Almost 100 % Peroxymonosulfate Conversion to Singlet Oxygen on Single‐Atom CoN2+2 Sites,Angewandte Chemie International Edition

当前位置： X-MOL 学术 › Angew. Chem. Int. Ed. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Almost 100 % Peroxymonosulfate Conversion to Singlet Oxygen on Single‐Atom CoN2+2 Sites
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-11-21 , DOI: 10.1002/anie.202014472
Xueyue Mi ₁ , Pengfei Wang ₂ , Shizhe Xu ₁ , Lina Su ₁ , Hui Zhong ₁ , Haitao Wang ₁ , Yi Li ₃ , Sihui Zhan ₁

Affiliation

Single‐atom CoN₄ active sites have demonstrated excellent efficiency in peroxymonosulfate activation. However, the identification of CoN₄ active sites and the detailed singlet oxygen generation mechanism in peroxymonosulfate activation remains ambiguous. We demonstrate a strategy to regulate the generation of reactive oxygen species by atomically dispersed cobalt anchored on nitrogen‐doped carbon. As indicated by experiment and DFT calculations, CoN₂₊₂ was the active site and singlet oxygen was the predominant reactive oxygen species with a proportion of 98.89 %. Spontaneous dissociation of adsorbed peroxymonosulfate on the CoN₂₊₂ active sites was energetically unfavorable because of the weakly positive Co atoms and CoN₂₊₂ coordination, which directed PMS oxidation by a non‐radical pathway and with simultaneous singlet oxygen generation. The generated singlet oxygen degraded several organic pollutants with high efficiency across a broad pH range.

中文翻译：

在单原子CoN2 + 2位置上几乎100％的过氧一硫酸盐转化为单重态氧

单原子CoN ₄活性位点在过氧单硫酸盐活化中表现出出色的效率。但是，CoN ₄活性位点的识别以及过氧单硫酸盐活化中详细的单线态氧产生机理仍然不清楚。我们展示了一种通过锚固在掺氮碳上的原子分散的钴来调节活性氧物种生成的策略。如实验和DFT计算所示，CoN _{2 + 2}是活性位点，单线态氧是主要的活性氧种类，比例为98.89％。由于弱的正Co原子和CoN ，吸附的过氧单硫酸盐在CoN _{2 + 2}活性位点上的自发解离在能量上不利_{2 + 2}配位，通过非自由基途径引导PMS氧化并同时产生单线态氧。产生的单重态氧在很宽的pH范围内能高效降解几种有机污染物。

更新日期：2020-11-21

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南