Low-spin state design of highly active diatomic catalysts for oxygen reduction reaction.

ABSTRACT: Fe-based atomic catalysts are widely considered among the most promising non-noble candidates for the oxygen reduction reaction (ORR). The precise manipulation of spin states directly determines their performance but remains highly challenging. Herein, we demonstrate a source-reduction approach to design a low-spin Fe²⁺/Cu-N-C diatomic catalyst with fully occupied d_z² orbitals. Compared with conventional Fe³⁺ catalysts, the adsorption energy of the *OH intermediate was significantly lowered by minimizing metal-oxygen orbital interactions. In situ synchrotron evidence and ab initio molecular dynamics simulations further reveal the unusually rapid O-O bond cleavage for *OOH dissociation that is viewed as another key rate-limit

SUBMITTER: Li H 

PROVIDER: S-EPMC12839530 | biostudies-literature | 2026 Jan

REPOSITORIES: biostudies-literature