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论文类型：期刊论文

发表时间：2020-04-27

发表刊物：ACS APPLIED ENERGY MATERIALS

收录刊物：SCIE

卷号：3

期号：4

页面范围：3465-3476

ISSN号：2574-0962

关键字：reconstruction; Cu2O-CuO mixed oxide; DFT calculations; oxygen dissociated adsorption; bidentate nitrate

摘要：Cubic cuprous oxide is applied in the selective catalytic oxidation of ammonia to nitrogen (NH3-SCO) to investigate the effect of structure evolution on catalytic performance. Different structures (Cu2O, Cu2O-CuO, and CuO) that formed progressively during the reconstruction process with time are discovered by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and other characterization methods. The optimal CuO-Cu2O exhibits the best catalytic performance, which has T-100% = 210 degrees C and above 80% N-2 selectivity. Combining the experimental method and the density functional theory (DFT), the oxygen molecule is adsorbed in the form of a stable molecular state on Cu2O particles, while the dissociative adsorption of O-2 occurs over the mixed CuO-Cu2O and pure CuO phases. It is found that O-2 is more likely to be dissociated and activated on CuO-Cu2O with E-ads = -7.15 eV. There are three kinds of intermediate species (monodentate, bidentate, and bridging nitrate) observed. The formation of key bidentate nitrate species facilitates NH3 conversion and N-2 formation, but the other intermediate species have a negative effect on NH3 oxidation.