沸石咪唑酯骨架-8的制备及其对刚果红的吸附性能

doi:10.13475/j.fzxb.20230900801

摘要/Abstract

摘要：

为制备印染废水的吸附材料,以六水合硝酸锌和2-甲基咪唑为原材料,以去离子水作溶剂,采用水溶剂法制备沸石咪唑酯骨架-8(ZIF-8)材料。借助扫描电子显微镜、红外光谱仪、X射线衍射仪等探究ZIF-8材料的结构,测试其对阴离子刚果红染料的吸附性能,并分析其吸附机制。结果表明:ZIF-8颗粒大小均匀,表面光滑,呈多面体结构;其热裂解温度为258 ℃,具有良好的热稳定性;ZIF-8对刚果红的吸附更符合准二级动力学模型和Langmuir吸附等温线模型,即以化学吸附为主且吸附位点等效;吸附过程为自发进行的放热反应,低温有利于吸附;在温度为20 ℃、pH值为7的条件下,ZIF-8对95 mg/L的刚果红溶液的吸附效果最佳,吸附量可达671.41 mg/g。

关键词: 沸石咪唑酯骨架-8, 刚果红, 阴离子染料, 印染废水, 废水处理, 吸附性能, 吸附机制

Abstract:

Objective In order to solve the problem that printing and dyeing wastewater is harmful to the environment and difficult to treat, this research aims to prepare an economical and environmentally friendly adsorbent with excellent adsorption effect, and the adsorption performance of ZIF-8 on azo dyes represented by anionic Congo Red dyes was investigated.

Method In this research, 2-methylimidazole and Zn(NO₃)₂·6H₂O were used as raw materials, and deionized water was used as solvent. The proportion of 2-methylimidazole, Zn(NO₃)₂·6H₂O and deionized water was adjusted and they mixed by mechanical stirring to prepare the homogeneous and clear particles of zeolitic imidazolate framework-8 (ZIF-8) material under normal temperature and normal pressure conditions. The structure of the ZIF-8 material was tested by scanning electron microscopy(SEM), infrared spectrometry, X-Ray diffraction, thermogravimetry, BET and other characterization methods. The adsorption performance of the material on dyes was evaluated by the water-bath constant-temperature shaking method, and the factors affecting the adsorption and the adsorption mechanism were analyzed.

Results It was found from SEM images that the ZIF-8 section was smooth, and that the particles were uniform and had a polyhedral structure. Infrared spectra analysis and X-Ray diffraction results showed that the ZIF-8 material was consistent with the finding reported in docoments. Thermogravimetric analysis and specific surface area tests revealed that the thermal cleavage temperature of the ZIF-8 material was 258 ℃, and the ZIF-8 had a good thermal stability. The specific surface area of BET was 869.63 m²/g, the specific surface area of Langmuir was 1 140.03 m²/g, and the average pore size was 3.27 nm. The adsorption equilibrium was reached in a shorter time at the lower initial concentration, and the adsorption amount reached the maximum when the initial concentration was 95 mg/L. It was found that the adsorption would first rise, then fall and finally tend to equilibrium with the increase of ion concentration, and the adsorption amount could reach the maximum when pH was neutral. It was also revealed that the adsorption rate of ZIF-8 could still be maintained at 69% after 4 cycles. The adsorption of ZIF-8 on Congo Red was more in line with the pseudo-second-order model through the fitting of kinetic model, which was dominated by chemical adsorption. The adsorption isotherm model fitting showed that the adsorption of ZIF-8 on Congo Red was in line with the Langmuir model, which belonged to the adsorption of the monolayer molecules. It was believed that the whole adsorption process was an exothermic reaction, and the low temperature was favorable for the adsorption. Under the conditions of 20 ℃ and pH=7, the adsorption effect of ZIF-8 on 95 mg/L Congo Red solution was the best, and the maximum adsorption rate was 671.41 mg/g.

Conclusion ZIF-8 prepared using deionized water as the solvent is found to reduce cost compared to the situation with methanol as the solvent, and the operation is simple and safe compared to other preparation methods. The ZIF-8 particles prepared are uniform and clear, with good thermal stability and large specific surface area. ZIF-8 has better adsorption performance on anionic dyes represented by Congo Red, so it can be applied to the treatment of general anionic dye waste liquid.

Key words: zeolitic imidazolate framework-8, Congo Red, anionic dye, printing and dyeing wastewater, wastewater treatment, adsorption performance, adsorption mechanism

中图分类号:

TS176

杨亮, 孔韩韩, 李韦霖, 祁小芬, 张天芸, 王雪梅, 李文全. 沸石咪唑酯骨架-8的制备及其对刚果红的吸附性能[J]. 纺织学报, 2024, 45(07): 140-149.

YANG Liang, KONG Hanhan, LI Weilin, QI Xiaofen, ZHANG Tianyun, WANG Xuemei, LI Wenquan. Preparation of zeolitic imidazolate framework-8 and its adsorption performance on Congo Red[J]. Journal of Textile Research, 2024, 45(07): 140-149.

