Synergy Effect of Acid Radical Anchors and Active Sites Protection in Co‐Based Spinel Catalyst for Efficient Amine Solution Regeneration During CO₂ Capture

Abstract Solid acid catalysts (SACs) have attracted significant attention for their role in enhancing the carbon capture desorption process, primarily due to their active acid sites. By employing a synergistic strategy involving acid anchoring and structural design, both the catalytic activity and durability of the catalyst throughout the desorption process are optimized. The TiO₂ shell layer in the Mn₂CoO₄@TiO₂/SO₄²⁻ (MC@TiO₂/S) catalyst effectively inhibits the leaching of active species into the solution, thereby enabling sustained high activity over ten cycles of absorption–desorption testing. The anchoring of protonated groups (SO₄²⁻) facilitates a novel pathway for proton transfer in solution via proton‐coupled electron transfer (PCET) effect, significantly reducing activation energy for this step and enhancing desorption reaction kinetics. Consequently, CO₂ regeneration capacity and regeneration rate increase by 103% and 111%, respectively, while energy consumption during regeneration decreases by ≈44%. Additionally, the environmental performance of the catalyst is evaluated using life cycle assessment (LCA), highlighting its sustainable potential for future scale‐up applications. This study presents a viable strategy for employing metal oxide solid acid materials to facilitate efficient and low‐energy solvent regeneration in carbon capture processes.