Mn-Fe-Ce/GAC CATALYZED OZONE OXIDATION TECHNOLOGY FOR ANILINE WASTEWATER
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摘要: 以颗粒活性炭为载体,在其上负载锰铁铈多金属氧化物,采用浸渍煅烧法制备了Mn-Fe-Ce/GAC催化剂。通过SEM、XRD、XPS、BET对催化剂结构进行表征,结果表明金属在催化剂表面均匀分散。研究了不同因素对催化臭氧氧化降解DOC和TN效果的影响,并且探究了催化剂的重复利用及稳定性。在臭氧投加量为1.9 mg/(L·min),废水初始pH为6.3,进水苯胺浓度为19.89 mg/L的条件下,反应150 min后,DOC和TN去除率分别达到88.88%和86.73%,催化剂处理效果良好,且重复使用5次后,DOC和TN去除率仍保持在75%和70%以上,其重复使用性能稳定。
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关键词:
- Mn-Fe-Ce/GAC /
- 催化臭氧氧化 /
- 非均相催化剂 /
- 苯胺废水 /
- DOC
Abstract: The Mn-Fe-Ce/GAC catalyst was prepared by impregnation calcination using activated carbon particles as the carrier and loaded with Mn-Fe-Ce polymetallic oxides, and its properties were characterized by SEM, XRD, XPS, and BET, and the results showed that the metal was well dispersed and uniformly loaded on the catalyst surface. The effects of catalyst dosage, initial pH and initial aniline concentration of wastewater on the catalytic ozone oxidation degradation of DOC and TN were investigated, and the reuse and stability of the catalyst were also investigated. The main conclusions were as follows: under the conditions of ozone dosage of 1.9 mg/(L·min), initial pH of wastewater of 6.3 and influent aniline concentration of 19.89 mg/L, the DOC and TN removal rates reached 88.88% and 86.73%, respectively, after 150 min of reaction, and the catalyst was proved to have good treatment effect. After the catalyst was reused five times, the DOC and TN removal rates were maintained more than 75% and 70% respectively, and the performance of the catalyst was stable after reuse.-
Key words:
- Mn-Fe-Ce-/GAC /
- catalytic ozone oxidation /
- non-homogeneous catalyst /
- aniline wastewater /
- DOC
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[1] 杨振兴, 郭绍辉. 苯胺废水处理技术综述[J]. 油气田环境保护, 2022, 32(4):1-6. [2] ZHANG C J, CHEN H, XUE G, et al. A critical review of the aniline transformation fate in azo dye wastewater treatment[J]. Journal of cleaner production, 2021,321:128971. [3] 周珉, 罗西子. 模拟苯胺废水的臭氧氧化过程初探[J]. 能源环境保护, 2021, 35(2):24-29. [4] ISSAKA E, AMU-DARKO J N O, YAKUBU S, et al. Advanced catalytic ozonation for degradation of pharmaceutical pollutants: a review[J]. chemosphere, 2022, 289:133208. [5] NASSEH N, ARGHAVAN F S, RODRIGUEZ-COUTO S, et al. Preparation of activated carbon@ZnO composite and its application as a novel catalyst in catalytic ozonation process for metronidazole degradation[J]. Advanced Powder Technology, 2019, 31(2):875-885. [6] JIANG H B, ZHANG R, HAO J L, et al. Design, preparation, characterization, and application of MnxCu1-xOy/γ-Al2O3 catalysts in ozonation to achieve simultaneous organic carbon and nitrogen removal in pyridine wastewater[J]. Science of the Total Environment, 2021, 774(45):145189. [7] SHAHHIRAN A F, RAMLI R M, ZAWAWI A, et al. Modification of TiO2/AC catalyst for visible light degradation of ionic liquid contaminated wastewater: effect of Cu loading on the characterization and efficiency[J]. Materials Today: Proceedings, 2021, 42:124-130. [8] 占小翠, 旷文君, 丁丁, 等. 