compared to the blank case, while the durability of the catalyst is confirmed. Thus, the enhanced PCET of C@Mn 3 O 4 , facilitated by sulfur migration and simultaneous transformation, effectively improves the SO 2 resistance and regeneration efficiency of amine solvents, providing a novel route for pursuing cost-effective CO 2 capture with an amine solvent.