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Deactivation mechanism of Fe/Al2O3 catalyst during the ozonation of reverse osmosis concentrates (ROCs): Effect of silicate    

文献类型:期刊文献

英文题名:Deactivation mechanism of Fe/Al2O3 catalyst during the ozonation of reverse osmosis concentrates (ROCs): Effect of silicate

作者:Cheng, Chen[1];Li, Jianping[1];Wen, Yuzhen[1];Wang, Jinling[1,2];Jin, Chengyu[3,4];Sun, Chenglin[3];Wang, Hualin[1,2];Wei, Huangzhao[3];Yang, Xuejing[1,2]

机构:[1]East China Univ Sci & Technol ECUST, Natl Engn Lab Ind Wastewater Treatment, Shanghai 200237, Peoples R China;[2]ECUST, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[3]Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China;[4]Univ Chinese Acad Sci, Beijing 100049, Peoples R China

年份:2020

卷号:1

外文期刊名:CHEMICAL ENGINEERING JOURNAL ADVANCES

收录:WOS:【ESCI(收录号:WOS:001108792800004)】;

基金:We acknowledge supports from the National Key Basic Research Program of China (2019YFC1906700) and National Natural Science Foundation of China (21876049 , 51878643) . The development of catalyst was supported by the internal research funding from Dalian National Laboratory for Clean Energy (Grant: DICP & QIBEBT UN201809) .

语种:英文

外文关键词:Catalytic ozonation; Fe/Al2 O3; Reverse osmosis concentrate (ROC); Deactivation; Zero liquid discharge(ZLD); Silicate

摘要:Catalytic ozonation is regarded as a promising process for the treatment of heavily contaminated industrial wastewater, but has not been widely implemented at full-scale due to the high expense of catalyst. In this paper, the catalysts from a fix-bed catalytic ozonation reactor were collected and analyzed after the consecutive opera-tion of three and a half years. The reactor was fed with 200 m3/h of Reverse osmosis concentrates (ROC) from a coal refinery plant located in mid-west China. The deactivation mechanism of the Fe/Al2O3 catalyst is revealed. It was found that the deposition of Si on the catalyst surface (an increase of about 40 times) was the main cause of deactivation. Herein, the role of typical functional sites of Fe/Al2O3 formed under various physicochemical conditions, for the silicate adsorption was studied based on the adsorption isotherms and theoretical analyses us -ing density functional theory (DFT) calculation. The sites associated with catalytic activation of ozone: Fe-OOH (-0.66 eV) and Fe-O-Al (-0.49 eV) sites have much higher binding energy of silicate than non-reactive Fe-OH (-0.05 eV) sites. As a relatively strong Bronsted acid, silicic acid preferentially interacts with Fe-O-Al and Fe-OOH to reduce the abundance of Lewis acidity on the catalyst surface, which leads to the catalyst poisoning. This work points out the deactivation mechanism of the ozonation catalyst when treating wastewater with high salinity or alkalinity, and will lead to the new direction on the design of heterogenous ozonation catalysts.

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