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Unique electron reservoir properties of manganese in Mn(II)-doped CeO2 for reversible electron transfer and enhanced Fenton-like catalytic performance

Journal 2019 · IF 5.155 · 发表于 2019 年 10 月 16 日
作者: Haitao Li,Qiang Gao,Guanshuai Wang,Bo Han,Kaisheng Xia,Chenghang Zhou
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摘要

Developing high-performance heterogeneous Fenton-like catalyst and understanding its intrinsic catalytic properties are of fundamental and practical significance. In this work, a mesoporous Mn(II)-doped CeO 2 (MCO) with monodisperse spherical morphology and large surface area (141.8 m 2  g −1 ) was fabricated through a simple hydrothermal–calcination process, and further utilized as the heterogeneous catalyst for oxidative degradation of organic pollutants in the presence of H 2 O 2 . The density functional theory (DFT) simulations were carried out to study the H 2 O 2 decomposition process on the MCO surface. It was revealed that the Mn(II) doping in the CeO 2 could significantly promote the complex of the surface Ce sites and H 2 O 2 molecules. More importantly, the manganese dopants could serve as electron reservoirs, capable of reversibly donating and accepting electrons, which facilitated the electron transfer between Ce and H 2 O 2 . Owing to the electron reservoir properties of manganese, this MCO showed significantly enhanced catalytic efficiency in comparison to pure CeO 2 . Moreover, the catalytic activity of MCO almost kept unchanged after reuse several times, demonstrating its long-circulating characteristics. This study provides new and important insights into the electron transfer pathway involved in the heterogeneous Fenton-like process.

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