Angstrom Confinement‐Triggered Adaptive Spin State Transition of CoMn Dual Single Atoms for Efficient Singlet Oxygen Generation

To achieve high selectivity in the transformation from peroxymonosulfate to singlet oxygen, adaptive tuning of atomic spin state as the peroxymonosulfate structure varied is crucial. The angstrom confinement can effectively tune spin state, but developing an adaptive angstrom-confined atomic system is challenging. Angstrom-confined cobalt (Co) manganese (Mn) dual single atoms within flexible 2D carbon nitride interlayer are constructed to drive adaptive tuning of spin state by changing atomic coordination under angstrom confinement. The in situ characterizations and density functional theory calculations showed that medium-spin Co in Co─N4 absorbed electrons after the adsorption of peroxymonosulfate on CoMn dual single-atom sites and then cleaved O─H of peroxymonosulfate to facilitate *SO5 generation, while the introduction of *SO5 increased interlayer distance and then cleaved Co─N and Mn─N, resulting in the spin state transition from medium to high. Subsequently, the high-spin Co and Mn in Co─N2 and Mn─N2 desorbed the *O2 from *SO5, restoring the initial medium spin state. The adaptive spin state transition enhanced 38.6-fold singlet oxygen yield compared to the unconfined control. The proposed angstrom-confined diatomic strategy is applicable to serial diatomic catalysts, providing an efficient and universal design scheme for singlet oxygen-mediated selective wastewater treatment technology at the atomic level.