碳纳米管负载层结构对复合膜分离性能的影响研究

doi:10.11949/j.issn.0438-1157.20171317

化工学报 ›› 2018, Vol. 69 ›› Issue (5): 2318-2326.DOI: 10.11949/j.issn.0438-1157.20171317

• 材料化学工程与纳米技术 • 上一篇下一篇

碳纳米管负载层结构对复合膜分离性能的影响研究

周丰¹, 黄慧敏¹, 钱飞跃^1,2, 沈耀良^1,2, 周晓吉³, 李欣¹, 夏雪¹

1. 苏州科技大学环境科学与工程学院, 江苏苏州 215009;
2. 江苏省环境科学与工程重点实验室, 江苏苏州 215009;
3. 苏州市分离净化材料与技术重点实验室, 江苏苏州 215009

收稿日期:2017-09-27 修回日期:2017-12-11 出版日期:2018-05-05 发布日期:2018-05-05
通讯作者: 钱飞跃
基金资助:
国家自然科学基金项目（51608341）；江苏省自然科学基金项目（BK20150284）；江苏高校优势学科建设工程资助项目；江苏省研究生科研创新计划项目（KYLX16-1359）；苏州科技大学研究生科研创新计划项目（SKCX16-025）。

Effects of carbon nanotubes mats structure on rejection performance of composite membranes

ZHOU Feng¹, HUANG Huimin¹, QIAN Feiyue^1,2, SHEN Yaoliang^1,2, ZHOU Xiaoji³, LI Xin¹, XIA Xue¹

1. School of Environmental Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, Jiangsu, China;
2. Jiangsu Key Laboratory of Environmental Science and Engineering, Suzhou 215009, Jiangsu, China;
3. Suzhou Key Lab of Separation and Purification Materials & Technologies, Suzhou 215009, Jiangsu, China

Received:2017-09-27 Revised:2017-12-11 Online:2018-05-05 Published:2018-05-05
Supported by:
supported by the National Natural Science Foundation of China (51608341), the Natural Science Fund of Jiangsu Higher Education (BK20150284), the Preponderant Discipline Construction Project in Higher Education of Jiangsu Province, the Graduate Student Scientific Research Innovation Projects in Jiangsu Province(KYLX16-1359), and the Graduate Student Scientific Research Innovation Projects in Suzhou University of Science and Technology(SKCX16-025).

摘要/Abstract

摘要：

采用过滤涂敷法将多壁碳纳米管（MWCNTs）负载于氧化铝微滤（MF）膜表面，构建了一种新型复合膜。通过系统考察碳管投加量、外形尺寸对表面碳层结构的影响，建立了其与复合膜分离性能的响应关系，为传统MF膜的改进提供了重要参考。结果表明，借助高分子表面活性剂和超声波辅助技术，可以实现碳管在水溶液中的充分分散，这有利于在膜表面形成相对均匀的碳负载层。对于同类型碳管而言，增大负载量对碳层孔径分布和过滤比阻（r_c）的影响较小。相比之下，使用低长径比（L/D）的碳管可以有效压缩负载碳层中的孔隙尺寸，导致复合膜渗透率降低。而高L/D比碳管在膜表面形成了高度缠绕的蓬松结构，对应的r_c值最小。利用负载碳层的吸附作用，复合膜对小分子富里酸（FA）的截留能力与碳管负载量和比表面积呈现正相关，同时，碳层结构的致密程度也是影响FA截留率的重要因素。

关键词: 碳纳米管, 微滤膜, 过滤, 负载层结构, 渗透率, 吸附作用

Abstract:

A novel composite membrane was prepared by loading multiwalled carbon nanotubes (MWCNTs) on the surface of existing aluminum oxide micro-filtration (MF) membrane using filtration-coating method. The effects of both loading dosages and dimensional sizes of MWCNTs on the surface mats structure were investigated, while the responses to the rejection performance of composite membranes were also established for improving the conventional MF process. The results showed that the effective dispersion of MWCNTs could be achieved by combining large molecular surfactant and ultrasonic technology, which was beneficial to form homogeneous carbon nanotubes mats on the surface of MF membranes. For the same type of MWCNTs, increasing MWCNTs loading dosage would have no significant effects on the pore size distribution and specific filtration resistance (r_c) of carbon nanotubes mats. When the MWCNTs with low length-diameter (L/D) ratio was used, the smaller pore size on the surface mats resulted in the decrease of membranes permeability. On the contrary, a highly twining and fluffy mat structure was observed with the high L/D ratio of MWCNTs, corresponding to the lowest value of r_c. In addition, the positive correlations between the rejection of composite membranes for small molecular fluvic acid and both loading dosages and specific surface area of MWCNTs were found, which was also related to the mats compactness based on the main mechanism of adsorption.

