Radiation effect of polyamide thin film composite membrane in the radioactive wastewater treatment

doi:10.16085/j.issn.1000-6613.2023-0065

Abstract

Abstract:

Polyamide thin film composite membranes usually are applied for water treatment processes such as reverse osmosis, forward osmosis and nanofiltration, and have been paid great attention in the radioactive wastewater treatment. Radiation which is a special characteristic for the radioactive wastewater compared to the traditional wastewater has challenged the stability of the organic separation membrane. This study started from the source analysis of the radioactive wastewater, and introduced the radiation effect on the surface color, separation performance, microstructure, surface functional groups and hydrogen bonds, hydrophilicity, element composition and mechanical properties. Then, the crosslinking and degradation mechanism of membrane material induced by radiation was discussed, and the feasibility of the radioactive wastewater treatment by polyamide membrane was analyzed. Finally, several problems related to radiation effect of polyamide thin film composite membrane were proposed. The radiation effect of polyamide composite membrane studied in this paper had a significant reference value in the analysis of effect of radiation on the structure and performance of composite membrane, exploration in the radiation damage mechanism of organic membrane and design on the radiation-resistant separation membrane.

Key words: radioactive wastewater, polyamide membrane, radiation, membrane structure, separation performance

摘要：

聚酰胺复合膜可被用于反渗透、正渗透、纳滤等水处理工艺，近年来在放射性废水处理中越来越受青睐。辐射是放射性废水区别于常规废水的显著特征，对有机分离膜稳定性提出了很大挑战。本文在分析放射性废水辐射源项的基础上，介绍了辐射对聚酰胺复合膜表面颜色、分离性能、微观结构、表面功能基团与氢键、亲水性、元素组成、力学性能等方面的影响，探讨了辐射诱导膜材料再交联和降解的反应机理，分析了聚酰胺复合膜处理放射性废水的可行性。最后，提出了聚酰胺复合膜辐射效应研究需要关注的几个问题。本文研究的聚酰胺复合膜辐射效应结论对于分析辐射对复合膜结构和性能的影响、探索有机分离膜的辐射损伤机理、开展耐辐射有机分离膜设计具有重要的参考价值。

关键词: 放射性废水, 聚酰胺复合膜, 辐射, 膜结构, 分离性能

CLC Number:

ZHAO Haiyang, LI Xin, ZHANG Lin, HOU Li’an, HE Mingqing. Radiation effect of polyamide thin film composite membrane in the radioactive wastewater treatment[J]. Chemical Industry and Engineering Progress, 2023, 42(12): 6544-6553.

赵海洋, 李鑫, 张林, 侯立安, 何明清. 放射性废水处理中聚酰胺复合膜辐射效应研究进展[J]. 化工进展, 2023, 42(12): 6544-6553.

