环糊精原位改性MoS2管式陶瓷复合膜的制备及性能

doi:10.16085/j.issn.1000-6613.2022-2084

摘要/Abstract

摘要：

在氧化铝陶瓷管基体上原位水热法制备二硫化钼（MoS₂）陶瓷膜的过程中，将β-环糊精（β-CD）作为添加剂加入前体溶液，得到环糊精改性的MoS₂/β-CD管式陶瓷复合纳滤膜。采用扫描电子显微镜、X射线衍射仪、X射线光电子能谱、水接触角和zeta电位等研究了膜的表面形貌、结构、化学组成、亲水性以及荷电性。探究了不同β-CD添加量对复合膜纳滤性能的影响，考察了膜的抗压性和长期运行稳定性。结果表明，β-CD固有的空腔结构提供了更多的水分子传输通道，提高了MoS₂/β-CD陶瓷复合膜的渗透性能。当添加质量分数为2.4%的β-CD时，制备的陶瓷复合纳滤膜水通量最高为325L/(m²·h·MPa)，对伊文思蓝（EB）的截留率达98.6%；对铬黑T（EBT）、二甲酚橙（XO）染料的截留率均在90%以上；且该陶瓷复合纳滤膜在0.2~0.8MPa的压力下运行，显示优异的抗压性，在错流纳滤操作体系中连续运行7天，表现出良好的长期运行稳定性。

关键词: MoS₂陶瓷复合膜, β-环糊精, 原位水热法, 纳滤, 染料分离

Abstract:

The β‍-cyclodextrin modified MoS₂ tubular ceramic composite membrane was prepared by in-situ hydrothermal method on the surface of alumina ceramic substrate with β‍-cyclodextrin (β‍-CD) as an additive into precursor solution. The surface morphology, structure, chemical composition, hydrophilicity and charge of the membrane were well investigated by search engine marketing, X-raydiffraction, X-ray photoelectron spectroscopy, water contact angle and zeta potential techniques. The effect of different β-CD amount on the membrane nanofiltration performance as well as the pressure resistance and long-term stability of the membranes were studied. The results indicated that the permeability of the membrane was greatly increased due to that the cavity-related structure of β‍-CD provided additional fast transport channels for water molecules. When the amount of β‍-CD was 2.4%, the water permeability of the membrane was highest as 325L/(m²·h·MPa) along with 98.6% rejection of Evans blue (EB), and more than 90% rejection for chrome Black T (EBT) and Xylenol orange (XO). The prepared membrane showed an excellent pressure resistance at 0.2—0.8MPa pressure and displayed a great long-term stability.

Key words: MoS₂ ceramic composite membrane, β?-cyclodextrin, in-situ hydrothermal method, nanofiltration, dye separation

中图分类号:

TQ028.8

王妍, 秦振平, 刘越, 张文海, 郭红霞. 环糊精原位改性MoS₂管式陶瓷复合膜的制备及性能[J]. 化工进展, 2023, 42(10): 5373-5380.

WANG Yan, QIN Zhenping, LIU Yue, ZHANG Wenhai, GUO Hongxia. Preparation and properties of β-cyclodextrin in-situ modified MoS₂ tubular ceramic composite membrane[J]. Chemical Industry and Engineering Progress, 2023, 42(10): 5373-5380.

图/表 10

图1 MoS2/β-CD管式陶瓷复合纳滤膜的表面形貌

图2 MoS2/β-CD管式陶瓷复合纳滤膜的断面形貌

图3 MoS2/β-CD管式陶瓷复合纳滤膜表面EDS元素分布图

图4 MoS2/β-CD管式陶瓷复合纳滤膜的XRD图

表1 XPS分析不同MoS2/β-CD管式陶瓷复合膜的元素含量

复合膜	Mo3d/%	S2p/%	C1s/%	O1s/%
M/β-0	22.56	38.35	34.73	4.36
M/β-3	20.47	35.17	39.11	5.25

