Tailored d-Band Facilitating in Fe Gradient Doping CuO Boosts Peroxymonosulfate Activation for High Efficiency Generation and Release of Singlet Oxygen.
ACS Appl Mater Interfaces
; 13(42): 49982-49992, 2021 Oct 27.
Article
in En
| MEDLINE
| ID: mdl-34636557
ABSTRACT
In the field of heterogeneous catalysis, limitations of the surface reaction process inevitably make improving the catalytic efficiency to remove pollutants in water a major challenge. Here, we report a unique structure of Fe surface-gradient-doped CuO that improves the overall catalytic processes of adsorption, electron transfer, and desorption. Interestingly, gradient doping leads to an imbalanced charge distribution in the crystal structure, thereby promoting the adsorption and electron transport efficiency of peroxymonosulfate (PMS). The orbital hybridization of Fe also improves the electronic activity. More importantly, the occupied d-orbital distribution is closer to the lower energy level, which improves the desorption of the reaction intermediate (1O2). As a result, the production and desorption of 1O2 have been improved, resulting in excellent BPA degradation ability (kinetic rate increased by 67.3 times). Two-dimensional infrared correlation spectroscopy is used to better understand the doping process and catalytic mechanism of Fe-CuO. Fe-O changes before Cu-O and is more active. The Fe-required active sites, active species intensity, and kinetic reaction rates show a good correlation. This research provides a scientific basis for expanding the purification of toxic organic pollutants in complex water environments by heterogeneous catalytic oxidation.
Full text:
1
Collection:
01-internacional
Database:
MEDLINE
Language:
En
Journal:
ACS Appl Mater Interfaces
Year:
2021
Document type:
Article