Spin-Regulated Fenton-Like Catalysis for Nonradical Oxidation over Metal Oxide@Carbon Composites
Date
2024
Authors
Li, B.
Liu, Y.
Hu, K.
Dai, Q.
Chen, C.
Duan, X.
Wang, S.
Wang, Y.
Editors
Advisors
Journal Title
Journal ISSN
Volume Title
Type:
Journal article
Citation
Advanced Functional Materials, 2024; 34(36):2401397-1-2401397-12
Statement of Responsibility
Bofeng Li, Ya Liu, Kunsheng Hu, Qin Dai, Chunmao Chen, Xiaoguang Duan, Shaobin Wang, and Yuxian Wang
Conference Name
Abstract
The 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.
School/Discipline
Dissertation Note
Provenance
Description
Published online: April 24, 2024
Access Status
Rights
© 2024 Wiley-VCH GmbH