Luo Haopeng, Du Heng, Weng Tingyi, Chen Zihan, Bao Xiangxin, Wang Binbin, An Fengxia, Chen Huan, Jiang Fang
Key Laboratory of Jiangsu Province for Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, Nanjing, 210094, China.
China Energy Science and Technology Research Institute Co. Ltd., Nanjing, 210023, China.
Environ Res. 2025 Jul 31;285(Pt 3):122474. doi: 10.1016/j.envres.2025.122474.
Low-temperature thermal catalysis without additional oxidants offers a promising solution to the challenges of pressure and temperature inherent in catalytic wet air oxidation (CWAO) for water treatment. Bimetallic oxides have demonstrated superior catalytic oxidation activity and stability compared to conventional monometallic oxides. However, research on the effects of bimetallic oxides in liquid-phase low-temperature thermal catalysis is still in its early stages. In this study, we modulate the catalytic performance of CeO by varying Mn doping levels to enhance the removal of contaminants such as acetaminophen from water. The results show that introducing manganese into the cerium lattice distorts the structure and generates oxygen vacancies, enhancing the catalyst's redox performance. This increased oxygen mobility and conversion significantly improve the catalytic oxidation of pollutants. Additionally, the cyclic conversion process of Mn/Mn (Mn) and Ce/Ce is crucial, promoting the cycle of "lattice oxygen reaction-dissolved oxygen replenishment" which is essential for maintaining catalyst stability. Fixed-bed column reactor experiments further confirmed the excellent stability of the MnCeO catalysts, demonstrating their potential for practical applications. This study presents an effective strategy to bolster both performance and stability in low-temperature thermal catalysis, significantly advancing its potential for practical pollutant degradation applications.
无需额外氧化剂的低温热催化为解决催化湿式空气氧化（CWAO）处理水中固有的压力和温度挑战提供了一个有前景的解决方案。与传统的单金属氧化物相比，双金属氧化物已显示出卓越的催化氧化活性和稳定性。然而，关于双金属氧化物在液相低温热催化中的作用的研究仍处于早期阶段。在本研究中，我们通过改变锰掺杂水平来调节CeO的催化性能，以增强从水中去除对乙酰氨基酚等污染物的能力。结果表明，将锰引入铈晶格会使结构变形并产生氧空位，从而增强催化剂的氧化还原性能。这种增加的氧迁移率和转化率显著提高了污染物的催化氧化能力。此外，Mn/Mn（Mn）和Ce/Ce的循环转化过程至关重要，促进了“晶格氧反应-溶解氧补充”的循环，这对于维持催化剂稳定性至关重要。固定床柱反应器实验进一步证实了MnCeO催化剂的优异稳定性，证明了它们在实际应用中的潜力。本研究提出了一种在低温热催化中提高性能和稳定性的有效策略，显著推进了其在实际污染物降解应用中的潜力。
