Bao Yan, Lian Cheng, Huang Kai, Yu Haoran, Liu Wenyuan, Zhang Jinlong, Xing Mingyang
Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
Shanghai Engineering Research Center for Multimedia Environmental Catalysis and Resource Utilization, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
Angew Chem Int Ed Engl. 2022 Oct 17;61(42):e202209542. doi: 10.1002/anie.202209542. Epub 2022 Aug 17.
The universal limit on the pH conditions is disturbing peroxymonosulfate (PMS)-triggered high-valent iron-oxo systems in environmental applications. Here, we propose for the first time the construction of a neutral microenvironment on the surface of Zn-Fe layered double hydroxide (ZnFe-LDH) by using the amphoteric properties of zinc hydroxide, which continuously generates ≡Fe =O over a wide pH range of 3.0-11.0 in activating PMS. The ≡Zn(OH) moiety offers a neutral microenvironment at the phase interface, which mitigates the self-decomposition of ≡Fe =O by protons and the hydrolysis reaction of iron by hydroxyl groups, which is supported by the Mossbauer spectra, density functional theory calculations and designed experiments. Consequently, ZnFe-LDH/PMS can satisfy the stability in long-term experiments, selectivity under conditions with high salinity or natural organic matter and efficient treatment of actual wastewater.
在环境应用中，pH条件的普遍限制困扰着过一硫酸盐（PMS）引发的高价铁氧体系。在此，我们首次提出利用氢氧化锌的两性性质在锌铁层状双氢氧化物（ZnFe-LDH）表面构建中性微环境，其在3.0至11.0的宽pH范围内活化PMS时持续生成≡Fe =O。≡Zn(OH)部分在相界面提供中性微环境，减轻了质子对≡Fe =O的自分解以及羟基对铁的水解反应，这得到了穆斯堡尔光谱、密度泛函理论计算和设计实验的支持。因此，ZnFe-LDH/PMS在长期实验中能满足稳定性，在高盐度或天然有机物条件下具有选择性，并能有效处理实际废水。
