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Enhanced mineralization of oxalate by heterogeneous peroxone: The interfacial reaction on the core-shell CeOx@SiO2

Journal 2019 · IF 8.355 · 发表于 2019 年 7 月 30 日
作者: Jinxin Xie,Xukai Li,Weirui Chen,Xianglin Sun,Kexin Chen,Yiming Tang,Laisheng Li
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摘要

The mesoporous core-shell CeO x @SiO 2 was synthesized and characterized by XRD, pyridine-FTIR, BET, SEM, TEM and XPS. CeO x @SiO 2 was the hollow nanosphere with high surface area of 1291.4 m 2  g −1 , which benefited for mass transfer of reactants. CeO x @SiO 2 exhibited the excellent catalytic activity for oxidizing oxalic acid (OA) in O 3 /H 2 O 2 /CeO x @SiO 2 . The greatest OA mineralization (91.2%) was achieved at pH = 3.2 in O 3 /H 2 O 2 /CeO x @SiO 2 , which was 5.5 times higher than that in peroxone (O 3 /H 2 O 2 , 15.9%). Influence of pH, HSO 3 − , PO 4 3− and detection of ozone and H 2 O 2 concentration were conducted to explore the mechanism. The interface reaction played vital role for OA removal in O 3 /H 2 O 2 /CeO x @SiO 2 process. Protonated surface hydroxyl groups (Ce-OH 2 + ) was the active sites, where OA, O 3 and H 2 O 2 were chemi-absorbed. The peroxide-like species (≡(Ce(IV)-O 2 H 2 )) formed by the complex of H 2 O 2 with active sites were the important intermediates, which initiated ozone decomposition into hydroxyl radical (·OH) and led to the high OA mineralization. Moreover, Lewis acid sites and electron transfer effect of Ce(III)/Ce(IV) also accounted for the high catalytic activity of CeO x @SiO 2 . In addition, CeO x @SiO 2 maintained stable structure and catalytic activity in three cycles.