Li, B.Liu, Y.Hu, K.Dai, Q.Chen, C.Duan, X.Wang, S.Wang, Y.2024-10-232024-10-232024Advanced Functional Materials, 2024; 34(36):2401397-1-2401397-121616-301X1616-3028https://hdl.handle.net/2440/142930Published online: April 24, 2024The spin state of the transition metal species (TMs) has been recognized as a critical descriptor in Fenton-like catalysis. The raised spin state of dispersed TMs in carbon will enhance the redox processes with adsorbed peroxides and improve the oxidation performance. Nevertheless, establishing the spin-activity correlations for the encapsulated TM nanoparticles remains challenging because of the difficulties in fine-tuning the spin state of TM species and the insufficient understanding of orbital hybridization states upon interaction with peroxides. Here, the advantage of the fast-temperature heating/quenching of microwave thermal shock is taken to engineer the structure and spin state of encapsulated TMs within the N-doped graphitic carbons. The reduced TMs particle size and enhanced TMs-carbon coupling increase surface entropy and regulate eg electron filling of the high-spin TM-N coordination, endowing electrons with high mobility and facilitating peroxymonosulfate (PMS) adsorption. The strong interactions further uplift the PMS O 2p band position toward the Fermi level and thus elevate the oxidation potential of surface-activated PMS (PMS*) as the dominant nonradical species for pollutant degradation. The deciphered orbital hybridizations of engineered high-spin TM and PMS enlighten the smart design of spin-regulated nanocomposites for advanced water purification.en© 2024 Wiley-VCH GmbHCo₃O₄; microwave-assisted synthesis; nonradical oxidation; peroxymonosulfate; spin state controlJournal article10.1002/adfm.2024013972024-05-16692224Liu, Y. [0000-0001-6329-5414]Hu, K. [0000-0002-8598-6336]Duan, X. [0000-0001-9635-5807]Wang, S. [0000-0002-1751-9162]