MnO_2/γ-Al_2O_3的制备及催化空气氧化处理制革含硫废水
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摘要
以γ-Al_2O_3为载体,采用等体积浸渍法制备了MnO_2/γ-Al_2O_3非均相负载型催化剂,并通过扫描电子显微镜(SEM)、X射线衍射(XRD)及N_2吸附-脱附对催化剂进行了表征。在常温、常压下,以空气为氧化剂、MnO_2/γ-Al_2O_3为催化剂,催化氧化硫化钠模拟废水和真实制革含硫废水,评价MnO_2/γ-Al_2O_3的催化氧化脱硫性能。考察了制备催化剂的焙烧温度、锰负载量、反应温度及催化剂用量对氧化脱硫反应的影响。结果表明:当焙烧温度为450℃、锰负载量为10%、催化剂用量为0.1 g/L时,处理硫离子浓度分别为1 000 mg/L和900 mg/L的硫化钠模拟废水和真实制革含硫废水,反应2.5 h后硫离子的去除率分别为92.2%和85%。催化剂重复使用10次,其催化活性几乎没有下降,具有较好的使用寿命。
A new heterogeneous supported catalyst MnO_2/γ-Al_2O_3 was prepared by impregnation method and characterized by scanning electron microscope, X-Ray Diffraction and N_2 adsorption-desorption. The performance of the catalyst for the removal of sulfion from the model and real sulfur-containing tannery wastewater was investigated by air as oxidant at the normal temperature and atmospheric pressure. The influence of calcination temperature, manganese oxide loading, reaction temperature and the catalyst dosage on the removal rate of sulfion was studied. The results indicate that the MnO_2/γ-Al_2O_3 catalyst has the best catalytic performance when the calcination temperature is 450 ℃ and the manganese oxide loading is 10%. The sulfion removal rate of 92.2% and 85% are obtained respectively from the model and real sulfur-containing tannery wastewater with 1000 mg/L and 900 mg/L sulfion at the normal temperature and atmospheric pressure, reaction time 2.5 h and catalyst dosage 0.1 g/L. There is no obvious decrease on catalytic activity after ten times recycle of the catalyst.
A new heterogeneous supported catalyst MnO_2/γ-Al_2O_3 was prepared by impregnation method and characterized by scanning electron microscope, X-Ray Diffraction and N_2 adsorption-desorption. The performance of the catalyst for the removal of sulfion from the model and real sulfur-containing tannery wastewater was investigated by air as oxidant at the normal temperature and atmospheric pressure. The influence of calcination temperature, manganese oxide loading, reaction temperature and the catalyst dosage on the removal rate of sulfion was studied. The results indicate that the MnO_2/γ-Al_2O_3 catalyst has the best catalytic performance when the calcination temperature is 450 ℃ and the manganese oxide loading is 10%. The sulfion removal rate of 92.2% and 85% are obtained respectively from the model and real sulfur-containing tannery wastewater with 1000 mg/L and 900 mg/L sulfion at the normal temperature and atmospheric pressure, reaction time 2.5 h and catalyst dosage 0.1 g/L. There is no obvious decrease on catalytic activity after ten times recycle of the catalyst.
引文
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[21] Zhang T, Wang D, Gao Z, et al. Performance optimization of a MnO2/carbon nanotube substrate for efficient catalytic oxidation of low-concentration NO at room temperature[J]. Rsc Advances,2016,6(74): 70 261-70 270.
[22] 牟一蒙, 梁红, 李树华,等. 焙烧温度对Mn/Al2O3-TiO2催化剂结构及氧化NO性能的影响[J]. 无机化学学报, 2016, 32(4): 602-608.
[2] 龚文莉. 浅析制革工业废水处理的技术现状[J]. 广东化工,2012,39(2): 136-141.
[3] Vu N D, Bui N D, Minh T T, et al. The oxidation of sulfur-containing compounds using heterogeneous catalysts of transition metal oxides deposited on the polymeric matrix[J]. Journal of Electronic Materials, 2016, 45(5): 2 316-2 321.