Figures/Tables 6

References 29

1	TAN Z, CHEN S G, PENG X S, et al. Polyamide membranes with nanoscale turing structures for water purification[J]. Science, 2018,360(6388): 518-521.
2	ZHANG Xiaoyuan, GU Ping, LIU Yu. Decontamination of radioactive wastewater: State of the art and challenges forward[J]. Chemosphere, 2019, 215: 543-553.
3	PHILLIPS D C. Effects of radiation on polymers[J]. Materials Science and Technology, 1988, 4(1): 85-91.
4	RAMACHANDHRAN V, MISRA B M. Studies on effect of irradiation on semipermeable membranes[J]. Journal of Applied Polymer Science, 1982, 27(9): 3427-3435.
5	RAMACHANDHRAN V, MISRA B M. Concentration of radioactive liquid streams by membrane processes[J]. Journal of Applied Polymer Science, 1983, 28(5):1641-1650.
6	CHMIELEWSKI A G, HARASIMOWICZ M. Influence of Gamma and electron irradiation on transport properties of ultrafiltration membranes[J]. Nukleonika, 1992, 37(4): 61-70.
7	YU Suping, ZHANG Xue, LI Fuzhi, et al. Influence of low dose Gamma-ray irradiation on the performance and degradation of PVDF ultrafiltration membrane[J]. Radiation Physics and Chemistry, 2017, 136:38-43.
8	赵海洋, 倪士英, 张林. 纳米材料在放射性废水处理中的应用进展[J]. 化工进展, 2020, 39(3): 1057-1069.
	ZHAO Haiyang, NI Shiying, ZHANG Lin. Application of nanomaterials in the radioactive wastewater treatment[J]. Chemical Industry and Engineering Progress, 2020, 39(3): 1057-1069.
9	环境保护部核与辐射安全中心组织. 核安全综合知识[M]. 修订版. 北京: 中国原子能出版社, 2018.
	Organized by the Nuclear and Radiation Safety Center of the Ministry of Environmental Protection. Comprehensive knowledge of nuclear safety[M]. Revised ed. Beijing: China Atomic Energy Press, 2018.
10	LIU Chao, ZHANG Jiaming, WANG Wenjing, et al. Effects of Gamma-ray irradiation on separation and mechanical properties of polyamide reverse osmosis membrane[J]. Journal of Membrane Science, 2020, 611: 118354.
11	COMBERNOUX Nicolas, SCHRIVE Luc, LABED Véronique, et al. Treatment of radioactive liquid effluents by reverse osmosis membranes: From lab-scale to pilot-scale[J]. Water Research, 2017, 123: 311-320.
12	CHMIELEWSKI A G, HARASIMOWICZ M. Influence of Gamma and electron irradiation on transport properties of nanofiltration and hyperfiltration membranes[J]. Nukleonika, 1997, 42(4):857-62.
13	EL-ARNAOUTY M B, ABDEL GHAFFAR A M, EID M, et al. Nano-modification of polyamide thin film composite reverse osmosis membranes by radiation grafting[J]. Journal of Radiation Research and Applied Sciences, 2018, 11(3): 204-216.
14	GUO Yongqiang, LIU Chao, LIU Hongpeng, et al. Influences of Gamma-ray irradiation on PVDF membrane behavior: an experimental study based on simulation and numerical analysis[J]. Polymer Degradation and Stability, 2021, 193: 109722.
15	NAKASE Yoshiaki, YANAGI Tadashi, UEMURA Tadahiro. Irradiation effects on properties of reverse osmosis membrane based on crosslinked aromatic polyamide[J]. Journal of Nuclear Science and Technology, 1994, 31(11): 1214-1221.
16	CHUNG Youngkun, PARK Daeseon, KIM Hyojeon, et al. The impact of Gamma-irradiation from radioactive liquid wastewater on polymeric structures of nanofiltration (NF) membranes[J]. Journal of Hazardous Materials, 2021, 403: 123578.
17	CLOUGH R L, GILLEN K T, MALONE G M, et al. Color formation in irradiated polymers[J]. Radiation Physics and Chemistry, 1996, 48(5): 583-594.
18	ARNAL J M, SANCHO M, VERDÚ G, et al. Treatment of ¹³⁷Cs liquid wastes by reverse osmosis Part I. Preliminary tests[J]. Desalination, 2003, 154(1): 27-33.
19	COMBERNOUX N, LABED V, SCHRIVE L, et al. Effect of Gamma irradiation at intermediate doses on the performance of reverse osmosis membranes[J]. Radiation Physics and Chemistry, 2016, 124:241-245.
20	COMBERNOUX Nicolas, SCHRIVE Luc, LABED Véronique, et al. Study of polyamide composite reverse osmosis membrane degradation in water under Gamma rays[J]. Journal of Membrane Science, 2015, 480: 64-73.
21	TANG Chuyang Y, KWON Young-Nam, LECKIE James O. Effect of membrane chemistry and coating layer on physiochemical properties of thin film composite polyamide RO and NF membranes I. FTIR and XPS characterization of polyamide and coating layer chemistry[J]. Desalination, 2009, 242(1/2/3): 149-167.
22	LIN Saisai, ZHAO Haiyang, ZHU Liping, et al. Seawater desalination technology and engineering in China: A review[J]. Desalination, 2021, 498: 114728.
23	LIU Xiaojing, WU Jinling, HOU Lian, et al. Performance and deterioration of forward osmosis membrane exposed to various dose of Gamma-ray irradiation[J]. Annals of Nuclear Energy, 2020, 135: 106950.
24	CADOTTE John E. Evolution of composite reverse osmosis membranes[M]//Materials Science of Synthetic Membranes. Washington, D.C.: American Chemical Society, 1985: 273-294.
25	YAN Hao, MIAO Xiaopei, XU Jian, et al. The porous structure of the fully-aromatic polyamide film in reverse osmosis membranes[J]. Journal of Membrane Science, 2015, 475: 504-510.
26	Nyoman RUPIASIH N, VIDYASAGAR P B. Comparative study of effect of low and medium dose rate of γ irradiation on microporous polysulfone membrane using spectroscopic and imaging techniques[J]. Polymer Degradation and Stability, 2008, 93(7): 1300-1307.
27	COMBERNOUX Nicolas, SCHRIVE Luc, LABED Véronique, et al. Irradiation effects on RO membranes: Comparison of aerobic and anaerobic conditions[J]. Polymer Degradation and Stability, 2016, 134: 126-135.
28	ORLANDO Coronell, MARIÑAS Benito J, CAHILL David G. Depth heterogeneity of fully aromatic polyamide active layers in reverse osmosis and nanofiltration membranes[J]. Environmental Science & Technology, 2011, 45(10): 4513-4520.
29	ARNAL J M, SANCHO M, VERDÚ G, et al. Treatment of ¹³⁷Cs liquid wastes by reverse osmosis Part II. Real application[J]. Desalination, 2003, 154(1): 35-42.

