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delta-MnO2-Mn3O4 Nanocomposite for Photochemical Water Oxidation: Active Structure Stabilized in the Interface

机译:用于光化学水氧化的δ-MnO2-Mn3O4纳米复合材料:界面稳定的活性结构

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摘要

Pure phase manganese oxides have been widely studied as water oxidation catalysts, but further improvement of their activities is much challenging. Herein, we report an effective method to improve the water oxidation activity by fabricating a nanocomposite of Mn3O4 and delta-MnO2 with an active interface. The nanocomposite was achieved by a partial reduction approach which induced an in situ growth of Mn3O4 nanoparticles from the surface of delta-MnO2 nanosheets. The optimum composition was determined to be 38% Mn3O4 and 62% delta-MnO2 as confirmed by X-ray photoelectron spectra (XPS) and X-ray absorption spectra (XAS). The (delta-MnO2-Mn3O4 nanocomposite is a highly active water oxidation catalyst with a turnover frequency (TOP) of 0.93 s(-1), which is much higher than the iridividUal components Of delta-MnO2 and Mn3O4. We consider that the enhanced water oxidation activity could be explained by the active interface between two components. At the phase interface, weak Mn-O bonds are introduced by lattice disorder in the transition of hausmannite phase to birnessite phase, which provides active sites for water oxidation CatalysisiOur study illustrates a new view to improve water oxidation activity of manganese oxides.
机译:纯相锰氧化物已作为水氧化催化剂得到了广泛研究,但进一步提高其活性却面临很大挑战。在这里,我们报告了一种有效的方法,可以通过制造具有活性界面的Mn3O4和δ-MnO2纳米复合材料来提高水的氧化活性。纳米复合材料是通过部分还原的方法实现的,该方法可从MnO2纳米片的表面诱导Mn3O4纳米粒子的原位生长。如通过X射线光电子能谱(XPS)和X射线吸收光谱(XAS)所证实的,确定的最佳组成为38%的Mn 3 O 4和62%的δ-MnO2。 (δ-MnO2-Mn3O4纳米复合材料是一种高活性水氧化催化剂,其周转频率(TOP)为0.93 s(-1),远高于δ-MnO2和Mn3O4的虹吸成分。水的氧化活性可以用两个组分之间的活性界面来解释,在相界面处,锰硅石弱相的引入是由菱锰矿无序引入的,改变了锰锌矿相向水钠锰矿相的转变,为水氧化提供了活性部位。改善锰氧化物水氧化活性的新观点。

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