“Outside‐in” Design of Single‐Atom Catalysts: Linking Specific Peripheral Geometry to Defined CO 2 Reduction Performance

RR intermediates (COOH* and CO*), enhancing catalytic performance for CO production. Extensive experimental studies corroborate these theoretical findings. The proposed "outside-in" design strategy can be extended to Ni SACs, offering new insights into the exploration of highly efficient single-atom centers through peripheral geometric effects.