Abstract: CuCe/ZSM-5 catalysts were prepared by microwave-assisted synthesis, and the changes of chemical oxygen demand (COD) removal rate of CuCe/ZSM-5 catalysts in phenol-containing wastewater and industrial wastewater were studied by changing the reaction temperature, initial pH and catalyst addition amount. The catalyst was characterized by XRD, XPS, SEM, TEM and other methods, and the results show that the formation of CuCe solid solution can accelerate the charge conversion between Cu+/Cu2+ and Ce4+/Ce3+ ion pairs, and promote the activation of H2O2 molecules to form strong oxidizing species. CuCe/ZSM-5 shows high activity and stability, and it can achieve a COD removal rate of 90% within 180 min at 75 ℃ and remain stable after five consecutive uses. The catalytic wet hydrogen peroxide oxidation (CWPO) reaction of phenol-containing wastewater and industrial wastewater conforms to the dynamic simulation curve of the first-order kinetic equation, and the complex pollutant composition in industrial wastewater is more difficult to degrade than that of phenol-containing wastewater. GC-MS was used to comprehensively analyze the intermediate products generated during the degradation process, and it was found that phenol was dehydrogenated, ring-opening and oxidized to generate intermediates such as acetic acid, and finally mineralized to generate small molecules such as CO2 and H2O.
许洪祝, 李长波, 赵国峥, 王硕, 梁慧, 付玉婷, 孙子凯, 杨佳潼, 李东彧, 张岱航. CuCe/ZSM-5复合材料的制备及降解有机废水研究[J]. 材料导报, 2022, 36(24): 21070083-7.
XU Hongzhu, LI Changbo, ZHAO Guozheng, WANG Shuo, LIANG Hui, FU Yuting, SUN Zikai, YANG Jiatong, LI Dongyu, ZHANG Daihang. Study on Preparation of CuCe/ZSM-5 Composite Material and Degradation of Organic Wastewater. Materials Reports, 2022, 36(24): 21070083-7.
1 Jiao Z J, Chen L G, Liu Y Q, et al. Journal of Chemical Industry and Engineering, 2020, 71(4), 1646(in Chinese). 焦昭杰, 陈立功, 柳云骐, 等. 化工学报, 2020, 71(4), 1646. 2 Yan Y, Wu X W, Zhang H P.Separation and Purification Technology, 2016, 171(17), 52. 3 He D L, Zhang H P, Yan Y.Royal Society Open Science, 2018, 5(4), 172364. 4 Geng L L, Yang K X, Zhang N W, et al.Journal of Chemical Industry and Engineering, 2018, 69(9), 3869(in Chinese). 耿莉莉, 杨凯旭, 张诺伟, 等. 化工学报, 2018, 69(9), 3869. 5 Geng L L, Chen B B, Yang J H, et al. Applied Catalysis A: General, 2020, 604, 117774. 6 Bin F, Wei X L, Li B, et al. Applied Catalysis B: Environmental, 2015, 162, 282. 7 Lin S S, Chen C L, Chang D J, et al. Water Research, 2002, 36(12), 3009. 8 Zeng X, Liu J, Zhao J F.Plos One, 2018, 13(10), 1. 9 Zhang X J, Sun Y, Liu M,et al. China Environmental Science, 2020, 40(10), 4330(in Chinese). 张宣娇, 孙羽, 刘明, 等. 中国环境科学, 2020, 40(10), 4330. 10 Kobra N, Yeganeh S, Faezeh J C. Mini-Reviews in Organic Chemistry, 2019, 16(2), 102. 11 Min June K, Min Woo L, Kwan-Young L.Applied Surface Science, 2020, 541, 148409. 12 Liu J, Wang C Y, Peng G, et al.Materials Reports, 2018, 32(Z2), 218(in Chinese). 刘剑, 王彩瑜, 彭钢, 等. 材料导报, 2018, 32(Z2), 218. 13 Karolina M V, Andrea K, Stanka Z.Industrial & Engineering Chemistry Research, 2011, 50(8), 4390. 14 Imane B, Laurie B, Rachid K,et al. Applied Catalysis B: Environmental, 2016, 187(15), 228. 15 Xie H M, Zeng J, Zhou G L.Environmental Science and Pollution Research, 2019, 27(1), 846. 16 Rachele C, Mariagrazia I, Mariacristina C, et al.Nanomaterials, 2019, 9(10), 1477. 17 Rita R Z, Pablo M, Fernando V D,et al. Chemical Engineering Journal, 2015, 270(15), 122. 18 Zhao G Z. Synthesize of mesoporous ceria based materials and mechanism of organic compounds degradations. Ph.D. Thesis, Liaoning Technical University, China, 2020(in Chinese). 赵国峥. 介孔氧化铈基材料制备及降解有机物作用机理. 博士学位论文, 辽宁工程技术大学, 2020. 19 Tu S H, Lin L, Luo Z C, et al.Materials Reports B:Research Papers, 2017, 31(12), 114(in Chinese). 涂盛辉, 林立, 骆中璨, 等. 材料导报:研究篇, 2017, 31(12), 114. 20 Xue C, Mao Y P, Wang W L, et al.Journal of Chemical Industry and Engineering, 2018, 69(S2), 210(in Chinese). 薛超, 毛岩鹏, 王文龙, 等. 化工学报, 2018, 69(S2), 210. 21 Ma J C, Guo J M, Ren K W,et al. Fine Chemicals, 2020, 37(10), 2112(in Chinese). 马建超, 郭精茂, 任凯文, 等. 精细化工, 2020, 37(10), 2112. 22 Xu L J, Wang J L.Environmental Science & Technology, 2012, 46(18), 10145. 23 Jiao Z J, Zhou G L, Zhang H D, et al. Journal of the Brazilian Chemical Society, 2018, 29(11), 2233. 24 Zhang L L, Xu D, Hu C, et al. Applied Catalysis B: Environmental, 2017, 207(15), 9.