超声波改性强化Mn/AC催化臭氧化降解苯酚效能分析[J]. 现代化工, 2019, 39(2):103-107. [9] ZHANG J W, GUO Q, WU W L, et al. Preparation of Fe-MnOx/AC by high gravity method for heterogeneous catalytic ozonation of phenolic wastewater[J]. Chemical Engineering Science, 2022, 255:117667. [10] 吴鑫明, 安浩, 赵俊宇, 等. Fe/Mn-PAC催化剂的制备及其催化臭氧氧化降解活性艳蓝KN-R[J]. 环境工程, 2023, 41(4):32-29. [11] JOTHINATHAN L, CAI Q Q, ONG S L, et al. Fe-Mn doped powdered activated carbon pellet as ozone catalyst for cost-effective phenolic wastewater treatment: mechanism studies and phenol by-products elimination[J]. Journal of hazardous materials, 2022, 424:127483. [12] 何帅明, 莫立焕, 徐峻, 等. 活性炭负载铈催化臭氧处理桉木制浆废水[J]. 中国造纸, 2016, 35(3):1-6. [13] 秦航道, 董清芝, 陈洪林, 等. Ce/AC催化臭氧化降解垃圾渗滤液中提取的富里酸[J]. 四川环境, 2015, 34(3):13-17. [14] 国家环境保护总局. 水和废水分析监测方法[M]. 4版. 北京: 中国环境科学出版社, 2002. [15] TRAN Q K, LY H V, KWON B, et al. Catalytic hydrodeoxygenation of guaiacol as a model compound of woody bio-oil over Fe/AC and Ni/γ-Al2O3 catalysts[J]. Renewable Energy, 2021, 173:886-895. [16] 甘玲, 刘琪琪, 李建军, 等. Fe掺杂Mn-Ce/AC催化剂的制备及其低温脱硝[J]. 环境工程学报, 2017, 11(1):445-449. [17] LIU B T, KE Y X. Enhanced selective catalytic oxidation of H2S over Ce-Fe/AC catalysts at ambient temperature[J]. Journal of the Taiwan Institute of Chemical Engineers, 2020, 110:28-33. [18] 胡云琪. Fe-Mn/AC催化臭氧/过硫酸盐处理垃圾渗滤液生化出水实验研究[D]. 南昌: 华东交通大学, 2018. [19] 刘东坡, 陈伟锐, 王静, 等. 铁锌共掺杂MCM-41构建双酸性中心及其催化臭氧化布洛芬[J]. 环境工程学报, 2022, 16(9):2850-2861. [20] 郭彤彤. 活性炭负载MgO掺杂MoO3催化臭氧化水中的磺胺间甲氧嘧啶钠[D]. 郑州: 郑州大学, 2019. [21] ZHAO P, ZHAO Y, GUO R, et al. Preparation of CuO/γ-Al2O3 catalyst for degradation of azo dyes (reactive brilliant red X-3B): an optimization study[J]. Journal of cleaner production, 2021, 328:129624. [22] 李家耀, 宋卫锋, 李秋华, 等. Mn-Fe-Ce/γ-Al2O3催化剂的制备及其在奶牛养殖废水处理中的臭氧催化氧化性能[J]. 环境工程学报, 2020, 14(4):875-883. [23] FAGGHIHINEZHAD M, BAFHDADI M, SHAHIN M S, et al. Catalytic ozonation of real textile wastewater by magnetic oxidized g-C3N4 modified with Al2O3 nanoparticles as a novel catalyst[J]. Separation and Purification Technology, 2022, 283:120208. [24] 仇一帆, 杨佐毅, 宋卫锋, 等. Fe3O4-CeOx/AC催化剂的制备及其催化臭氧氧化降解盐酸四环素[J]. 环境科学学报, 2022, 42(8):146-155. [25] LUO Z F, WANG D H, ZENG W S, et al. Removal of refractory organics from piggery bio-treatment effluent by the catalytic ozonation process with piggery biogas residue biochar as the catalyst[J]. Science of the Total Environment, 2020, 734:139448. [26] LIU J, LI J, HE S, et al. Heterogeneous catalytic ozonation of oxalic acid with an effective catalyst based on copper oxide modified g-C3N4[J]. Separation and Purification Technology, 2020, 234:116120.
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