Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume -, Issue -, Pages -Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.2c03769
Keywords
O2 activation; photocatalysis; excitonic effects; NO oxidation; surface boronizing
Categories
Funding
- National Natural Science Foundation of China
- China Postdoctoral Science Foundation
- [21936003]
- [21872061]
- [U20A20129]
- [2022M712049]
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This study demonstrates the weakened excitonic effect of BiOBr nanosheets by surface boronizing, leading to the efficient oxidation of nitrogen oxides (NOx) and providing a facile method for managing reactive oxygen species (ROS) generation in pollutant removal.
The photocatalytic O2 activation for pollutant removal highly depends on the controlled generation of desired reactive oxygen species (ROS). Herein, we demonstrate that the robust excitonic effect of BiOBr nanosheets, which is prototypical for singlet oxygen (1O2) production to partially oxidize NO into a more toxic intermediate NO2, can be weakened by surface boronizing via inducing a staggered band alignment from the surface to the bulk and simultaneously generating more surface oxygen vacancy (VO). The staggered band alignment destabilizes excitons and facilitates their dissociation into charge carriers, while surface VO traps electrons and efficiently activates O2 into a superoxide radical (center dot O2-) via a one-electron-transfer pathway. Different from 1O2, center dot O2 -enables the complete oxidation of NO into nitrate with high selectivity that is more desirable for safe indoor NO remediation under visible light irradiation. This study provides a facile excitonic effect manipulating method for layered two-dimensional photocatalysts and sheds light on the importance of managing ROS production for efficient pollutant removal.
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