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金属有机框架衍生的杂原子双掺杂多孔碳催化剂在过一硫酸盐活化中增强超氧自由基向单线态氧的转化

Enhanced conversion of superoxide radical to singlet oxygen in peroxymonosulfate activation by metal-organic frameworks derived heteroatoms dual-doped porous carbon catalyst.

作者信息

Xie Jinling, Pan Xiaofang, Jiang Chenming, Zhao Li, Gong Xiaobo, Liu Yong

机构信息

Key Laboratory of Land Resources Evaluation and Monitoring in Southwest, Ministry of Education, Sichuan Normal University, Chengdu, 610068, China.

Key Laboratory of Land Resources Evaluation and Monitoring in Southwest, Ministry of Education, Sichuan Normal University, Chengdu, 610068, China; College of Chemistry and Materials Science, Sichuan Normal University, Chengdu, Sichuan, 610068, China; Key Laboratory of Special Waste Water Treatment of Sichuan Province Higher Education System, Sichuan Normal University, Chengdu, Sichuan, 610068, China; Sichuan Environmental Protection Key Laboratory of Persistent Pollutant Wastewater Treatment, Chengdu, Sichuan, 610068, China.

出版信息

Environ Res. 2023 Nov 1;236(Pt 1):116745. doi: 10.1016/j.envres.2023.116745. Epub 2023 Jul 25.

DOI:10.1016/j.envres.2023.116745
PMID:37500040
Abstract

The activation of persulfate technology using carbon-based materials doped with heteroatoms has been extensively researched for the elimination of refractory pollutants in wastewater. In this study, metal-organic frameworks were utilized as precursors to synthesize P, N dual-doped carbon material (PNC), which was employed to activate peroxymonosulfate (PMS) for the degradation of tetracycline hydrochloride (TCH). The results demonstrated a 90.2% removal efficiency of total organic carbon within 60 min. The significant increase of surface defects on the nitrogen self-doped porous carbon materials anchored with phosphorus promoted the conversion of superoxide radical to singlet oxygen during PMS activation, which was identified as the key active species of PNC/PMS system. Additionally, the enhanced direct electron transfer also facilitated the degradation of TCH. Consequently, TCH was successfully degraded into nontoxic and harmless inorganic small molecules. The findings of this research provide valuable insights into improving the performance of heteroatom-doped carbon materials for pollutant degradation by activating PMS and transforming the non-radical pathway. The results highlight the potential of metal-organic frameworks derived heteroatoms dual-doped porous carbon catalysts for the development of advanced treatment technologies in wastewater treatment.

摘要

利用掺杂杂原子的碳基材料活化过硫酸盐技术已被广泛研究用于去除废水中的难降解污染物。在本研究中,金属有机框架被用作前驱体来合成P、N双掺杂碳材料(PNC),该材料用于活化过一硫酸盐(PMS)以降解盐酸四环素(TCH)。结果表明,在60分钟内总有机碳的去除效率达到90.2%。磷锚定的氮自掺杂多孔碳材料表面缺陷的显著增加促进了PMS活化过程中超氧自由基向单线态氧的转化,这被确定为PNC/PMS体系的关键活性物种。此外,增强的直接电子转移也促进了TCH的降解。因此,TCH成功降解为无毒无害的无机小分子。本研究结果为通过活化PMS和转变非自由基途径提高杂原子掺杂碳材料的污染物降解性能提供了有价值的见解。结果突出了金属有机框架衍生的杂原子双掺杂多孔碳催化剂在开发废水处理高级处理技术方面的潜力。

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