导出引用管理器 EndNote|Reference Manager|ProCite|BibTeX|RefWorks

链接本文: http://www.fzxb.org.cn/CN/10.13475/j.fzxb.20230900801

http://www.fzxb.org.cn/CN/Y2024/V45/I07/140

图/表 17

图1

图2

图3

图4

图5

图6

图7

图8

图9

图10

图11

表1

表2

内扩散参数"

温度/ ℃	表面扩散		中孔扩散		微孔扩散
温度/ ℃	K₁	$R 12$	K₂	$R 22$	K₃	$R 32$
20	9.126 6	0.995 7	1.672 5	0.911 3	0.012 4	0.110 0
30	9.842 8	0.992 1	0.923 2	0.840 8	0.028 6	0.367 6
40	0.957 0	0.999 3	1.541 6	0.924 9	0.012 8	0.411 0

表2

表3

图12

表4

图13

参考文献 24

[1]	付玮康, 郭筱洁, 潘孟涛, 等. 柳絮纤维生物质炭的制备及其对染料废液中Cr(Ⅵ)的吸附性能[J]. 纺织学报, 2022, 43(12): 8-15. doi: 10.13475/j.fzxb.20210905908
	FU Weikang, GUO Xiaojie, PAN Mengtao, et al. Preparation of biomass charcoal from willow floss fibers and its adsorption performance on Cr(VI) in dye wastewater[J]. Journal of Textile Research, 2022, 43(12): 8-15. doi: 10.13475/j.fzxb.20210905908
[2]	MOK C F, CHING Y C, MUHAMAD F, et al. Adsorption of dyes using poly(vinyl alcohol) (PVA) and PVA-based polymer composite adsorbents: a review[J]. Journal of Polymers and the Environment, 2020, 28(3): 775-793.
[3]	HAMAD M T M H, SAIED M S S. Kinetic studies of Congo red dye adsorption by immobilized aspergillus niger on alginate[J]. Applied Water Science, 2021. DOI: 10.1007/s13201-021-01362-z.
[4]	AOOPNGAN C, NONKUMWONG J, PHUMYING S, et al. Amine-functionalized and hydroxyl-functionalized magnesium ferrite nanoparticles for congo red adsorp-tion[J]. ACS Applied Nano Materials, 2019, 2(8): 5329-5341.
[5]	RADOOR S, KARAYIL J, PARAMESWARANPILLAI J, et al. Adsorption of methylene blue dye from aqueous solution by a novel PVA/CMC/halloysite nanoclay bio-composite: characterization, kinetics, isotherm and antibacterial properties[J]. Journal of Environmental Health Science and Engineering, 2020, 18(2): 1311-1327.
[6]	王宸杨, 贾洁, 李发学. β-环糊精基金属有机框架材料的制备及其对重金属离子的吸附[J]. 纺织学报, 2023, 44(8): 158-166.
	WANG Chenyang, JIA Jie, LI Faxue. Preparation of β-cyclodextrin-based metal-organic framework materials and their adsorption of heavy metal ions[J]. Journal of Textile Research, 2023, 44(8): 158-166.
[7]	JAMES J B, LIN Y S. Thermal stability of ZIF-8 membranes for gas separations[J]. Journal of Membrane Science, 2017, 532: 9-19.
[8]	FUJIWARA A, WATANABE S, MIYAHARA M T. Flow microreactor synthesis of zeolitic imidazolate framework (ZIF)@ZIF core-shell metal-organic framework particles and their adsorption properties[J]. Langmuir, 2021, 37(13): 3858-3867. doi: 10.1021/acs.langmuir.0c03378 pmid: 33626277
[9]	张磊, MUHAMMAD I P, 王波涛, 等. 不同方法合成ZIF-8及其对有机染料的吸附动力学研究[J]. 内江科技, 2020, 41(2): 147-148.
	ZHANG Lei, MUHAMMAD I P, WANG Botao, et al. Synthesis of ZIF-8 by different methods and its adsorption kinetics on organic dyes[J]. Neijiang Science and Technology, 2020, 41(2): 147-148.
[10]	王静, 娄娅娅, 张书涛, 等. ZIF-8的制备及其对染料的吸附和可见光降解[J]. 印染, 2019, 45(19): 44-47.
	WANG Jing, LOU Yaya, ZHANG Shutao, et al. Preparation of ZIF-8 and its adsorption and visible light degradation of dyes[J]. China Dyeing & Finishing, 2019, 45 (19): 44-47.
[11]	杨亮, 孔韩韩, 李韦霖, 等. 聚乙烯醇/ZIF-8复合膜的制备及吸附性能[J]. 印染, 2024, 50(2): 72-78.
	YANG Liang, KONG Hanhan, LI Weilin, et al. Preparation and adsorption properties of polyvinyl alcohol/ZIF-8 composite membrane[J]. China Dyeing & Finishing, 2024, 50(2): 72-78.
[12]	AHMADIJOKANI F, MOLAVI H, BAHI A, et al. Electrospun nanofibers of chitosan/polyvinyl alcohol/ UiO-66/nanodiamond: versatile adsorbents for waste-water remediation and organic dye removal[J]. Chemical Engineering Journal, 2023. DOI: 10.1016/j.cej.2022.141176.
[13]	YANG H, GUO X, CHEN R, et al. Enhanced anti-biofouling ability of polyurethane anti-cavitation coating with ZIF-8: a comparative study of various sizes of ZIF-8 on coating[J]. European Polymer Journal, 2021. DOI: 10.1016/j.eurpolymj. 2020.110212.
[14]	VENNA S R, JASINSKI J B, CARREON M A. Structural evolution of zeolitic imidazolate framework-8[J]. Journal of the American Chemical Society, 2010, 132(51): 18030-18033. doi: 10.1021/ja109268m pmid: 21133378
[15]	ZHANG H, HOU J, HU Y, et al. Ultrafast selective transport of alkali metal ions in metal organic frameworks with subnanometer pores[J]. Science Advances, 2018. DOI: 10.1126 /sciadv. aaq0066.
[16]	WANG Z, HE Y, ZHU L, et al. Natural porous wood decorated with ZIF-8 for high efficient iodine capture[J]. Materials Chemistry and Physics, 2021. DOI: 10.1016/j.matchemphys.2020.123964.
[17]	CHU F, ZHENG Y, WEN B, et al. Adsorption of toluene with water on zeolitic imidazolate framework-8/graphene oxide hybrid nanocomposites in a humid atmosphere[J]. RSC Advances, 2018, 8(5): 2426-2432.
[18]	XIAO F, CHENG J, FAN X, et al. Adsorptive removal of the hazardous anionic dye Congo red and mechanistic study of ZIF-8[J]. Desalination and Water Treatment, 2018, 101: 291-300.
[19]	BHAT S A, ZAFAR F, MONDAL A H, et al. Efficient removal of Congo red dye from aqueous solution by adsorbent films of polyvinyl alcohol/melamine-formaldehyde composite and bactericidal effects[J]. Journal of Cleaner Production, 2020. DOI: 10.1016/j.jclepro.2020.120062.
[20]	HAN L-J, GE F-Y, SUN G-H, et al. Effective adsorption of Congo red by a MOF-based magnetic material[J]. Dalton Transactions, 2019, 48(14): 4650-4656.
[21]	NAYAK A, SAHOO J K, SAHOO S K, et al. Removal of congo red dye from aqueous solution using zinc oxide nanoparticles synthesised from Ocimum sanctum (Tulsi leaf): a green approach[J]. International Journal of Environmental Analytical Chemistry, 2022, 102(19): 7889-7910.
[22]	SINGH N J, WAREPPAM B, KUMAR A, et al. Zeolite incorporated iron oxide nanoparticle composites for enhanced congo red dye removal[J]. Journal of Materials Research, 2023, 38(4): 1149-1161.
[23]	DHANAVEL S, NIVETHAA E A K, DHANAPAL K, et al. α-MoO₃/polyaniline composite for effective scavenging of Rhodamine B, Congo red and textile dye effluent[J]. RSC Advances, 2016, 6(34): 28871-28886.
[24]	DAI J, CHEN T, CHEN Q, et al. Facile synthesis of ZIF-8-lignosulfonate microspheres with ultra-high adsorption capacity for Congo red and tetracycline removal from water[J]. International Journal of Biological Macromolecules, 2023. DOI: 10.1016/j.ijbiomac.2023.124672.

