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Low-temperature catalytic CO oxidation over mixed silver-copper oxide Ag2Cu2O3

机译:混合银铜氧化物Ag2Cu2O3上的低温CO催化氧化

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Mixed silver-copper oxide Ag2Cu2O3 was investigated by a combination of physicochemical techniques, including X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and temperature programmed reaction (TPR). The catalytic properties of Ag2Cu2O3 in the reaction of CO oxidation were studied by the TPR-CO + O-2 method and compared with those of CuO nanopowder characterized by a similar specific surface area. On the surface of Ag2Cu2O3, two unequivalent oxygen species (E-b(O1s)= 529.4 eV and 531 eV) with different reaction probability towards CO were observed. Previously, similar oxygen species had been found on the surface of CuO nanopowder. Mixed silver-copper oxide interacted with CO at room temperature, which resulted in the surface reduction Cu2+ -> Cu1+. Such reduction was accompanied by the removal of only oxygen with E-b(O1s) 531 eV. When the mixed oxide was heated in the reaction medium, both oxygen species were eliminated from the surface, leading to the partial decomposition of the Ag2Cu2O3 structure and the appearance of metallic silver. The TPR-CO study showed the presence of weakly bound oxygen species which can be adsorbed on oxygen vacancies in the Ag2Cu2O3 paramelaconite structure. The energy of oxygen vacancy formation on the (001) and (101) surfaces of Ag2Cu2O3 were calculated by periodic density functional theory (DFT). The role of different oxygen species in CO oxidation over the Ag2Cu2O3 surface is discussed. (C) 2015 Elsevier B.V. All rights reserved.
机译:通过物理化学技术的组合研究混合银-铜氧化物Ag2Cu2O3,包括X射线衍射(XRD),X射线光电子能谱(XPS)和程序升温反应(TPR)。通过TPR-CO + O-2方法研究了Ag2Cu2O3在CO氧化反应中的催化性能,并与比表面积相似的CuO纳米粉进行了比较。在Ag2Cu2O3的表面上,观察到了两个对CO反应概率不同的不等价氧物种(E-b(O1s)= 529.4 eV和531 eV)。以前,在CuO纳米粉的表面发现了类似的氧。混合的银铜氧化物在室温下与CO相互作用,导致表面还原Cu2 +-> Cu1 +。这种还原伴随着仅用E-b(O1s)531 eV除去氧气。当在反应介质中加热混合氧化物时,两种氧都从表面被消除,导致Ag2Cu2O3结构的部分分解和金属银的出现。 TPR-CO研究表明存在弱结合的氧,可以吸附在Ag2Cu2O3副黑云母结构中的氧空位上。通过周期性密度泛函理论(DFT)计算了Ag2Cu2O3(001)和(101)表面氧空位形成的能量。讨论了不同氧物种在Ag2Cu2O3表面的CO氧化中的作用。 (C)2015 Elsevier B.V.保留所有权利。

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