Ge Xiao, Xie Donghua, Cheng Rui-Fen, Chen Wenxing, Chen Cai, Zhou Fangyao, Wang Xiaozhi, Chen Jie-Jie, Sheng Guo-Ping, Wu Yuen
The First Affiliated Hospital of USTC, Division of Life Sciences and Medicine, University of Science and Technology of China, Hefei 230026, China.
School of Environmental Science and Engineering, Yangzhou University, Yangzhou 225000, China.
Precis Chem. 2023 Feb 16;1(3):153-160. doi: 10.1021/prechem.2c00006. eCollection 2023 May 22.
Reactive oxygen species (ROS) have a significant part in the elimination of recalcitrant organic pollutants and commonly coexist in one advanced oxidation system. It is difficult for us to make clear the effect of the co-instantaneous generation of radicals and nonradicals, which would cover and obscure the transformation pathway. Herein, a coordinate welding process is presented for fabricating accessible Mn site catalysts (Mn SSCs) in order to clarify the nonradical (singlet oxygen/O) generated pathway and transformation in oxidative removal of contaminants. The Mn SSCs achieve nearly 100% O fabrication by activating peroxymonosulfate, which displays an excellent sulfamethoxazole elimination performance, super anti-anion interference, and extraordinary stability. As revealed by density functional theory calculations, the Mn SSCs with a special welded three-dimensional nanostructure could significantly boost the activation process by oxidizing the peroxymonosulfate at the interlayer of Mn SSCs and reducing dissolved oxygen on the surface of Mn SSCs. This design of Mn SSCs with a three-dimensional welded nanostructure might offer a potential approach for employing single site catalysts for environmental remediation.
活性氧(ROS)在难降解有机污染物的去除中起着重要作用,且通常共存于一个高级氧化体系中。我们很难弄清楚自由基和非自由基同时产生的影响,这会掩盖和模糊转化途径。在此,提出了一种配位焊接工艺来制备可及锰位点催化剂(Mn SSCs),以阐明非自由基(单线态氧/O)在污染物氧化去除中的产生途径和转化过程。Mn SSCs通过活化过一硫酸盐实现了近100%的O生成,表现出优异的磺胺甲恶唑去除性能、超强的抗阴离子干扰能力和非凡的稳定性。密度泛函理论计算表明,具有特殊焊接三维纳米结构的Mn SSCs可以通过氧化Mn SSCs层间的过一硫酸盐和还原Mn SSCs表面的溶解氧来显著促进活化过程。这种具有三维焊接纳米结构的Mn SSCs设计可能为采用单位点催化剂进行环境修复提供一种潜在方法。