超声辅助离子交换法制备Fe/Co/Al-Mt催化剂及性能
Preparation of Fe/Co/Al-Mt catalysts by ultrasound-assisted ion exchange method and its property investigation
-
摘要: 以铁为活性组分,柱撑蒙脱土(Mt)为载体,分别采用传统离子交换法与超声辅助离子交换法制备Fe/Co/Al-Mt(C)与Fe/Co/Al-Mt(U)催化剂.通过FT-IR、XRD、DR UV-Vis、SEM和BET等表征手段分析催化剂的物化性质及表面结构,以甲基橙(MO)染料废水为目标降解物研究催化剂的催化性能,并借助叔丁醇/苯醌验证CWPO反应体系中·OH的产生及降解机理.结果表明,与Fe/Co/Al-Mt(C)相比,Fe/Co/Al-Mt(U)比表面积增大16.2%,孔径增大10.2%,活性组分分散更加均匀,催化活性明显提高,对甲基橙染料废水的COD去除率高达80.3%;并且Fe/Co/Al-Mt(U)催化剂稳定性更高且活性组分流失较少,在四次催化循环后COD去除率仍在70%以上,活性组分Fe离子溶出量仅为0.59 mg·L-1.
-
关键词:
- Fe/Co/Al-Mt /
- CWPO /
- 甲基橙 /
- 超声辅助 /
- ·OH
Abstract: Fe/Co/Al-Mt(C) and Fe/Co/Al-Mt(U) catalysts were prepared by conventional ion exchange method and ultrasound-assisted ion exchange method with iron as active component and pillared montmorillonite(Mt) as carrier. The physicochemical properties and surface structure of the (Fe/Co/Al-Mt) samples were examined by FT-IR,XRD,DR UV-Vis,SEM and BET. In addition, With the methyl orange (MO) of dye wastewater, the catalytic performance of the prepared catalyst was examined, the TBA/BQ was used to infer the·OH generation and degradation mechanism in the CWPO system. The results show that compared with Fe/Co/Al-Mt(C), the Fe/Co/Al-Mt(U) specific surface area was increased by 16.2%, the pore diameter was increased by 10.2%, and the active component was more uniformly dispersed, which made the catalytic activity much higher, the COD removal rate of methyl orange dye wastewater was as high as 80.3%. Fe/Co/Al-Mt(U) had higher stability and reduced active component loss, after four catalytic cycles, the COD removal rate was still above 70%, and the active component Fe ion elution was only 0.59 mg·L-1.-
Key words:
- Fe/Co/Al-Mt /
- CWPO /
- methyl orange /
- ultrasonic method /
- ·OH
-
-
[1] GAO H, ZHAO B X, LUO J C, et al. Fe-Ni-Al pillared montmorillonite as a heterogeneous catalyst for the catalytic wet peroxide oxidation degradation of orange acid Ⅱ:Preparation condition and properties study[J]. Microporous and Mesoporous Materials, 2014, 196:208-215. [2] LI H Y, YAN B, ZHAO B X, et al. Catalytic wet peroxide oxidation of dye wastewater using Fe2O3-CeO2/γ-Al2O3 as Catalyst[J]. Advanced Materials Research, 2014, 884/885:29-32. [3] NEAMTU M, CATRINESCU C, KETTYUP A. Effect of dealumination of iron(Ш)-exchanged Y zeolites on oxidation of Reactive Yellow 84 azo dye in the presence of hydrogen peroxide[J]. Applied Catalysis B:Environmental, 2004, 51(3):149-157. [4] 孙甜, 赵彬侠, 王琪, 等. 铁锆柱撑蒙脱土的制备及其催化湿式过氧化氢氧化染料废水的研究[J]. 高校化学工程学报, 2014, 28(3):659-664. SUN T, ZHAO B X, WANG Q, et al. Preparation of iron-zirconium pillared montmorillonite and its catalytic oxidation of dye wastewater by wet hydrogen peroxide[J]. Journal of Chemical Engineering of Chinese Universities, 2014, 28(3):659-664(in Chinese).
[5] 陈修栋, 邹洪涛, 毛海立, 等. 超声波辅助Al-Fe柱撑蒙脱土催化降解茜素红[J]. 山东化工, 2016, 45(11):149-150. CHEN X D, ZOU H T, MAO H L, et al. Ultrasonic-assisted Al-Fe pillared montmorillonite for catalytic degradation of alizarin red[J]. Shandong Chemical, 2016, 45(11):149-150(in Chinese).
