Oxygen vacancies-mediated CuO@N-doped carbon nanocomposites for non-radical-dominated photothermal catalytic degradation of contaminants

纳米复合材料 催化作用 氧气 光热治疗 碳纤维 化学工程 单线态氧 材料科学 吸附 化学 光化学 纳米技术 有机化学 复合材料 复合数 工程类
作者
Yi Chen,Yao Dai,Yanwei Li,Zexi Hou,Baoyu Gao,Qinyan Yue,Qian Li
出处
期刊:Journal of Cleaner Production [Elsevier BV]
卷期号:389: 136054-136054 被引量:5
标识
DOI:10.1016/j.jclepro.2023.136054
摘要

Efficient molecular oxygen activation (MOA) is a critical step for most of the environmental catalysis applications for generating reactive oxygen species (ROS), which is often limited by the lack of energy to excite electrons. The emergence of photothermal catalyst provides an opportunity to make effective use of solar energy to energize electrons for boosting activation of molecular oxygen. Herein, CuO nanoparticles wrapped into nitrogen-doped carbon nanocomposites ([email protected]) with abundant oxygen vacancies (OVs) were prepared through a facile one-step synthesis using carboxymethyl chitosan hydrogel as a template. The as-obtained [email protected] exhibited excellent photothermal catalytic properties under visible-light irradiation to achieve efficient molecular oxygen activation, thus allowing the effective degradation of bisphenol F (BPF) in complex aqueous environments and actual water matrices. Density functional theory (DFT) calculations reveal that both the enhanced properties of OVs for molecular oxygen adsorption and the accelerated properties of graphitic N for electron transfer contribute significantly to the MOA and charge separation efficiency, resulting in a large amount of ROS. Molecular oxygen is converted to superoxide (·O2−) and ultimately to singlet oxygen (1O2), which is the dominant ROS responsible for contaminants degradation. Additionally, a photothermal catalytic degradation pathway of BPF was proposed based on the product detection and theoretical calculations. This study provides an effective method for the in-situ fabrication of [email protected] carbon nanocomposite photothermal catalysts and elucidates the mechanism of the photothermal catalytic activation of molecular oxygen for contaminants degradation, providing a promising approach for making effective use of solar energy for environmental remediation.
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