Phytic acid‐doped <scp>H‐Beta</scp> facilitates proton‐coupled electron transfer for efficient carbamate decomposition in <scp> CO ₂ </scp> capture

Abstract Although catalytic amine regeneration can effectively reduce heat duty in CO 2 capture, the insufficient activity and stability of existing solid acid catalysts in high‐temperature basic environments impede their practical implementation. Herein, phosphorus‐doped H‐Beta (P‐Hβ) catalysts were employed for CO 2 desorption for the first time. Phosphorus doping Hβ forms POH, which undergoes in situ reconstruction into active ‐PO 3 H groups, generating abundant strong acid sites (SAS) and enhancing electron transfer efficiency. This synergistic effect significantly enhances the proton‐coupled electron transfer (PCET) process, thereby facilitating CO 2 desorption. The optimal P‐Hβ catalyst improves the CO 2 desorption rate by 368.0%, lowers the activation energy (Ea) by 33.3%, and reduces the regeneration energy consumption by 49.1%, while maintaining stable performance over 10 cycles. Online fourier transform infrared spectroscopy (FT‐IR) analysis reveals the synergistic catalytic mechanism. This work thus provides a novel perspective for designing highly efficient and robust CO 2 desorption catalysts by elucidating the clear mechanism of the PCET process.