Revisiting the Graphitized Nanodiamond-Mediated Activation of Peroxymonosulfate: Singlet Oxygenation versus Electron Transfer,Environmental Science & Technology

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Revisiting the Graphitized Nanodiamond-Mediated Activation of Peroxymonosulfate: Singlet Oxygenation versus Electron Transfer
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2021-10-11 , DOI: 10.1021/acs.est.1c02042
Penghui Shao ₁ , Yunpeng Jing ₁ , Xiaoguang Duan ₂ , Huiyun Lin ₃ , Liming Yang ₁ , Wei Ren ₁ , Fang Deng ₁ , Buhong Li ₃ , Xubiao Luo ₁ , Shaobin Wang ₂

Affiliation

Graphitized nanodiamonds (ND) exhibit outstanding capability in activating peroxymonosulfate (PMS) for the removal of aqueous organic micropollutants (OMPs). However, controversial observation and interpretation regarding the effect of graphitization degree on ND’s activity and the role of singlet oxygen (¹O₂) in OMP degradation need to be clarified. Herein, we investigated graphitized ND-mediated PMS activation. Experiments show that the activity of ND increases first and then decreases with the monotonically increased graphitization degree. Further experimental and theoretical studies unveil that the intensified surface graphitization alters the degradation mechanism from singlet oxygenation to an electron-transfer pathway. Moreover, for the first time, we applied a self-constructed, time-resolved phosphorescence detection system to provide direct evidence for ¹O₂ production in the PMS-based system. This work not only elucidates the graphitization degree-dependent activation mechanism of PMS but also provides a reliable detection system for in situ analysis of ¹O₂ in future studies.

中文翻译：

重新审视石墨化纳米金刚石介导的过氧单硫酸盐活化：单线态氧化与电子转移

石墨化纳米金刚石 (ND) 在活化过硫酸盐 (PMS) 以去除水性有机微污染物 (OMP) 方面表现出出色的能力。然而，关于石墨化程度对ND活性的影响和单线态氧( ¹ O ₂) 在 OMP 降解中需要澄清。在此，我们研究了石墨化 ND 介导的 PMS 激活。实验表明，随着石墨化程度的单调增加，ND的活性先增加后降低。进一步的实验和理论研究表明，强化的表面石墨化改变了从单线态氧化到电子转移途径的降解机制。此外，我们首次应用自建的时间分辨磷光检测系统为基于 PMS 的系统中¹ O _{2 的}产生提供直接证据。这项工作不仅阐明了 PMS 的石墨化程度依赖性激活机制，而且为^{1 的}原位分析提供了可靠的检测系统。O ₂在未来的研究中。

更新日期：2021-12-07

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