科研之友
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摘要
Fenton-like reactions is attractive for environmental pollutant control, but there is an urgent need to improve the utilisation of hydroxyl radicals (center dot OH) in practical applications. Here, for the first time, FeOCl is encapsulated within a Metal Organic Framework (MOF) (Materials of Institut Lavoisier-101 (MIL-101(Fe))) as a yolk-shell reactor (FeOCl-MOF) by in situ growth. The interaction between FeOCl and the MOF not only increases the electron density of FeOCl, but also shifts down the d-band centre. The increase of electron density could promote the efficient conversion of H2O2 to center dot OH catalysed by FeOCl. And the shift of the d-band centre to the lower energy level facilitates the desorption of center dot OH. Experimental and theoretical calculations showed that the high catalytic performance was attributed to the unique yolk-shell structure that concentrates the catalytic and adsorption sites in a confinement space, as well as the improved electron density and d-band centre for efficient generation, rapid desorption and utilized nearby of center dot OH. Which is utilized nearby by the organic pollutants adsorbed by the surface MOF, thus greatly improving the effective conversion of H2O2 and the center dot OH utilisation (from 25.5% (Fe2+/H2O2) to 77.1% (FeOCl-MOF/H2O2)). In addition, a catalytic reactor was constructed to achieve continuous efficient treatment of organic pollutants. This work provides a Fenton-like microreactor for efficient generation, rapid desorption, and nearby utilization of center dot OH to improve future technologies for deep water purification in complex environments.
