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Phosphorus Regulates Coordination Number and Electronegativity of Cobalt Atomic Sites Triggering Efficient
Yuqi Zhao1,2, Xi Wu2, Hengliang Wang3
1School of Materials Science and Engineering, Shandong University of Science and Technology, Qingdao 266590, China.
Abstract:
Optimizing the local electronic structure of a single-atom catalyst (SAC) is crucial for efficient photocatalytic hydrogen evolution reactions. This study synthesized a Co-P4/g-C3N4 heterostructure by selective phosphidation of the Co metal-organic framework/graphitic carbon nitride (Co-MOF/g-C3N4), converting the Co-O6 configuration into a highly electronegative, coordinatively unsaturated Co-P4 configuration anchored to a carbon matrix. P-doping induces strong charge redistribution, shifting the d-band center toward the Fermi level, transforming the Co sites from an electron-deficient state to an electron-rich state, and resulting in a significant reduction in the free energy barrier for HER to -0.08 eV. The Co-P4/g-C3N4 heterostructure demonstrated a HER rate of 13.51 mmol g-1 h-1, approximately 4.82-8.35 times greater than those of photocatalysts loaded with noble metals. The apparent quantum efficiency (AQE) was 28.45% at 380 nm. The synergistic effect of the low coordination number and high electronegativity metal sites significantly enhances the photocatalytic HER performance.
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