Xu Zhenghao, Yang Wenhao, Si Wenzhe, Chen Jianjun, Peng Yue, Li Junhua
State Key Joint Laboratory of Environment Simulation and Pollution Control, National Engineering Laboratory for Multi Flue Gas Pollution Control Technology and Equipment, School of Environment, Tsinghua University, Beijing 100084, PR China.
State Key Joint Laboratory of Environment Simulation and Pollution Control, National Engineering Laboratory for Multi Flue Gas Pollution Control Technology and Equipment, School of Environment, Tsinghua University, Beijing 100084, PR China.
J Hazard Mater. 2021 Oct 15;420:126641. doi: 10.1016/j.jhazmat.2021.126641. Epub 2021 Jul 19.
MnO catalysts have been widely studied for catalytic gaseous ozone decomposition. However, their poor moisture resistance often leads to undesirable catalytic effects in the presence of high humidity. In this study, a novel catalyst with γ-like MnO was synthesized using the selective dissolution method on LaMnO perovskites. The as-prepared catalyst exhibited quite stable ozone conversion of ~90% within 12 h under 75% relative humidity (400-800 ppm of ozone, 30 °C, 150 000 mL·g·h of WHSV). In contrast, traditional γ-MnO catalyst showed deficient resistance to HO and sensitivity to space velocity. Detailed characterizations showed that the larger number of oxygen vacancies induced by structure reconstruction of the γ-like MnO and residual La cations facilitated ozone decomposition in humid atmosphere. Finally, the reaction rate of ozone decomposition was proposed by a kinetic study, which further proved that the amount and hydrophilicity of oxygen vacancies are the determinants of the first-order reaction rate constant.
MnO催化剂已被广泛研究用于催化气态臭氧分解。然而,它们较差的耐湿性常常导致在高湿度环境下产生不理想的催化效果。在本研究中,采用选择性溶解法在LaMnO钙钛矿上合成了一种具有类γ-MnO的新型催化剂。所制备的催化剂在75%相对湿度下(400 - 800 ppm的臭氧,30°C,150000 mL·g·h的WHSV)12小时内表现出相当稳定的约90%的臭氧转化率。相比之下,传统的γ-MnO催化剂对HO的抗性不足且对空速敏感。详细表征表明,类γ-MnO的结构重构诱导的大量氧空位和残留的La阳离子促进了潮湿气氛中的臭氧分解。最后,通过动力学研究提出了臭氧分解的反应速率,这进一步证明了氧空位的数量和亲水性是一级反应速率常数的决定因素。