期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 276, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119016
关键词
Fenton-like reaction; Hydroxyl radicals; MIL-88B(Fe)-X; Substituent; Electrophilicity
资金
- National Natural Science Foundation of China [21590813]
- Programme of Introducing Talents of Discipline to Universities [B13012]
- Programme for Changjiang Scholars and Innovative Research Team in University [IRT_13R05]
Heterogeneous Fenton-like reaction was a promising approach for generating center dot OH. However, the heterogeneous catalysts generally exhibited low activity because of slow reduction of Fe(III) in Fe(III)/Fe(II) redox cycle. Here, decreasing electron density was expected to quicken Fe(III) reduction and consequently enhance the catalytic activity of heterogeneous catalysts. This hypothesis was validated by the enhanced hydroxyl radicals generation and accelerated Fe(III) reduction on MIL-88B(Fe)-X (2-X-terephthalic acid, X= NH2, CH3, H, Br and NO2) by reducing electron density of Fe(III) with substituent of higher electrophilicity. MIL-88B(Fe)-NO2, with the substituent of highest electrophilicity among these catalysts, has the lowest electron density of Fe(III) and highest redox potential (E-Fe(III)/Fe(II)= 0.35 V). As a result, it exhibited the best catalytic performance, which was 1.7-20 times higher than that for other MIL-88B(Fe)-X and was comparable to that of homogeneous Fe2+. This study provides scientific basis for rational construction of highly effective heterogeneous Fenton-like catalyst.
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