Efficient peroxymonosulfate nonradical activity of Zn-Mn-Al2O3@g-C3N4 via synergism of Zn, Mn doping and g-C3N4 composite

Electronic structural engineering is critical to high-performance catalysis. However, it is difficult to achieve the best state with a single method to control the electronic structure. In this, Zn, Mn orbital hybridization, and polarization built-in electric field (heterostructure of g-C3N4 composite ZnMn-Al2O3) was used to control the electronic structure of Al2O3 to catalyze peroxymonosulfate to deal with environmental pollution. The obtained Zn-Mn-Al2O3@g-C3N4 (ZnMnAlO-CN) exhibits an intrinsic activity 71.1 times higher than that of Al2O3. Experiments and theoretical calculations have determined that the hybridization of Zn and Mn orbitals generates new orbitals that cross the Fermi level, and the polarization built-in electric field (polarization electric field) promotes the charge polarity on ZnMnAlO-CN. Orbital hybridization regulation and polarized electric field can coordinately adjust the electronic structure, thereby synergizing the non-radical reaction of surface reactive complexes and 1O2. The optimized catalytic mechanism shows good adaptability to pH, anions, and actual water bodies (tap water, surface water, and groundwater). It can stably remove environmental pollutants in continuous flow reaction. The coordinated use of multiple control methods is expected to provide ideas for releasing the inherent activity of the catalyst.

Automated summary

This study investigates the use of Zn, Mn orbital hybridization, and polarization built-in electric field to control the electronic structure for enhancing catalytic performance. Experimental and theoretical findings suggest that these methods can coordinately adjust the electronic structure, promote non-radical reactions, and effectively remove pollutants in various water environments.