Metrics

Viewed

Full text

Abstract

Cited

Shared

Discussed

C₀/(mg·L^-1)	准二级动力学模型			准一级动力学模型
C₀/(mg·L^-1)	q_e/(mg·g^-1)	k₂/(g_·mg^-1·min^-1)	q_t/(mg·g^-1)	R²	k₁/min^-1	q_t/(mg·g^-1)	R²
15	52.456 3	0.052 4	8.632 0	0.997 2	0.018 3	53.264 1	0.867 5
45	206.238 9	0.087 4	235.360 0	0.997 6	0.004 4	219.385 0	0.925 6
95	415.654 0	0.520 0	325.513 2	0.998 7	0.002 1	452.361 4	0.970 4

温度/ ℃	Freundlich模型
温度/ ℃	K_F	n	R²	b/ (L·mg^-1)	q_m/ (mg·g^-1)	R²
20	103.967 2	2.963 2	0.996 8	0.060 6	670.632 6	0.997 9
30	59.638 9	2.689 1	0.997 4	0.108 4	430.361 0	0.999 1
40	46.310 5	2.736 4	0.997 0	0.160 4	342.698 1	0.998 9

温度/ ℃	ΔG/ (kJ·mol^-1)
20	-12.444 7	-156.802 0	-58.387 7
30	-10.876 7
40	-9.308 7