Tailored
d‑Band Facilitating in Fe Gradient
Doping CuO Boosts Peroxymonosulfate Activation for High Efficiency
Generation and Release of Singlet Oxygen
posted on 2021-10-12, 15:38authored byShiyu Zuo, Dongya Li, Zeyu Guan, Fan Yang, Haiming Xu, Dongsheng Xia, Jinquan Wan
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.