Overlooked key role of Mo(VI) in Fe2(MoO4)3 for peroxymonosulfate activation with 1O2 dominated degradation pathway

被引:15
作者
Chang, Lian [1 ]
Xie, Xinyu [1 ]
Zhang, Xiaodan [2 ]
Chai, Hongxiang [1 ]
Huang, Yuming [2 ]
机构
[1] Chongqing Univ, Key Lab Ecoenvironm Three Gorges Reservoir Reg, Coll Environm & Ecol, Minist Educ, Chongqing 400045, Peoples R China
[2] Southwest Univ, Coll Chem & Chem Engn, Key Lab Ecoenvironm Three Gorges Reservoir Reg, Minist Educ, Chongqing 400715, Peoples R China
关键词
Mo(VI); Mo(VI) peroxo-complex; Fe2(MoO4)3; Peroxymonosulfate; HETEROGENEOUS ACTIVATION; ORGANIC CONTAMINANTS; ADVANCED OXIDATION; PERSULFATE; MECHANISM; REMOVAL; TRANSFORMATION; CARBOCATALYST; ANTIBIOTICS; PERFORMANCE;
D O I
10.1016/j.seppur.2023.124360
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
In this study, an eco-friendly Fe2(MoO4)3 was synthesized via template assistant methods for peroxymonosulfate activation to remove RodanminhB (RhB). X-ray photoelectron spectroscopy (XPS) and UV-vis results illustrated the high valence Mo(VI) was the active center to initiate the nonradical-dominated pathway. Electron para-magnetic resonance (EPR) with chemical quenching experiments confirmed the leading role of 1O2 in RhB degradation, which originated from the Mo(IV)/Mo(VI) redox cycle and Mo(VI) peroxo-complex MoO(O2)22-. Also, the improved Fe(II)/Fe(III) cycle produced radicals, like SO4 & BULL;and & BULL;OH, to assist the degradation process, and promoted Mo(VI) regeneration alongside. 10 mg/L RhB can be completely removed after adding 0.2 g/L Fe2(MoO4)3-4 and 0.1 g/L PMS within 30 min. The effects of PMS and catalyst dosages, initial pH, inorganic anions, and humic acid on RhB degradation were studied and analyzed. Due to the anti-interference of 1O2, Fe2(MoO4)3-4 could sustain its high reactivity from pH 3 to 11. It also contained its original crystal structure with a high degradation rate after five cycle runs. Multiple kinds of dyes and antibiotics were eliminated effi-ciently within 30 min. The intermediates involved in the reaction were examed by liquid chromatography-mass spectrometry (LC-MS) to propose the degradation pathway of RhB. This work shed light on the overlooked key role of high valence Mo(VI) during PMS activation, instead of traditional low valence Fe(II) or Mo(IV).
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页数:12
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