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首页> 外文期刊>Applied Surface Science >Unique electron reservoir properties of manganese in Mn(Ⅱ)-doped CeO_2 for reversible electron transfer and enhanced Fenton-like catalytic performance
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Unique electron reservoir properties of manganese in Mn(Ⅱ)-doped CeO_2 for reversible electron transfer and enhanced Fenton-like catalytic performance

机译：锰在Mn（Ⅱ）掺杂的CeO_2中的独特电子储库性质可逆电子转移和增强的Fenton类催化性能

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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 CeO2 (MCO) with monodisperse spherical morphology and large surface area (141.8m(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 H2O2. The density functional theory (DFT) simulations were carried out to study the H2O2 decomposition process on the MCO surface. It was revealed that the Mn(II) doping in the CeO2 could significantly promote the complex of the surface Ce sites and H2O2 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 H2O2. Owing to the electron reservoir properties of manganese, this MCO showed significantly enhanced catalytic efficiency in comparison to pure CeO2. 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.
机译：开发高性能的非均相类Fenton催化剂并了解其固有的催化性能具有根本和现实意义。在这项工作中，通过简单的水热煅烧工艺制备了具有单分散球形形态和大表面积（141.8m（2）g（-1））的介孔Mn（II）掺杂CeO2（MCO）。在H2O2存在下用于有机污染物氧化降解的非均相催化剂。进行了密度泛函理论（DFT）模拟，以研究MCO表面上H2O2的分解过程。揭示了CeO2中的Mn（II）掺杂可以显着促进表面Ce位点和H2O2分子的复合。更重要的是，锰掺杂剂可以用作电子储库，能够可逆地提供和接受电子，从而促进了Ce和H2O2之间的电子转移。由于锰的电子储库特性，与纯CeO2相比，该MCO的催化效率显着提高。此外，多次重复使用后，MCO的催化活性几乎保持不变，证明了其长循环特性。这项研究为异质Fenton样过程中涉及的电子转移途径提供了新的重要见解。

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