Fe增强Ni_(2)(CO_(3))(OH)_(2)臭氧分解抗湿性与催化性能

Iron-doping Enhanced Basic Nickel Carbonate for Moisture Resistance and Catalytic Performance of Ozone Decomposition

臭氧污染已成为我国继PM2.5之后的主要污染物,传统的臭氧分解催化材料在湿润环境中性能不稳定。本工作采用水热法制备了一种铁掺杂改性的碱式碳酸镍催化剂(NiCH-Fe),该催化剂可在60%相对湿度下稳定分解2.14μg/L臭氧12 h,去除率达99%。水分子吸附质量检测结果表明,NiCH-Fe表面的水分子吸附量比纯NiCH明显减少,表面水分子吸脱附可逆;密度泛函理论结果证明,Fe原子是新的代替Ni原子的臭氧吸附位点,并且Fe原子对臭氧分子的吸附能力更强。此外,XPS表明作为活性位点的Fe元素在反应前后保持稳定。掺杂Fe后的催化材料具有优异的抗湿性与长效稳定性。本研究表明通过金属离子掺杂,改变催化材料的表面性质,可获得具有良好抗湿性能的臭氧催化分解材料,这为进一步开发兼具高抗湿性和高活性的臭氧催化分解材料,提供了有效的技术方法。

Ozone pollution is taking more dominant position in China than PM2.5,traditional ozonolysis catalytic materials have limited performance in humid conditions.In this study,an iron-doped basic nickel carbonate catalyst(NiCH-Fe)was successfully fabricated via a facile hydrothermal method,which could stably decompose 2.14μg/L ozone at 60%relative humidity for 12 h with nearly 100%removal ratio.The result of the Quartz Crystal Microbalance test showed that the water molecules adsorbed on the surface of NiCH-Fe were significantly reduced as compared with that adsorbed on pure NiCH,which were favorable for the competitive adsorption of ozone.Density functional theory results proved that Fe atoms were new sites instead of Ni atoms and had stronger adsorption capacity for ozone molecules.In addition,the XPS results demonstrated that the iron atoms serving as active sites were substantially stable in the reaction.Therefore,material doped with Fe provided excellent moisture resistance and long-term stability.This work provides an effective technical method for the development of materials with high moisture resistance ability for efficient ozone catalytic decomposition.