Performance Study of Carbon Adsorption of Spent Membranes for the Removal of Typical Pollutants in Wastewater

doi:10.12422/j.issn.1006-396X.2024.02.001

Abstract

Abstract:

Organic polymer membranes have been widely used for wastewater treatment.Due to occurrence of irreversible membrane contamination,the replacement of the membrane after the performance decay leads to the generation of a large number of discarded membranes.How to realize the reuse of these waste polymer films has important economic and environmental value.In this study,a carbonaceous material with both ultramicroporous,mesoporous,and macroporous structures was prepared by a simple pyrolysis remodeling reaction using waste hollow fiber membranes as a template.The differences in the adsorption performance of the waste membrane?derived activated carbon and commercial activated carbon were investigated based on the structural characterizations of the carbonaceous materials.The kinetic and thermodynamic processes for the adsorption removal of typical aromatic hydrocarbon organic contaminants and antibiotics from water were investigated.It was found that the the waste membrane carbon with hierarchical pore structure had a higher removal capacity for aromatic hydrocarbon organic pollutants than commercial carbon,while the adsorption performance for antibiotics such as ciprofloxacin,carbamazepine and sulfadiazine was lower than that of commercial carbon.

Key words: Activated carbon, Waste watertreatment membranes, Adsorption, Pore structure, Pollutants

摘要：

在膜法处理污水过程中，广泛使用有机聚合物分离膜。但是，由于不可逆膜污染的发生，需要更换性能衰减后膜，导致大量废膜的生成，因此实现废聚合物膜的再利用具有重要的经济和环境价值。以污水处理厂的废旧中空纤维膜为模板，通过简单的热解重塑反应制备了一种具有超微孔?介孔?大孔结构的炭材料；结合炭材料的结构表征，对活性炭的吸附性能进行了分析，研究了其吸附水中典型芳香烃类和抗生素类污染物的动力学和热力学过程。结果表明，具有分级孔结构的废膜炭对芳香烃类有机污染物的去除能力高于商业炭，而对环丙沙星、卡马西平、磺胺嘧啶等抗生素的吸附性能低于商业炭。

关键词: 活性炭, 废水处理膜, 吸附, 孔结构, 污染物

CLC Number:

TQ203.8

Ruijuan LIU, Lan YANG, Shiyu MIAO, Yanhong LI, Xiaoqiang AN, Huachun LAN. Performance Study of Carbon Adsorption of Spent Membranes for the Removal of Typical Pollutants in Wastewater[J]. Journal of Petrochemical Universities, 2024, 37(2): 1-8.

刘瑞娟, 杨兰, 苗时雨, 李艳红, 安晓强, 兰华春. 废膜炭吸附去除废水中典型污染物的性能研究[J]. 石油化工高等学校学报, 2024, 37(2): 1-8.

Figures/Tables 10

Fig.1 Eelectron microscopy images of waste membrane carbon without and with added KOH

Fig.2 FT?IR spectra of waste membrane carbon andcommercial carbon

Table 1 Comparison of specific surface area,pore volume and average pore size of waste membrane carbon and commercial carbon

炭材料

比表面积/

（m² $⋅$ g^-1）

孔体积/（cm³

⋅

Table 1 Comparison of specific surface area,pore volume and average pore size of waste membrane carbon and commercial carbon

炭材料

比表面积/

（m² $⋅$ g^-1）

孔体积/（cm³

⋅

g^-1）

平均孔径/nm

废膜炭

1 183

0.66

2.23

商业炭

1 937

1.47

3.04

Fig.3 N2 adsorption?desorption isotherms of two carbon materialsand and pore size distributions obtained by DFT modeling

Fig.4 Experimental data and adsorption kinetics fitting curve of petroleum hydrocarbon contaminants and antibiotic by carbon materials

Table 2 Results of model fitting for adsorption kinetics of waste membrane carbon and commercial carbon

污染物	吸附剂	伪一级动力学模型			伪二级动力学模型
污染物	吸附剂	k₁/min^-1	Q_e/(mg·g^-1)	R²	k₂/(g·mg^-1·min^-1)	Q_e/(mg·g^-1)	R²
4⁃氯苯酚	废膜炭	0.144	413.932	0.989	4.14 × 10^-4	459.576	0.997
4⁃氯苯酚	商业炭	0.657	327.829	0.999	4.32 × 10^-3	330.056	0.926
苯甲醛	废膜炭	0.167	415.832	0.978	4.93 × 10^-4	458.775	0.994
苯甲醛	商业炭	1.378	236.444	0.996	2.59 × 10^-2	239.422	0.998
硝基苯	废膜炭	0.197	314.781	0.978	8.04 × 10^-4	343.955	0.998
硝基苯	商业炭	1.177	178.423	0.999	1.54 × 10^-2	180.819	0.999
环丙沙星	废膜炭	0.101	136.567	0.878	8.84 × 10^-3	153.356	0.939
环丙沙星	商业炭	0.355	369.899	0.964	1.39 × 10^-3	396.265	0.996
卡马西平	废膜炭	0.098	190.293	0.964	5.46 × 10^-4	217.854	0.993
卡马西平	商业炭	0.578	388.100	0.990	2.76 × 10^-3	405.608	0.999
磺胺嘧啶	废膜炭	0.060	118.203	0.981	4.50 × 10^-4	142.455	0.995
磺胺嘧啶	商业炭	0.495	170.749	0.918	4.17 × 10^-3	182.693	0.969

Table 3 Physical and chemical properties parameter of modeled pollutants

模型污染物	分子式	分子质量/ （g·mol^-1）	最大吸收波长/nm	XlgP³	pK_a	分子三维尺寸/nm
4⁃氯苯酚	C₆H₅ClO	128.5	224	2.4	9.41	0.91×0.65×0.36
苯甲醛	C₇H₆O	106.1	249	1.5	14.90	0.85×0.69×0.32
硝基苯	C₆H₅NO₂	123.1	267	1.9	3.98（0 ℃）	0.83×0.65×0.32
环丙沙星	C₁₇H₁₈FN₃O₃	331.3	277	-1.1	5.90、8.90	1.50×1.02×0.58
卡马西平	C₁₅H₁₂N₂O	236.3	285	2.5	13.90	1.23×0.92×0.57
磺胺嘧啶	C₁₀H₁₀N₄O₂S	250.3	260	-0.1	6.36	1.19×0.87×0.59

Fig.5 Adsorption isotherms for the adsorption of aromatic hydrocarbon organics by two carbon materials

Fig. 6 Adsorption isotherms for the adsorption of antibiotic pollutants on two charcoal materials

Fig.7 Effect of the number of waste membrane regeneration on the nitrobenzene removal rate

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