Designing and Understanding the Outstanding Tri‐Iodide Reduction of N‐Coordinated Magnetic Metal Modified Defect‐Rich Carbon Dodecahedrons in Photovoltaics

Nitrogen‐coordinated metal‐modified carbon is regarded as a novel frontier electrocatalyst in energy conversion devices. However, the construction of intrinsic defects in a carbon matrix remains a great challenge. Herein, N‐coordinated magnetic metal (Fe, Co) modified porous carbon dodecahedrons (Fe/Co‐NPCD) with a large surface area, rich intrinsic defects, and evenly distributed metal‐N x species are successfully synthesized via the rational design of iron precursor and the bimetallic‐organic frameworks. Because of a synergistic effect between N‐coordinated dual magnetic metal active sites, the Fe/Co‐NPCD exhibits exceptional electrocatalytic activity and electrochemical stability. A solar cell fabricates with the Fe/Co‐NPCD yields an impressive power conversion efficiency of 8.35% in dye‐sensitized solar cells, superior to that of mono‐metal‐doped carbon‐based cells and conventional Pt‐based cells. Furthermore, density functional theory calculations illustrate that Fe, Co, and N doping are in favor of improving the adsorption capacity of the catalyst for I 3 − species by optimizing the magnetic momentum between the magnetic metal atoms, thereby upgrading its catalytic activity. This work develops a general strategy for synthesizing a high‐performance defect‐rich carbon‐based catalyst, and offers valuable insight into the role of magnetic metals in catalysis, which can be used to guide the design of high‐performance catalysts in the energy field.