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2D MOF derived cobalt and nitrogen-doped ultrathin oxygen-rich carbon nanosheets for efficient Fenton-like catalysis: Tuning effect of oxygen functional groups in close vicinity to Co-N sites
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2022-11-12 , DOI: 10.1016/j.jhazmat.2022.130345
Heng Shi 1 , Yi He 2 , Yubin Li 3 , Pingya Luo 1
Affiliation  

Developing highly efficient catalysts for peroxymonosulfate (PMS) activation is an important issue in advanced oxidation processes (AOPs) technology. In this work, cobalt and nitrogen-doped ultrathin oxygen-rich carbon nanosheets derived from 2D metal-organic framework (MOF) were successfully fabricated. The as-prepared catalyst can effectively degrade tetracycline (TC) with a high reaction constant (0.088 min−1). Quenching test, electron paramagnetic resonance (EPR) technology, and the electrochemical test indicate that the radical pathway plays a minor role in the degradation process, the 1O2 based nonradical pathway dominates the reaction. Experimental and density functional theory (DFT) studies revealed that the Co-N sites on the carbon structure serve as the dominant active sites, and the oxygen functional groups in close vicinity to Co-N sites can dramatically influence local electronic structure and its interaction with PMS molecule, a high correlation between the reaction constant and hydroxy groups content could be due to the Co-N sites close to hydroxyl groups has a moderate PMS adsorption energy. This work provides new insight into the design of highly efficient Fenton-like catalysts.



中文翻译:

用于高效类芬顿催化的二维 MOF 衍生钴和氮掺杂超薄富氧碳纳米片:靠近 Co-N 位点的氧官能团的调节作用

开发用于过一硫酸盐 (PMS) 活化的高效催化剂是高级氧化工艺 (AOP) 技术中的一个重要问题。在这项工作中,成功地制备了源自二维金属有机骨架 (MOF) 的钴和氮掺杂超薄富氧碳纳米片。所制备的催化剂可以有效地降解四环素 (TC),具有高反应常数(0.088 min -1)。淬灭试验、电子顺磁共振(EPR)技术和电化学试验表明,自由基途径在降解过程中起次要作用,1 O 2基于非自由基途径主导反应。实验和密度泛函理论 (DFT) 研究表明,碳结构上的 Co-N 位点是主要的活性位点,靠近 Co-N 位点的氧官能团可以显着影响局部电子结构及其与PMS分子,反应常数与羟基含量之间的高度相关性可能是由于靠近羟基的Co-N位点具有适度的PMS吸附能。这项工作为高效类芬顿催化剂的设计提供了新的见解。

更新日期:2022-11-15
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