Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2021-01-28 , DOI: 10.1016/j.apcatb.2021.119943 Yue Yin , Yi Ren , Junhe Lu , Weiming Zhang , Chao Shan , Ming Hua , Lu Lv , Bingcai Pan
Fe3O4 nanoparticles supported on zirconium-based metal-organic frameworks, UiO-66, were firstly used as a tool for exploring the interaction between dual active centers in Fenton-like reactions. Compared with traditional H2O2/Fe3O4 system, nearly 3 times hydroxyl radicals (HO•) were found in the H2O2/Fe3O4@UiO-66 system at pH 5. Additionally, singlet oxygen (1O2) was also detected in the H2O2/Fe3O4@UiO-66 system. X-ray photoelectron and Mössbauer spectroscopy analyses indicate that the electrons on ≡Fe(II) were directed towards Zr, causing ≡Fe(II) to lose electrons more easily, which facilitates H2O2 reduction. However, 1O2 was formed when superoxide anions (O2•−) lost electrons on the Zr center; these electrons can be transferred to ≡Fe(III), accelerating ≡Fe(III) reduction. These findings reveal that Zr centers can interact with Fe to form dual active centers in Fenton-like reactions. And it also provides a novel strategy to optimize dual active center catalysts for Fenton-like processes in water remediation.
中文翻译:
UiO-66负载的Fe 3 O 4纳米颗粒的性质和催化反应性为Fenton样反应中的Fe-Zr双活性中心提供了新见解
锆基金属有机骨架UiO-66上负载的Fe 3 O 4纳米颗粒首先被用作探索类Fenton反应中双活性中心之间相互作用的工具。与传统的H 2 O 2 / Fe 3 O 4体系相比,在pH 5的H 2 O 2 / Fe 3 O 4 @ UiO-66体系中发现了近3倍的羟基自由基(HO •)。在H 2 O 2 / Fe 3 O 4中也检测到1 O 2)@ UiO-66系统。X射线光电子和Mössbauer光谱分析表明,≡Fe(II)上的电子被导向Zr,导致≡Fe(II)更容易失去电子,从而促进了H 2 O 2的还原。但是,当超氧阴离子(O 2 •-)在Zr中心失去电子时,会形成1 O 2。这些电子可以转移到≡Fe(III),加速≡Fe(III)的还原。这些发现表明Zr中心可以与Fe相互作用,从而在Fenton样反应中形成双重活性中心。它还提供了一种新颖的策略来优化水修复中类似Fenton的工艺的双重活性中心催化剂。