FeN4-doped carbon nanotubes derived from metal organic frameworks for effective degradation of organic dyes by peroxymonosulfate: Impacts of FeN4 spin states
FeN4-doped carbon nanotubes derived from metal organic frameworks for effective degradation of organic dyes by peroxymonosulfate: Impacts of FeN4 spin states
复制标题
DOI：
10.1016/j.cej.2021.133339
复制
发表时间：
2022-01-06
影响因子：
15.1
通讯作者：
Chen, Shaowei
中科院分区：
文献类型：
--
作者：
Li, Meng;Li, Zilong;Chen, Shaowei
开发低成本、高性能的有机染料高效降解催化剂对环境治理具有重要的基础和技术意义。在此，FeN 4掺杂的碳纳米管对过一硫酸盐（PMS）存在下的酸性橙子7（AO 7）的降解表现出显著的催化活性。这是由丰富的分散良好的FeN 4网站和适当的吸附能占。自由基猝灭实验和电子顺磁共振测量表明，单线态氧是主要的活性氧物种。Fe-57穆斯堡尔谱测量表明，FeN 4部分包含多个自旋态，并结合密度泛函理论计算，确认具有低/中自旋态的FeN 4作为PMS激活的关键位点，因此AO 7降解。从这项研究的结果突出了自旋状态在FeN 4中的单线态氧的有效降解有机污染物的产生中的关键作用。
Development of low-cost, high-performance catalysts for the effective degradation of organic dyes is of both fundamental and technological significance for environmental remediation. Herein, FeN4-doped carbon nano tubes exhibit a remarkable catalytic activity towards the degradation of acid orange 7 (AO7) in the presence of peroxymonosulfate (PMS). This is accounted for by the abundant well-dispersed FeN4 sites and appropriate adsorption energy. Radical quenching experiments and electron paramagnetic resonance measurements suggest that singlet oxygen is the main reactive oxygen species. Fe-57 Mossbauer spectroscopy measurements show that the FeN4 moieties contain multiple spin states, and in conjunction with density functional theory calculations, confirm that FeN4 with a low/medium spin state serves as the key sites for PMS activation and hence AO7 degradation. Results from this study highlight the critical role of spin states in FeN4 in the generation of singlet oxygen for effective degradation of organic pollutants.