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Controllable redox-induced in-situ growth of MnO2 over Mn2O3 for toluene oxidation: Active heterostructure interfaces
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-06-26 , DOI: 10.1016/j.apcatb.2020.119279
Wenhao Yang , Yue Peng , Ya Wang , Yun Wang , Hao Liu , Zi’ang Su , Weinan Yang , Jianjun Chen , Wenzhe Si , Junhua Li

Mn-based heterostructure catalysts show great potential for catalytic oxidation of toluene owing to the unique properties of their hetero-interfaces. Herein, we tailored the MnO2 heteroepitaxy over Mn2O3 to achieve well-defined morphology and constructed clean MnO2-Mn2O3 heterostructure interfaces by H+/KMnO4 treatment. The T-0.5 catalyst (treating duration of 0.5 h) gave the highest activity and good stability. The interface enhanced the reducibility and oxygen storage capacity compared with pure Mn2O3. Surface reconstruction and metastable facets exposure were observed after the H+/KMnO4 treatment, leading to the easy-release of lattice oxygen. Additionally, abundant oxygen vacancies and redundant coordination lattice oxygen were observed at the MnO2 and Mn2O3 sides of the hetero-interface, respectively. These features provided ample oxygen adspecies and increased lattice oxygen mobility. The interface-related oxygen vacancies facilitated methyl dehydrogenation and demethylation of adsorbed toluene. The redundant coordination lattice oxygen contributed to the enhanced aromatic ring breakage capability.



中文翻译:

MnO 2在Mn 2 O 3上可控制的氧化还原诱导的MnO 2原位生长以进行甲苯氧化:活性异结构界面

锰基异质结构催化剂由于其异质界面的独特性质而具有很大的甲苯催化氧化潜力。本文中,我们在Mn 2 O 3上修整了MnO 2异质外延性,以实现明确的形态,并通过H + / KMnO 4处理构建了干净的MnO 2 -Mn 2 O 3异质结构界面。T-0.5催化剂(处理时间为0.5 h)具有最高的活性和良好的稳定性。与纯Mn 2 O 3相比,该界面增强了还原性和储氧能力。H + / KMnO 4处理后,观察到表面重建和亚稳态小平面暴露,导致晶格氧易于释放。另外,在异质界面的MnO 2和Mn 2 O 3侧分别观察到大量的氧空位和冗余的配位晶格氧。这些特征提供了充足的氧气种类和增加的晶格氧气迁移率。与界面有关的氧空位促进了吸附的甲苯的甲基脱氢和脱甲基。多余的配位晶格氧有助于增强芳环的断裂能力。

更新日期:2020-07-18
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