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氧空位增强Mg-Co-Ce氧化物复合材料对水中氨选择性催化臭氧化的性能

Oxygen vacancies enhancing performance of Mg-Co-Ce oxide composite for the selective catalytic ozonation of ammonia in water.

作者信息

Zhang Zhiyong, Ai Huiying, Fu Ming-Lai, Hu Yi-Bo, Liu Jianqiao, Ji Yuxi, Vasudevan Vasanthakumar, Yuan Baoling

机构信息

Xiamen Key Laboratory of Municipal and Industrial Solid Waste Utilization and Pollution Control, College of Civil Engineering, Huaqiao University, Xiamen, Fujian 361021, P.R. China.

Xiamen Key Laboratory of Municipal and Industrial Solid Waste Utilization and Pollution Control, College of Civil Engineering, Huaqiao University, Xiamen, Fujian 361021, P.R. China.

出版信息

J Hazard Mater. 2022 Aug 15;436:129000. doi: 10.1016/j.jhazmat.2022.129000. Epub 2022 Apr 25.

Abstract

Catalytic ozonation based on heterogeneous metal oxides is a promising approach to removing ammonia as gaseous nitrogen from water. Herein, MgO/CoO/CeO was prepared for catalytic ozonation of ammonia in an aqueous solution. The influence of various reaction conditions was systematically investigated and optimized, in which the reaction kinetics was also analyzed. After doping Ce, the catalyst with Mg-Co-Ce molar ratio of 4:1:1 and calcined at 700 °C for 3 h, has abundant surface oxygen vacancies and exhibited excellent performance for the selective catalytic oxidation of ammonia to gaseous nitrogen by ozone. It was found that the catalytic activity of catalysts was positively related to oxygen vacancies concentration on the composites surface, which might play a vital role in selective catalytic ozonation. Under the optimal conditions, the ammonia removal rate in MgO/CoO/CeO catalytic system was 0.03328 min (R = 0.99942), about 2.1 times greater than that of MgO/CoO (0.01597 min, R = 0.99813), and the selectivity was further enhanced from 73.57% to 86.94%. Moreover, the evolution of nitrogen and chlorine species was determined to discuss the mechanism of selective oxidation of ammonia in the low chlorine-containing solution. This study might promote the understanding of catalytic ozonation of ammonia to gaseous nitrogen selectively.

摘要

基于非均相金属氧化物的催化臭氧化是一种从水中去除氨并将其转化为气态氮的很有前景的方法。在此,制备了MgO/CoO/CeO用于水溶液中氨的催化臭氧化。系统研究并优化了各种反应条件,并分析了反应动力学。掺杂Ce后,Mg-Co-Ce摩尔比为4:1:1且在700℃煅烧3小时的催化剂具有丰富的表面氧空位,并表现出优异的性能,可通过臭氧将氨选择性催化氧化为气态氮。发现催化剂的催化活性与复合材料表面的氧空位浓度呈正相关,这可能在选择性催化臭氧化中起关键作用。在最佳条件下,MgO/CoO/CeO催化体系中的氨去除率为0.03328 min⁻¹(R = 0.99942),约为MgO/CoO(0.01597 min⁻¹,R = 0.99813)的2.1倍,选择性从73.57%进一步提高到86.94%。此外,还确定了氮和氯物种的演变,以探讨低氯溶液中氨的选择性氧化机制。该研究可能有助于增进对氨选择性催化臭氧化为气态氮的理解。

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