图5 M/β-0和M/β-3陶瓷复合纳滤膜的XPS谱图

图6 各MoS2/β-CD管式陶瓷复合纳滤膜的动态水接触角和在不同pH条件的zeta电位变化

图7 不同含量β-CD制备的MoS2/β-CD陶瓷复合膜对EB-水溶液的纳滤分离性能

图8 M/β-3陶瓷复合膜对不同染料-水溶液的纳滤分离性能

图9 MoS2/β-CD管式陶瓷复合纳滤膜的抗压性和长期运行稳定性

参考文献 32

1	GAO Jie, SUN Shipeng, ZHU Wenping, et al. Chelating polymer modified P84 nanofiltration (NF) hollow fiber membranes for high efficient heavy metal removal[J]. Water Research, 2014, 63: 252-261.
2	GAO Zhoufan, SHI Guimin, CUI Yue, et al. Organic solvent nanofiltration (OSN) membranes made from plasma grafting of polyethylene glycol on cross-linked polyimide ultrafiltration substrates[J]. Journal of Membrane Science, 2018, 565: 169-178.
3	SOROKO Iwona, LIVINGSTON Andrew. Impact of TiO₂ nanoparticles on morphology and performance of crosslinked polyimide organic solvent nanofiltration (OSN) membranes[J]. Journal of Membrane Science, 2009, 343(1/2): 189-198.
4	ZHANG Huiru, HE Qiming, LUO Jianquan, et al. Sharpening nanofiltration: Strategies for enhanced membrane selectivity[J]. ACS Applied Materials & Interfaces, 2020, 12(36): 39948-39966.
5	LI Rui, Zhaohua MAI, PENG Donglai, et al. In situ formation of porous organic polymer-based thin polyester membranes for loose nanofiltration[J]. Journal of Membrane Science, 2022, 644: 120074.
6	XIA Lingling, REN Jian, WEYD Marcus, et al. Ceramic-supported thin film composite membrane for organic solvent nanofiltration[J]. Journal of Membrane Science, 2018, 563: 857-863.
7	GAO Enlai, LIN Shaozhen, QIN Zhao, et al. Mechanical exfoliation of two-dimensional materials[J]. Journal of the Mechanics and Physics of Solids, 2018, 115: 248-262.
8	SUN Luwei, HUANG Hubiao, PENG Xinsheng. Laminar MoS₂ membranes for molecule separation[J]. Chemical Communications, 2013, 49: 10718.
9	WANG Zhongying, MI Baoxia. Environmental applications of 2D molybdenum disulfide (MoS₂) nanosheets[J]. Environmental Science & Technology, 2017, 51(15): 8229-8244.
10	RADISAVLJEVIC B, RADENOVIC A, BRIVIO J, et al. Single-layer MoS₂ transistors[J]. Nature Nanotechnology, 2011, 6(3): 147-150.
11	LIU Gongping, JIN Wanqin, XU Nanping. Two-dimensional-material membranes: a new family of high-performance separation membranes[J]. Angewandte Chemie International Edition, 2016, 55(43): 13384-13397.
12	LI Yi, YANG Shishi, ZHANG Kaisong, et al. Thin film nanocomposite reverse osmosis membrane modified by two dimensional laminar MoS₂ with improved desalination performance and fouling-resistant characteristics[J]. Desalination, 2019, 454: 48-58.
13	LI Yuanzhen, LINGHU Yaoyao, WU Chao. Separation properties of porous MoS₂ membranes decorated with small molecules[J]. ACS Applied Materials & Interfaces, 2020, 12(17): 20096-20102.
14	RAN Jin, ZHANG Pengpeng, CHU Chengquan, et al. Ultrathin lamellar MoS₂ membranes for organic solvent nanofiltration[J]. Journal of Membrane Science, 2020, 602: 117963.
15	LIU Yang, ZHAO Yingcan, ZHANG Xinbo, et al. MoS₂-based membranes in water treatment and purification[J]. Chemical Engineering Journal, 2021, 422: 130082.
16	GUO Bingyi, JIANG Shudong, TANG Mingjian, et al. MoS₂ membranes for organic solvent nanofiltration: stability and structural control[J]. Journal of Physical Chemistry Letters, 2019, 10(16): 4609-4617.
