Hu Shiyu, Guo Rujia, Gao Yiqian, Chen Feng
Key Laboratory for Advanced Materials and Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, 200237, Shanghai, P. R. China.
Chem Asian J. 2023 Jan 17;18(2):e202201134. doi: 10.1002/asia.202201134. Epub 2022 Dec 16.
Oxoiron(IV) species are a critical intermediate in the Fe-based Fenton-like process at circumneutral pH, and its oxidative reactivity is closely related to the ligands. An optional inorganic host material, MoS , is selected to construct a highly reactive sulfur ligand coordinated Fe species in this work. The Fe species doped in MoS is presented as the Fe centre and triggers the transformation of the 2H phase to the octahedral 1T phase MoS . The role of the interaction between doped Fe and the MoS host lattice on the formation of oxoiron(IV) is studied. A significant Fenton-like reactivity and a remarkable accumulation of oxoiron(IV) species were observed for Fe-MoS . The quenching experiment was implemented to disclose the predominant role of oxoiron(IV) species in the Fe-MoS /H O Fenton-like system. Furthermore, oxoiron(IV) species could transform into the ⋅O and O , which further expedites the Fenton-like reaction.
氧代铁（IV）物种是铁基类芬顿过程在近中性pH值下的关键中间体，其氧化反应活性与配体密切相关。在本工作中，选择一种可选的无机主体材料二硫化钼（MoS₂）来构建具有高反应活性的硫配体配位铁物种。掺杂在二硫化钼中的铁物种以铁中心的形式存在，并引发二硫化钼从2H相转变为八面体1T相。研究了掺杂铁与二硫化钼主体晶格之间的相互作用对氧代铁（IV）形成的作用。对于铁-二硫化钼（Fe-MoS₂），观察到显著的类芬顿反应活性和氧代铁（IV）物种的显著积累。进行了猝灭实验以揭示氧代铁（IV）物种在铁-二硫化钼/过氧化氢（Fe-MoS₂/H₂O₂）类芬顿体系中的主要作用。此外，氧代铁（IV）物种可以转化为超氧阴离子自由基（⋅O₂⁻）和单线态氧（¹O₂），这进一步加速了类芬顿反应。
