Sulfur Migration Enhanced Proton-Coupled Electron Transfer for Efficient CO₂ Desorption with Core-Shelled C@Mn₃O₄

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 CO₂ desorption kinetics and SO₂-poisoning solvent of amine scrubbing, we propose a novel method for preparing a high-performance core-shell C@Mn₃O₄ catalyst for heterogeneous sulfur migration and in situ reconstruction to active -SO₃H groups, and thus inducing an enhanced proton-coupled electron transfer (PCET) effect for CO₂ desorption. As anticipated, the rate of CO₂ desorption increases significantly, by 255%, when SO₂ is introduced. On a bench scale, dynamic CO₂ capture experiments reveal that the catalytic regeneration heat duty of SO₂-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@Mn₃O₄, facilitated by sulfur migration and simultaneous transformation, effectively improves the SO₂ resistance and regeneration efficiency of amine solvents, providing a novel route for pursuing cost-effective CO₂ capture with an amine solvent.