17	ZHOU Jingyuan, QIN Zhenping, LU Yahua, et al. MoS₂/polyelectrolytes hybrid nanofiltration (NF) membranes with enhanced permselectivity[J]. Journal of the Taiwan Institute of Chemical Engineers, 2018, 84: 196-202.
18	ZHANG Hao, TAYMAZOV Dovletjan, LI Mengping, et al. Construction of MoS₂ composite membranes on ceramic hollow fibers for efficient water desalination[J]. Journal of Membrane Science, 2019, 592: 117369.
19	GAO Jing, ZHANG Miyu, WANG Jingtao, et al. Bioinspired modification of layer-stacked molybdenum disulfide (MoS₂) membranes for enhanced nanofiltration performance[J]. ACS Omega, 2019, 4(2): 4012-4022.
20	LIU Tongtong, QIN Zhenping, LIU Qiaohong, et al. In situ growth of a tubular MoS₂ membrane on a ceramic tube with improved organic solvent nanofiltration performance[J]. Materials Chemistry Frontiers, 2021, 5(7): 3184-3191.
21	LIU Yue, QIN Zhenping, ZHANG Xuehong, et al. In-situ growth of graphene quantum dots modified MoS₂ membrane on tubular ceramic substrate with high permeability for both water and organic solvent[J]. Journal of Membrane Science, 2021, 627: 119247.
22	LIU Yue, LI Xuejian, LIU Tongtong, et al. Alcohols assisted in-situ growth of MoS₂ membrane on tubular ceramic substrate for nanofiltration[J]. Journal of Membrane Science, 2022, 659: 120777.
23	DEL Valle E M Martin. Cyclodextrins and their uses: A review[J]. Process Biochemistry, 2004, 39(9): 1033-1046.
24	KOZLOWSKI Cezary A, SLIWA Wanda. The use of membranes with cyclodextrin units in separation processes: Recent advances[J]. Carbohydrate Polymers, 2008, 74(1): 1-9.
25	李春, 贾萌萌, 张梦蕾, 等. 基于羟丙基-β-环糊精的界面聚合纳滤膜及其性能研究[J]. 膜科学与技术, 2021, 41(6): 118-125.
	LI Chun, JIA Mengmeng, ZHANG Menglei, et al. The interface polymerized nanofiltration membrane with hydroxypropyl-β-cyclodextrin as aqueous monomer[J]. Membrane Science and Technology, 2021, 41(6): 118-125.
26	XUE Jing, JIAO Zhiwei, BI Ran, et al. Chlorine-resistant polyester thin film composite nanofiltration membranes prepared with β-cyclodextrin[J]. Journal of Membrane Science, 2019, 584: 282-289.
27	MAO Heng, ZHANG Haoqing, LI Yifan, et al. Tunable solvent permeation properties of thin film nanocomposite membrane by constructing dual-pathways using cyclodextrins for organic solvent nanofiltration[J]. ACS Sustainable Chemistry & Engineering, 2015, 3(9): 1925-1933.
28	KIBSGAARD Jakob, CHEN Zhebo, REINECKE Benjiamin N, et al. Engineering the surface structure of MoS₂ to preferentially expose active edge sites for electrocatalysis[J]. Nature Materials, 2012, 11: 963-969.
29	HAN Meisheng, LIN Zijia, YU Jie. Ultrathin MoS₂ nanosheets homogenously embedded in a N,O-codoped carbon matrix for high-performance lithium and sodium storage[J]. Journal of Materials Chemistry A, 2019, 7(9): 4804-4812.
30	XIANG Ting, TAO Shi, XU Weiyu, et al. Stable 1T-MoSe₂ and carbon nanotube hybridized flexible film: Binder-free and high-performance Li-ion anode[J]. ACS Nano, 2017, 11(6): 6483-6491.
31	WANG Zhongying, TU Qingsong, ZHENG Sunxiang, et al. Understanding the aqueous stability and filtration capability of MoS₂ membranes[J]. Nano Letters, 2017, 17(12): 7289-7298.
32	JIANG Jinwu, QI Zenan, PARK Harold S, et al. Elastic bending modulus of single-layer molybdenum disulfide (MoS₂): Finite thickness effect[J]. Nanotechnology, 2013, 24(43): 435705.