Key words: carbon nanotubes, micro-filtration membrane, filtration, mats structure, permeability, adsorption

中图分类号:

周丰, 黄慧敏, 钱飞跃, 沈耀良, 周晓吉, 李欣, 夏雪. 碳纳米管负载层结构对复合膜分离性能的影响研究[J]. 化工学报, 2018, 69(5): 2318-2326.

ZHOU Feng, HUANG Huimin, QIAN Feiyue, SHEN Yaoliang, ZHOU Xiaoji, LI Xin, XIA Xue. Effects of carbon nanotubes mats structure on rejection performance of composite membranes[J]. CIESC Journal, 2018, 69(5): 2318-2326.

参考文献 31

[1]	LIU X, WANG M, ZHANG S, et al. Application potential of carbon nanotubes in water treatment:a review[J]. Journal of Environmental Sciences, 2013, 25(7):1263-1280.
[2]	DAS R, ALI M E, HAMID S B A, et al. Carbon nanotube membranes for water purification:a bright future in water desalination[J]. Desalination, 2014, 336(1):97-109.
[3]	王震宇, 赵建, 李娜, 等. 人工纳米颗粒对水生生物的毒性效应及其机制研究进展[J]. 环境科学, 2010, 31(6):1409-1418. WANG Z Y, ZHAO J, LI N, et al. Review of ecotoxicity and mechanism of engineered nanoparticles to aquatic organisms[J]. Environmental Science, 2010, 31(6):1409-1418.
[4]	王玉琳, 闻韵, 王晓慧, 等. 多壁碳纳米管长期作用对活性污泥系统的影响[J]. 环境科学研究, 2014, 27(12):1486-1492. WANG Y L, WEN Y, WANG X H, et al. Long-term effects of multi-walled carbon nanotubes on activated sludge system[J]. Research of Environmental Sciences, 2014, 27(12):1486-1492.
[5]	MADAENI S S, ZINADINI S, Vatanpour V. Convective flow adsorption of nickel ions in PVDF membrane embedded with multi-walled carbon nanotubes and PAA coating[J]. Separation & Purification Technology, 2011, 80(1):155-162.
[6]	Ajmani G S, Goodwin D, Marsh K, et al. Modification of low pressure membranes with carbon nanotube layers for fouling control[J]. Water Research, 2012, 46(17):5645-5654.
[7]	Yang X, Lee J, Yuan L, et al. Removal of natural organic matter in water using functionalised carbon nanotube buckypaper[J]. Carbon, 2013, 59(4):160-166.
[8]	王利颖, 石洁, 王凯伦, 等. 碳纳米管改性PVDF中空纤维超滤膜处理二级出水抗污染性能研究[J]. 环境科学, 2017, 38(1):220-228. Wang L Y, Shi J, Wang K L, et al. Effect of PVDF hollow fiber ultrafiltration membranes modification with carbonnanotube on membrane fouling control during ultrafiltration of sewage effluent[J]. Environmental Science, 2017, 38(1):220-228.
[9]	Wang Y, MA J, ZHU J, et al. Multi-walled carbon nanotubes with selected properties for dynamic filtration of pharmaceuticals and personal care products[J]. Water Research, 2016, 92:104-112.
[10]	WANG Y, ZHU J, HUANG H, et al. Carbon nanotube composite membranes for microfiltration of pharmaceuticals and personal care products:capabilities and potential mechanisms[J]. Journal of Membrane Science, 2015, 479:165-174.
[11]	Kukovecz Á, Smajda R, Kónya Z, et al. Controlling the pore diameter distribution of multi-wall carbon nanotube buckypapers[J]. Carbon, 2007, 45(8):1696-1698.
[12]	Ajmani G S, Cho H H, Chalew T E A, et al. Static and dynamic removal of aquatic natural organic matter by carbon nanotubes[J]. Water Research, 2014, 59(4):262-270.
[13]	PAN B, XING B. Adsorption mechanisms of organic chemicals on carbon nanotubes[J]. Environmental Science & Technology, 2008, 42(24):9005-9013.
[14]	史运华, 任玲玲, 李殿卿. 碳纳米管分散研究进展[J]. 化学通报, 2012, 75(6):502-507. SHI Y H, REN L L, LI D Q. The progress on carbon nanotube dispersions[J]. Chemistry, 2012, 75(6):502-507.
