测量了七种非理想化学计量比的UO2+x（0＜x＜0.66）及UO2和U3O7等理想化学计量比氧化铀的拉曼和红外光谱， 并进行了对比分析， 其中U3O7和U3O8之间UO2+x的分子振动光谱为首次报道。 拉曼光谱结果显示， 随着UO2+x中x值的增加， UO2特征峰中的578和1　150 cm-1峰强度快速减弱， 当x=0.19时， 这两峰基本消失， 可视为准完美萤石晶体结构UO2的标志。 445 cm-1峰强度在减弱的同时变宽并偏移， 当x=0.32时， 该峰已偏移至459 cm-1处， 同时在～630 cm-1出现一弱肩峰， 这与四方相U3O7的特征峰一致。 当x≥0.39时， 459 cm-1峰发生分裂， 在235和754 cm-1处出现新峰并增强， 其特征逐渐与正交相的α-U3O8接近。 但直至x=0.60时， 与α-U3O8相比其333， 397， 483和805 cm-1峰仍不突出。 红外光谱结果显示， 随着UO2+x中x值的增加， UO2位于400～570 cm-1区间的强吸收特征谱带逐渐分裂为～421和～515 cm-1两峰并增强， 同时UO2在～700 cm-1的弱吸收峰逐渐消失， ～645 cm-1处的肩峰逐渐显现， 出现的这三个峰正是U3O7的特征红外吸收峰。 当x≥0.39时， 在744 cm-1出现一强吸收峰并增强， 该峰是α-U3O8的最强特征峰。 但即使x=0.60时， ～645 cm-1峰仍然存在， 同时～515 cm-1峰也未明显分裂成485和535 cm-1峰， 这表明UO2.60仍处于四方相和正交相的过渡阶段。 上述结果表明， 随着x值的增加， UO2+x的晶体结构发生变化， 每次变化均在拉曼和红外光谱中得到体现。 通过对比各特征峰相对强度和位置的变化情况， 可很好区分和表征不同的氧化铀。

Both of Raman and infrared spectra of seven non-stoichiometry and threestoichiometry uranium oxides， including UO2, U3O7 and UO2+x（0＜x＜0.66）, are presented and discussed. The spectra of UO2+x in the stoichiometry range, U3O7 to U3O8, were first obtained and reported.　Three typical peaks were observed at 445, 578 and 1　150 cm-1 in the Raman spectrum of uranium dioxide. The intensities of the peaks at 578 and 1　151 cm-1 decrease quickly with increasing x value of UO2+x, and while x=0.19, the two peaks disappear. Such peaks can therefore be considered as a fin-gerprint of the quasi-perfect UO2 fluorite structure. The peak at 445 cm-1 tends to weaken, broaden and shift to higher wavenumber in more oxidised samples. When x=0.32, this peak is shifted to the 459 cm-1 and a weak peak at about 630 cm-1 appears. The two new peaks are typical of the tetragonal U3O7. While x≥0.39, the peak at 459 cm-1 further splits into separate components. Two peaks at 235 and 754 cm-1 appear for UO2.39 and are visible with increased intensity as the oxygen-uranium ratio is increased. And the Raman spectra of UO2+x are gradually close to U3O8 in the α-phase, which has an orthorhombic unit cell. But several strongest features of theα-U3O8 specturm at 333, 397, 483 and 805 cm-1 are still not outstanding even in UO2.60. The main feature of the UO2 infrared spectrum shows a very broad and strong adsorption band at 400～570 cm-1 and another feature is a weak adsorption peak at about 700 cm-1. The 400～570 cm-1 band undergoes a progressive splitting into two new peaks at ～421 and ～515 cm-1 through increasing incorporation of oxygen into UO2. The weak peak at about 700 cm-1 disappears and a new weak peak appears at about 645 cm-1. The three new peaks are the infrared absorption features of U3O7. An absorption peak at 744 cm-1 which is the strongest feature ofα-U3O8 infrared spectrum appears for UO2.39 and is visible with increased intensity in more oxidised samples. The peak at about 645 cm-1 still exists and 515 cm-1 peak has no further splitting into two new peaks at 485 and 535 cm-1 which also are the infrared absorption features of U3O8 in UO2.60. This indicates that UO2.60 is still in the transition period between tetragonal and orthorhombic phase of uranium oxide. A sequence of phase transitions occurs through increasing x value of UO2+x with different Raman and infrared features.It is easy to identify different uranium oxides by comparing of relative intensities and locations of their characteristic peaks.