吴铎教授与吴张雄教授合作在 Journal of Colloid and Interface Science 上发表研究论文

Sintering- and oxidation-resistant ultrasmall Cu(I)/(II) oxides supported on defect-rich mesoporous alumina microspheres boosting catalytic ozonation

Hua Chen, Cunxia Fang, Xingmin Gao, Guanyun Jiang, Xiaoning Wang, Sheng-Peng Sun, Winston Duo Wu *(吴铎), Zhangxiong Wu *(吴张雄)


Engineering Research Centre of Advanced Powder Technology (ERCAPT), School of Chemical and Environmental Engineering, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, Jiangsu Province 215123, PR China


Journal of Colloid and Interface Science 581 (2021) 964--978


Supported copper oxides with well-dispersed metal species, small size, tunable valence and high stability are highly desirable in catalysis. Herein, novel copper oxide (CuOx) catalysts supported on defect-rich mesoporous alumina microspheres are developed using a spray-drying-assisted evaporation induced self-assembly method. The catalysts possess a special structure composed of a mesoporous outer layer, a mesoporous-nanosphere-stacked under layer and a hollow cavity. Because of this special structure and the defective nature of the alumina support, the CuOx catalysts are ultrasmall in size (1  3 nm), bivalent with a very high Cu+/Cu2+ ratio (0.7), and highly stable against sintering and oxidation at high temperatures (up to 800 °C), while the wet impregnation method results in CuOx catalysts with much larger sizes ( 15 nm) and lower the Cu+/Cu2+ ratios ( 0.29). The catalyst formation mechanism through the spray drying method is proposed and discussed. The catalysts show remarkable performance in catalytic ozonation of phenol wastewaters. With high-concentration phenol (250 ppm) as the model organic pollutant, the optimized catalyst delivers promising catalytic performance with 100 % phenol removal and 53 % TOC removal in 60 minutes, and a high cyclic stability. Superoxide anion free radicals (•O2-), singlet oxygen (1O2) and hydroxyl radicals (•OH) are the predominant reactive species. A detailed structure-performance study reveals the surface hydroxyl groups and Cu+/Cu2+ redox couples play cooperatively to accelerate O3 decomposition generating reactive radicals. The plausible catalytic O3 decomposition mechanism is proposed and discussed with supportive evidences.



链接:https://www.sciencedirect.com/science/article/pii/S0021979720311620