[6] RUI S R, FRONTISTIS Z, MANTZAVINOS D, et al. Magnetic carbon xerogels for the catalytic wet peroxide oxidation of sulfamethoxazole in environmentally relevant water matrices[J]. Applied Catalysis B Environmental, 2016, 199:170-186. [7] SHIRSATH S R, PINJARI D V, GOGATE P R, et al. Ultrasound assisted synthesis of doped TiO2 nano-particles:Characterization and comparison of effectiveness for photocatalytic oxidation of dyestuff effluent[J]. Ultrasonics Sonochemistry, 2013, 20(1):277-286. [8] 吴平霄, 肖文丁. 柱撑蒙脱石制备与表征[J]. 矿物学报, 1997, 17(2):200-207. WU P X, XIAO W D. Preparation and characterization of pillared montmorillonite[J]. Acta Minerala Sinica, 1997(2):200-207(in Chinese).
[9] 彭勇刚, 纪俊玲, 张云龙, 等. 纳米ZnO的超声辅助合成及其光催化性能研究[J]. 印染助剂, 2013(10):12-15. PENG Y G, JI J L, ZHANG Y L, et al. Ultrasound-assisted synthesis of nano-ZnO and its photocatalytic properties[J]. Dyeing and Auxiliaries, 2013 (10):12-15(in Chinese).
[10] KHANIKAR N, BHATTACHARYYA K G. Cu(Ⅱ)-kaolinite and Cu(Ⅱ)-montmorillonite as catalysts for wet oxidative degradation of 2-chlorophenol,4-chlorophenol and 2,4-dichlorophenol[J]. Chemical Engineering Journal, 2013, 233(11):88-97. [11] CATRINESCU C, ARSENE D, APOPEI P, et al. Degradation of 4-chlorophenol from wastewater through heterogeneous Fenton and photo-Fenton process, catalyzed by Al-Fe PILC[J]. Applied Clay Science, 2012, 58(1):96-101. [12] YE W, ZHAO B, GAO H, et al. Preparation of highly efficient and stable Fe,Zn,Al-pillared montmorillonite as heterogeneous catalyst for catalytic wet peroxide oxidation of Orange Ⅱ[J]. Journal of Porous Materials, 2016, 23(2):301-310. [13] KUMARARAIA P, MANJAIAH K M, DATTA S C, et al. Remediation of metal contaminated soil by aluminium pillared bentonite:Synthesis, characterisation, equilibrium study and plant growth experiment[J]. Applied Clay Science, 2017, 137:115-122. [14] 张占梅, 何世德, 周富春. 超声辐射浸渍法制备Fe-Ni-Mn/Al2O3催化剂及性能研究[J]. 环境工程学报, 2012, 6(1):173-177. ZHANG Z M, HE S D, ZHOU F C. Preparation of Fe-Ni-Mn/Al2O3 catalyst by ultrasonic irradiation impregnation method and its properties[J]. Journal of Environmental Engineering, 2012, 6(1):173-177(in Chinese).
[15] BANKOVIC P, MILUTINOVIC N A, MOJOVIC Z, et al. Al,Fe-pillared clays in catalytic decolorization of aqueous tartrazine solutions[J]. Applied Clay Science, 2012, (58):73-78. [16] CHOI J S, YOON S S, JANG S H, et al. Catalytic applications of Fe-MCM-41 for phenol hydroxylation and CNTs synthesis[J]. Studies in Surface Science & Catalysis, 2005, 158:1405-1412. [17] LI N, YANG H M, ZHAO H, et al. Catalytic dehydration of glycerol to acrolein over sulfuric acid-activated montmorillonite catalysts[J]. Applied Clay Science, 2013, 74(4):154-162. [18] BETHI B, MANASA V, SRINIJA K, et al. Intensification of rhodamine-B dye removal using hydrodynamic cavitation coupled with hydrogel adsorption[J]. Chemical Engineering and Processing:Process Intensification, 2018, 134(1):51-57. [19] [20] OLIVIERO L, BARBIER J, DUPREZ D, et al. Catalytic wet air oxidation of phenol and acrylic acid over Ru/C and Ru-CeO2/C catalysts[J]. Applied Catalysis B:Environmental, 2000, 25(4):267-275. -

计量
- 文章访问数: 2084
- HTML全文浏览数: 2084
- PDF下载数: 104
- 施引文献: 0