[15]	JIANG L, GAO L, SUN J. Production of aqueous colloidal dispersions of carbon nanotubes[J]. Journal of Colloid & Interface Science, 2003, 260(1):89-94.
[16]	Ryabenko A G, Dorofeeva T V, Zvereva G I. UV-VIS-NIR spectroscopy study of sensitivity of single-wall carbon nanotubes to chemical processing and van-der-Waals SWNT/SWNT interaction. Verification of the SWNT content measurements by absorption spectroscopy[J]. Carbon, 2004, 42(8/9):1523-1535.
[17]	Smajda R, Kukovecz Á, Kónya Z, et al. Structure and gas permeability of multi-wall carbon nanotube buckypapers[J]. Carbon, 2007, 45(6):1176-1184.
[18]	Chen X, QIU M, DING H, et al. A reduced graphene oxide nanofiltration membrane intercalated by well-dispersed carbon nanotubes for drinking water purification[J]. Nanoscale, 2016, 8(10):5696-5705.
[19]	Whitby R L D, Fukuda T, Maekawa T, et al. Geometric control and tuneable pore size distribution of buckypaper and buckydiscs[J]. Carbon, 2008, 46(6):949-956.
[20]	špitalský Z, Aggelopoulos C, Tsoukleri G, et al. The effect of oxidation treatment on the properties of multi-walled carbon nanotube thin films[J]. Materials Science & Engineering B, 2009, 165(3):135-138.
[21]	Wang H. Dispersing carbon nanotubes using surfactants[J]. Current Opinion in Colloid & Interface Science, 2009, 14(5):364-371.
[22]	Georgakilas V, Demeslis A, Ntararas E, et al. Hydrophilic nanotube supported graphene-water dispersible carbon superstructure with excellent conductivity[J]. Advanced Functional Materials, 2015, 25(10):1481-1487.
[23]	XIN X, XU G, ZHAO T, et al. Dispersing carbon nanotubes in aqueous solutions by a starlike block copolymer[J]. Journal of Physical Chemistry C, 2008, 112(42):16377-16384.
[24]	Ansón-Casaos A, González-Domínguez J M, Terrado E, et al. Surfactant-free assembling of functionalized single-walled carbon nanotube buckypapers[J]. Carbon, 2010, 48(5):1480-1488.
[25]	Barbari T. Basic principles of membrane technology[J]. Journal of Membrane Science, 1992, 72(3):304-305.
[26]	Zhang J, Jiang D. Influence of geometries of multi-walled carbon nanotubes on the pore structures of buckypaper[J]. Composites Part A, 2012, 43(3):469-474.
[27]	KARANFIL T, Kitis M, KILDUFF J E, et al. Role of granular activated carbon surface chemistry on the adsorption of organic compounds(2):Natural organic matter[J]. Environmental Science & Technology, 1999, 33(11):3217-3224.
[28]	Hyung H, Kim J H. Natural organic matter (NOM) adsorption to multi-walled carbon nanotubes:effect of NOM characteristics and water quality parameters[J]. Environmental Science & Technology, 2008, 42(12):4416-4421.
[29]	Yang K, Xing B. Adsorption of fulvic acid by carbon nanotubes from water[J]. Environmental Pollution, 2009, 157(4):1095-1100.
[30]	Engel M, Chefetz B. Adsorption and desorption of dissolved organic matter by carbon nanotubes:effects of solution chemistry[J]. Environmental Pollution, 2016, 213:90-98.
[31]	Oleszczuk P, Pan B, Xing B. Adsorption and desorption of oxytetracycline and carbamazepine by multiwalled carbon nanotubes[J]. Environmental Science & Technology, 2010, 44(12):9167-9173.

碳纳米管负载层结构对复合膜分离性能的影响研究

Effects of carbon nanotubes mats structure on rejection performance of composite membranes

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