[4] 王瑀婷. 制革污水处理方法研究进展[J]. 当代化工研究, 2017(1): 58-59.
[5] 苏帝翰, 王春华, 周加境,等. 氧化锰/AT复合吸附材料去除废水中硫化物的研究[J]. 中国皮革,2013,42(23): 24-28.
[6] Nguyen T A, Juang R S. Treatment of waters and wastewaters containing sulfur dyes: A review[J]. Chemical Engineering Journal, 2013, 219(3): 109-117.
[7] 陶亮亮, 李鹏, 张虹. 制革含硫废水处理技术研究进展[J]. 西部皮革, 2011(20): 43-46.
[8] 傅学忠. 含硫脱毛废水的危害及处置[J]. 皮革与化工, 2012(2): 27-30.
[9] UOP INC. Treatment of an aqueous stream containing water-soluble inorganic sulfide compounds to selectively produce the corresponding sulfate[P]:EP,0623554A1.1994-11-09.
[10] J wolff.关于制革厂内部污水处理站的经验介绍一、除去硫化物硫和用硫酸铁中和废水[J].皮革科技动态,1973(6):24-29.
[11] Touach N, Ortiz-Martínez V M, Salar-García M J, et al. Influence of the preparation method of MnO2 -based cathodes on the performance of single-chamber MFCs using wastewater[J]. Separation & Purification Technology, 2016,171: 174-181.
[12] Nawaz F, Cao H, Xie Y, et al. Selection of active phase of MnO2 for catalytic ozonation of 4-nitrophenol[J]. Chemosphere,2017,168: 1 457-1 466.
[13] Wu D, Hu Z, Zhang X, et al. Remarkable lignin degradation in paper wastewaters over Fe2O3/γ-Al2O3 catalysts using the catalytic wet peroxide oxidation method[J]. Rsc Advances, 2017,7(60): 37 487-37 494.
[14] Lu M, Yao Y, Gao L, et al. Continuous treatment of phenol over an Fe2O3/γ-Al2O3, catalyst in a fixed-bed reactor[J]. Water Air & Soil Pollution,2015,226(4): 87.
[15] Zhang X, Gu P, Li X, et al. Efficient adsorption of radioactive iodide ion from simulated wastewater by nano Cu2O/Cu modified activated carbon[J]. Chemical Engineering Journal, 2017,322(15): 129-139.
[16] 张昊楠, 唐海, 沙俊鹏,等. 热辅助CuO/ZSM-5活化过硫酸盐降解苯酚废水研究[J]. 化工新型材料, 2017(3): 186-189.
[17] Fernández J A, Suan A, Ramírez J C, et al. Treatment of real wastewater with TiO2-films sensitized by a natural-dye obtained from Picramniasellowii[J]. Journal of Environmental Chemical Engineering, 2016, 4(3): 2 848-2 856.
[18] Nhi B D, Maratovich A R, Garipovna A A, et al. Investigation of factors influencing sodium sulfide oxidation in the presence of polymeric heterogeneous catalysts of transition metal oxides[J]. Journal of Sulfur Chemistry, 2014, 35(1): 74-85.
[19] 王婷婷. 硫化钠废碱液的催化氧化研究[D]. 北京: 北京化工大学, 2011.
[20] 张安超, 郑雯雯, 孙志君,等. 负载型MnOx/Al2O3催化剂低温下脱除烟气中单质汞特性[J]. 煤炭学报, 2013,38(2): 471-477.
[21] Zhang T, Wang D, Gao Z, et al. Performance optimization of a MnO2/carbon nanotube substrate for efficient catalytic oxidation of low-concentration NO at room temperature[J]. Rsc Advances,2016,6(74): 70 261-70 270.
[22] 牟一蒙, 梁红, 李树华,等. 焙烧温度对Mn/Al2O3-TiO2催化剂结构及氧化NO性能的影响[J]. 无机化学学报, 2016, 32(4): 602-608.
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