Researchers at Sun Yat-Sen University synthesized a high-entropy spinel catalyst that achieves 99% removal of methyl mercaptan, according to a study published in Nature Communications on August 15, 2026. The material, formulated as (CuNiMnCo)Fe2O4, substantially outperformed conventional CoFe2O4, which removed 51% of the pollutant under catalytic ozonation.
Conventional catalytic ozonation of electron-rich sulfur pollutants faces efficiency limits caused by the nonselective oxidation of hydroxyl radicals (•OH) and the deactivation of active metal sites by sulfate accumulation. To resolve these issues, the researchers applied high-entropy doping to induce lattice distortion and local coordination disorder. Spectroscopic analyses and density functional theory calculations revealed that this structure strengthens A–O–B covalency and inter-site electronic communication.
Electronic reconstruction
The structural changes drive a sublattice-resolved electronic reconstruction that enriches cobalt and manganese sites while depleting iron, copper, and nickel sites. This electronic differentiation enables cooperative dual-end activation of ozone on Fe–Co and Fe–Mn motifs, alongside preferential methyl mercaptan adsorption on copper and nickel sites. Orbital modulation of cobalt t2g and iron eg states near the Fermi level balances interfacial charge transfer, promoting the formation of surface-bound *O3 species instead of standard oxygen-oxygen bond cleavage.
Spatially separating the activation and oxidation sites allows methyl mercaptan mineralization via an electron transfer process. This pathway suppresses hydroxyl radical generation and minimizes sulfate accumulation, maintaining catalyst durability under humid conditions.
The paper was authored by Shulin Zuo, Muke Lin, Guizhi Xu, Jiahao Huang, Rumeng Zhang, Ji Mei, Jingyun Fang, and Dehua Xia from the Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology. The work was funded by the National Natural Science Foundation of China and the Guangdong Basic and Applied Basic Research Foundation, with material characterization support from the Analytical and Testing Center of Sun Yat-sen University.
