Lan Yuanpei, Xia Xuewen, Li Junqi, Mao Xisong, Chen Chaoyi, Ning Deyang, Chu Zhiyao, Zhang Junshan, Liu Fengyuan
Department of Metallurgical Engineering, College of Materials and Metallurgy, Guizhou University, Huaxi, Guiyang 550025, China.
Guizhou Province Key Laboratory of Metallurgical Engineering and Process Energy Saving, Guiyang 550025, China.
Nanomaterials (Basel). 2021 Apr 29;11(5):1168. doi: 10.3390/nano11051168.
Oxygen vacancies (OVs) have critical effects on the photoelectric characterizations and photocatalytic activity of nanoceria, but the contributions of surface OVs on the promoted photocatalytic properties are not clear yet. In this work, we synthesized ceria nanopolyhedron (P-CeO), ceria nanocube (C-CeO) and ceria nanorod (R-CeO), respectively, and annealed them at 600 °C in air, 30%, 60% or pure H. After annealing, the surface OVs concentration of ceria elevates with the rising of H concentration. Photocatalytic activity of annealed ceria is promoted with the increasing of surface OVs, the methylene blue photodegradation ratio with pure hydrogen annealed of P-CeO, C-CeO or R-CeO is 93.82%, 85.15% and 90.09%, respectively. Band gap of annealed ceria expands first and then tends to narrow slightly with the rising of surface OVs, while the valence band (VB) and conductive band (CB) of annealed ceria changed slightly. Both of photoluminescence spectra and photocurrent results indicate that the separation efficiency of photoinduced electron-hole pairs is significantly enhanced with the increasing of the surface OVs concentration. The notable weakened recombination of photogenerated carrier is suggested to attribute a momentous contribution on the enhanced photocatalytic activity of ceria which contains surface OVs.
氧空位(OVs)对纳米氧化铈的光电特性和光催化活性具有关键影响,但表面氧空位对光催化性能提升的贡献尚不清楚。在本工作中,我们分别合成了氧化铈纳米多面体(P-CeO)、氧化铈纳米立方体(C-CeO)和氧化铈纳米棒(R-CeO),并在空气、30%、60%或纯氢气中于600℃对它们进行退火处理。退火后,氧化铈的表面氧空位浓度随氢气浓度的升高而增加。退火后的氧化铈的光催化活性随着表面氧空位的增加而提高,P-CeO、C-CeO或R-CeO在纯氢气中退火后的亚甲基蓝光降解率分别为93.82%、85.15%和90.09%。退火后的氧化铈的带隙先扩大,然后随着表面氧空位的增加略有变窄,而退火后的氧化铈的价带(VB)和导带(CB)变化不大。光致发光光谱和光电流结果均表明,随着表面氧空位浓度的增加,光生电子-空穴对的分离效率显著提高。光生载流子复合的显著减弱被认为是对含有表面氧空位的氧化铈光催化活性增强的重要贡献。