氮化钼钝化层中钼的价态特征及钼(5+)的发现

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以MoO_3为前身化合物,在H_2/N_2混合气氛中利用程序升温反应方法制备了钝化后比表面为 115 m~2· g~(-1)的γ-Mo_2N粉末催化剂.在低温条件下,该催化剂显示出良好的 CO氧化反应活性.借助X射线电子能谱(XPS)、电子自旋共振(EPR)及激光Raman光谱(LRS)技术对氮化铝的表面钝化层进行了表征,结果表明其中钼以混合价态存在并得到了Mo~(5+)(g=1.932,g//=1.892)存在的证据,同时还发现了超氧负离子O~-(2_)(g=2.001,Raman吸收峰1124 Cm~(-1))的存在.研究表明,它的产生与 MO~(5+)/MO~(4+)氧化还原电对的转换存在着协同性, O~-(_2)可能是 CO氧化反应的活性氧种. Γ-Mo_2N powder catalyst with a specific surface area of ​​115 m 2 · g -1 was prepared by a programmed temperature-programmed reaction in a H 2 / N 2 mixed atmosphere with MoO 3 as the precursor. The catalyst shows good CO oxidation reactivity at low temperature. The surface passivation layer of aluminum nitride was characterized by X-ray photoelectron spectroscopy (XPS), electron spin resonance (EPR) and laser Raman spectroscopy (LRS). The results show that molybdenum exists in a mixed valence state (5) (g = 1.932, g // = 1.892). At the same time, it was also found that the superoxide anion O ~ - (2 _) (-1)). The results show that there is synergy between its production and conversion of MO ~ (5 +) / MO ~ (4+) redox couple. O ~ - (_2) may be the active oxygen species of CO oxidation reaction.
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