A Phosphorus‐Bridged Spin Trigger for Oxygen Reduction
Abstract
Abstract Precise control over the spin degree of freedom of catalytic metal centers represents a significant challenge in enhancing the oxygen reduction reaction (ORR). In this work, we report a phosphorus(P)‐bridged composite comprising Fe single atoms (SAs) and atomic clusters (ACs), Fe SA/AC /PNC, wherein the Fe SA ‐P‐Fe AC structure functions as an efficient electron channel and, more importantly, a spin trigger. This trigger induces a spin‐state transition of Fe II from low‐spin (S = 0) to medium‐spin (S = 1), as unequivocally deciphered by advanced spectroscopic and magnetic analyses. This spin‐state reconstruction directly optimizes the reaction pathway by enhancing O 2 adsorption and facilitating *OH desorption. The resulting catalyst exhibits exceptional oxygen reduction activity in both acidic and neutral media, with half‐wave potentials of 0.852 and 0.831 V, respectively, and achieves a peak power density of 1.35 W cm −2 in proton exchange membrane fuel cells (PEMFCs). This strategy is universally effective for Co and Ni systems, establishing spin‐state engineering as a general principle for designing high‐performance non‐precious metal catalysts.
Article Details
Authors (9)
Wu Wang
Department of Physics
Xiaoyang Cheng
State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen P. R. China
Hong‐Guan Li
School of Metallurgy Northeastern University Shenyang P. R. China
Min‐Le Li
State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen P. R. China
Long Chen
Department of Chemistry, Frontiers Science Center for New Organic Matter and State Key Laboratory of Advanced Chemical Power Sources, College of Chemistry
Jian Yang
Yan‐Xia Jiang
State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen P. R. China
Rui Huang
School of Chemistry
Shi‐Gang Sun
State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical Engineering Xiamen University Xiamen P. R. China