核素种类	射线类型	能量
核素种类	射线类型	/MeV	/kJ·mol^-1
⁶⁰Co	γ	1.17 1.33	1.12×10⁸ 1.28×10⁸
¹³⁴Cs	γ	0.605	5.81×10⁷
⁹⁰Sr	β	0.546	5.24×10⁷

核素种类	射线类型	能量
核素种类	射线类型	/MeV	/kJ·mol^-1
⁶⁰Co	γ	1.17 1.33	1.12×10⁸ 1.28×10⁸
¹³⁴Cs	γ	0.605	5.81×10⁷
⁹⁰Sr	β	0.546	5.24×10⁷

复合膜种类	⁶⁰Co外照射		¹³⁴Cs浸入照射		参考文献
复合膜种类	AD1/kGy	AD2/kGy	AD1/kGy	AD2/kGy	参考文献
PA-300	10	15	—	—	[4]
SU-500^①	7	8~9	6	7~8	[12]
SU-600^①	7	8~9	6	7~8	[12]
SU-700L^①	7	8~9	6	7~8	[12]
SU-700R^①	7	8~9	6	7~8	[12]
NTR-7197	>40	>40	>30	>30	[12]
FT-30	>40	>40	>30	>30	[12]

复合膜种类	⁶⁰Co外照射		¹³⁴Cs浸入照射		参考文献
复合膜种类	AD1/kGy	AD2/kGy	AD1/kGy	AD2/kGy	参考文献
PA-300	10	15	—	—	[4]
SU-500^①	7	8~9	6	7~8	[12]
SU-600^①	7	8~9	6	7~8	[12]
SU-700L^①	7	8~9	6	7~8	[12]
SU-700R^①	7	8~9	6	7~8	[12]
NTR-7197	>40	>40	>30	>30	[12]
FT-30	>40	>40	>30	>30	[12]

PA膜			源项			条件		性能参数		参考文献
膜来源	种类	样式	辐射源	剂量率/kGy·h^-1	剂量/kGy	辐射	测试	渗透通量/L·m^-2·h^-1·bar^-1	截留率/%	参考文献
PA-300	反渗透膜	平板膜	⁶⁰Co	—	0	湿	NaCl 200mg/kg，压力39.2bar	324	98.3	[4]
				0.48	25	湿		499	98.4
				0.48	50	湿		875	79.5
未知	反渗透膜	平板膜	加速器		0	湿	NaCl 1500mg/kg，压力14.71bar，pH6.5，25℃	3.14	99.5	[15]
					400	湿		3.14	99.5
					1000	湿		2.95	99.4
					2000	湿		2.83	88.1
					4000	湿		132.00	2.1
Osmonics SE	反渗透膜	平板膜	⁶⁰Co	0.5	0	湿	膜面积138cm²，NaCl 1.0g/L，压力28bar，流速250L/h，pH6.0，(25±0.5)℃	2.9	98.6	[20]
				0.5	100	湿		2.7^①	96.0^①
				0.5	1000	湿		7.0	64
Osmonics SE	反渗透膜	平板膜	⁶⁰Co	0.5	0	干	膜面积138cm²，NaCl 0.5g/L，压力28bar，流速250L/h，pH6.0，(25±0.5)℃	2.9	98.5	[19]
				0.5	100	干		2.3	97.0
				0.5	200	干		2.5	96.3
				0.5	500	干		4.3	95
				0.5	1000	干		7.0	64
SW30 HR	反渗透膜	巻式膜	⁶⁰Co	0	0		膜面积2.6cm²，压力30bar，流速300L/h，pH6.0，(25±3)℃	1.1	99.1	[11]
				0.5	1000			2.2	75
Osmonics SE	反渗透膜	巻式膜		0	0			2.9	98.5
				0.5	1000			7.2	64
				5	1000				92.3
自制	反渗透膜	平板膜	⁶⁰Co	0	0	干/湿	膜面积6.48cm²，NaCl 2000mg/kg，压力15.5bar，流速0.19m/s，pH7.0，(25±0.5)℃	1.94	98.1	[10]
				6	20	干/湿		1.93/1.92^①	98.5/99.0^①
				6	50	干/湿		1.95/1.89^①	98.0/98.8^①
				6	100	干/湿		2.00/1.94^①	97.5/98.5^①
				6	200	干/湿		2.15/2.02^①	95.0/98.0^①
				6	500	干/湿		2.50/2.27	87.7/94.0
自制	正渗透膜	平板膜	⁶⁰Co	0	0	湿	膜面积40.5cm²，盐浓度20mg/L，流速11cm/s，pH7.0，(25±0.5)℃	11.65^②	Co:93.5 Sr:92.4	[23]
				12	20	湿		11.52^②	Co:95.0 Sr:97.3
				12	120	湿		17.82^②	Co:91.3 Sr:95.8
Dow NF90	纳滤膜	平板膜	⁶⁰Co	0	0	湿	膜面积27cm²，UO₂(NO₃)₂·6H₂O 8.0mg/L，CsCl 50mmol/L，CaCl₂ 50mmol/L，压力10bar，流速 10m/s，pH7.2±0.1，(22±1.0)℃	6.74	UO₂²⁺:97 Ca²⁺:96 Cs⁺:95.6	[16]
				10	10	湿		6.14	—
				10	100	湿		4.60	—
				10	300	湿		4.28	UO₂²⁺:81.0 Ca²⁺:74.6 Cs⁺:72.7