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碳掺杂氮化硼非自由基活化低添加量高碘酸盐降解对乙酰氨基酚:高电位亚稳中间体的意义

Non-radical activation of low additive periodate by carbon-doped boron nitride for acetaminophen degradation: Significance of high-potential metastable intermediates.

作者信息

Jiang Longbo, Li Wenqin, Wang Hui, Yang Jinjuan, Chen Haoyun, Wang Xinyu, Yuan Xingzhong, Wang Hou

机构信息

College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.

College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha 410082, PR China.

出版信息

J Hazard Mater. 2024 May 5;469:133806. doi: 10.1016/j.jhazmat.2024.133806. Epub 2024 Feb 15.

DOI:10.1016/j.jhazmat.2024.133806
PMID:38430599
Abstract

Metal-free environmental-friendly and cost-effective catalysts for periodate (PI) activation are crucial to popularize their application for micropollutant removal in water. Herein, we report that carbon-doped boron nitride (C-BN) can efficiently activate PI to degrade acetaminophen under very low oxidant doses (40 μM) and over a relatively wide pH range (3-9). As expected, the significant reduction in periodate addition is likely to be due to the higher chemical utilization efficiency achieved by a non-radical oxidation pathway. This involved two main mechanisms, the electron transfer process mediated by the high-potential metastable C-BN-900-PI* complex and singlet oxygen. In this case, the CO groups and defects on the C-BN surface were identified as key active sites for PI activation. Notably, the prepared C-BN-900 had good cycling performance and the degradation efficiency is recovered after simple annealing. The existence of HCO and HA significantly inhibited the reaction, whereas Cl, SO, and NO had little effect on the degradation of ACE. Overall, this study provides a new alternative method to regulate the non-radical pathway of boron nitride/periodate system.

摘要

用于活化高碘酸盐(PI)的无金属、环境友好且具有成本效益的催化剂对于推广其在水中去除微污染物的应用至关重要。在此,我们报道碳掺杂氮化硼(C-BN)能够在非常低的氧化剂剂量(40 μM)和相对较宽的pH范围(3-9)内有效活化PI以降解对乙酰氨基酚。正如预期的那样,高碘酸盐添加量的显著减少可能是由于通过非自由基氧化途径实现了更高的化学利用效率。这涉及两个主要机制,即由高电位亚稳C-BN-900-PI*复合物介导的电子转移过程和单线态氧。在这种情况下,C-BN表面的羰基和缺陷被确定为PI活化的关键活性位点。值得注意的是,制备的C-BN-900具有良好的循环性能,并且在简单退火后降解效率得以恢复。HCO和HA的存在显著抑制了反应,而Cl、SO和NO对ACE的降解影响很小。总体而言,本研究提供了一种调节氮化硼/高碘酸盐体系非自由基途径的新替代方法。

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