[1]	叶海星, 陈宇昊, 陈仪, 孙海翔, 牛青山. 镁锂分离复合纳滤膜研究进展[J]. 化工进展, 2023, 42(4): 1934-1943.
[2]	杨凯璐, 陈明星, 王新亚, 张威, 肖长发. 染料废水处理用纳滤膜制备及改性研究进展[J]. 化工进展, 2023, 42(10): 5470-5486.
[3]	王进, 陈青柏, 王建友, 李鹏飞, 董林. 压力驱动及电驱动膜法水软化技术研究现状与展望[J]. 化工进展, 2022, 41(5): 2649-2661.
[4]	孟祥伟, 吴晓莉, 高展鹏, 李文鹏, 王景涛. 蛭石层状膜的制备及有机溶剂纳滤性能[J]. 化工进展, 2022, 41(11): 5986-5995.
[5]	李泽辉, 崔恒, 王军. 氯化聚氯乙烯复合纳滤膜的制备及其在模拟RB5染料废水处理中的应用[J]. 化工进展, 2021, 40(S1): 456-465.
[6]	李志录, 王敏, 赵有璟, 彭正军, 白露. 膜特征对锂资源提取过程的影响[J]. 化工进展, 2021, 40(9): 5061-5072.
[7]	陈宇昊, 刘家辉, 刘娟, 章洪斌, 孙海翔. 新型复合纳滤膜研究进展[J]. 化工进展, 2021, 40(5): 2665-2675.
[8]	金业豪, 冯孝权, 朱军勇, 张亚涛. 有机溶剂纳滤传递模型及最新膜材料研究进展[J]. 化工进展, 2021, 40(11): 6181-6194.
[9]	海玉琰, 何灿, 马瑞, 熊日华. 反渗透/纳滤膜剖检分析与膜污染诊断研究进展[J]. 化工进展, 2021, 40(10): 5720-5729.
[10]	赵东升. 二硫化钼纳米片基水处理纳滤/反渗透膜研究进展[J]. 化工进展, 2021, 40(10): 5590-5599.
[11]	刘紫洋, 秦振平, 崔素萍, 贾萌萌, 安全福, 王乃鑫, 刘燕, 郭红霞. 有机溶剂纳滤膜的润湿性对渗透和分离性能的影响[J]. 化工进展, 2020, 39(7): 2715-2723.
[12]	曹阳, 任玉灵, 郭世伟, 万印华, 罗建泉. 聚酰胺薄层复合膜的界面聚合制备过程调控研究进展[J]. 化工进展, 2020, 39(6): 2125-2134.
[13]	秘一芳, 安全福. 界面聚合聚酰胺纳滤膜渗透选择性能优化的研究进展[J]. 化工进展, 2020, 39(6): 2093-2104.
[14]	许家晟, 谢建国, 鹿燕, 任杰, 陈爽. 碟管式纳滤膜在生活用水处理中的膜污染特性[J]. 化工进展, 2020, 39(5): 2000-2008.
[15]	陈献富, 季华, 范益群. 纳滤膜在功能性低聚糖分离纯化中的应用研究进展[J]. 化工进展, 2019, 38(01): 394-403.

环糊精原位改性MoS₂管式陶瓷复合膜的制备及性能

Preparation and properties of β-cyclodextrin in-situ modified MoS₂ tubular ceramic composite membrane

RichHTML

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

图/表 10

参考文献 32

相关文章 15

编辑推荐

Metrics

本文评价