用于喷墨印花染料纯化的自组装GO/TiO2复合纳滤膜的制备

doi:10.11949/0438-1157.20190861

摘要/Abstract

摘要：

数码喷墨打印技术对墨水高纯度和低含盐量要求，不断促使染料纯化技术的开发与研究。基于氧化石墨烯(GO)/纳米二氧化钛(TiO₂)自组装的纳滤膜材料的开发，探究了纳米TiO₂颗粒尺寸和与GO共混比例，所获最优GO/TiO₂复合纳滤膜中TiO₂颗粒尺寸为60 nm，与GO共混比例为1∶1。其纯水通量为10.69 L/(m²·h·bar)，对NaCl和Na₂SO₄的截留分别为12.6%和15.7%，对铬黑T、刚果红和考马斯亮蓝R的截留均高于99%。采用自制的连续恒容渗滤装置对粗品墨水进行染料脱盐浓缩的实验，所获染料的浓度由最初的2.0 g/L浓缩至9.74 g/L，NaCl和Na₂SO₄浓度则由起始10 g/L分别下降至5.3 mg/L和11 mg/L，满足数码印花对墨水高纯度以及低盐度的要求。

关键词: GO/TiO₂复合膜, 分离, 纳米粒子, 连续恒容渗滤, 纳滤

Abstract:

The technology of digital inkjet printing requires inkjet printing dye with high purity and low salt. Based on preparation of GO / nano TiO₂ self-assembled nanofiltration membrane, the size of nano TiO₂ particles and the blending ratio with GO were explored. The optimal GO/TiO₂ composite nanofiltration membrane was obtained in which the TiO₂ particle size was 60 nm and the blending ratio with GO was 1∶1. The pure water permeance was 10.69 L/(m²·h·bar), the rejection of NaCl and Na₂SO₄ was 12.6% and 15.7% respectively, and the rejection of Eriochrome black T, Congo red and Coomassie brilliant blue R were all higher than 99%. The home-made continuous constant volume diafitration device was used to conduct the dye desalination and concentration experiment. The concentration of obtained ink was increased from the initial 2.0 g/L to 9.74 g/L, and the concentration of NaCl and Na₂SO₄ was reduced from the initial 10 g/L to 5.3 mg/L and 11 mg/L respectively, meeting the requirements of digital inkjet printing dye.

Key words: GO/TiO₂ composite membrane, separation, nanoparticles, continuous constant volume diafiltration, nanofiltration

中图分类号:

TQ 028.8

徐燕青, 李文飞, 吴梦瑶, 沈江南. 用于喷墨印花染料纯化的自组装GO/TiO₂复合纳滤膜的制备[J]. 化工学报, 2020, 71(3): 1352-1361.

Yanqing XU, Wenfei LI, Mengyao WU, Jiangnan SHEN. Preparation of self-assembled graphene oxide / nano TiO₂ composite nanofiltration membrane for inkjet printing dye[J]. CIESC Journal, 2020, 71(3): 1352-1361.

图/表 13

图1 GO/TiO2复合膜制备示意图

Fig.1 Schematic illustration of preparation of GO/TiO2 composite membrane

图2 膜性能测试及连续恒容渗滤装置

Fig.2 Schematic illustration of membrane performance device and continuous constant volume diafiltration device

图3 氧化石墨烯的形貌及化学结构

Fig.3 Morphology and chemical structure of GO

图4 不同纳米TiO2尺寸对渗透通量和截留的影响(GO∶TiO2=1∶1；NaCl：1000 mg/L，Na2SO4：1000 mg/L，铬黑T：50 mg/L)

Fig.4 Effect of TiO2 sizes on permeance and rejection (GO∶TiO2=1∶1；NaCl: 1000 mg/L, Na2SO4:1000 mg/L, Eriochrome black T: 50 mg/L)

图5 GO与纳米TiO2比例对渗透通量和截留的影响(TiO2 60 nm，NaCl 1000 mg/L，Na2SO4 1000 mg/L，铬黑T 50 mg/L)

Fig.5 Effect of TiO2 content on permeance and rejection (TiO2 60 nm，NaCl 1000 mg/L, Na2SO4 1000 mg/L, Eriochrome black T 50 mg/L)

图6 GO/TiO2复合膜的电镜图

Fig.6 SEM images of GO/TiO2 composite film

图7 GO/TiO2复合膜表征

Fig.7 Characterization of GO/TiO2 composite membrane

图8 不同染料的通量和截留(染料浓度 50 mg/L)

Fig.8 Permeance and rejection of different dyes (dye concentration 50 mg/L)

图9 GO/TiO2复合纳滤膜的截留分子量测定

Fig.9 MWCO measurement of GO/TiO2composite membrane

图10 GO/TiO2复合纳滤膜染料脱盐的示意图

Fig.10 Schematic diagram of dyes desalination for GO/TiO2 composite membrane

图11 长时间下GO/TiO2复合纳滤膜的分离性能

Fig.11 Long-term separation performance of GO/TiO2composite membrane

图12 盐浓度对渗透通量和截留的影响(染料浓度 50 mg/L)

Fig.12 Effect of salts concentration on permeance and rejection (dye concentration 50 mg/L)

图13 染料脱盐过程中铬黑T和盐的浓度变化

Fig.13 Changes in concentration of Eriochrome black T and salts during dye desalination

参考文献 34

1	Memon N A.Digital inkjet printing holds future potential[J].Pakistan Textile Journal,2012,10:36-37.
2	Xue C,Chen Q,Liu Y Y,et al.Acid blue 9 desalting using electrodialysis[J].Journal of Membrane Science,2015,493:28-36.
3	郝家春,占红武,龚振亮.基于FPGA的宽幅单PASS多喷头驱动研究[J].轻工机械,2014,32(2):16-19.
	Hao J C,Zhan H W,Gong Z L.Research of multi-jet drive with wide format and single-PASS based on FPGA[J].Light Industry Machinery,2014,32(2):16-19.
4	方彦彦,李倩,王晓琳.解读纳滤: 一种具有纳米尺度效应的分子分离操作[J].化学进展,2012,24(5):863-870.
	Fang Y Y,Li Q,Wang X L.Nanofiltration understanding: a separation process of molecular-level with nano-scale effect[J].Progress in Chemistry,2012,24(5):863-870.
5	陈慧娟,纪晓声,陈霄翔,等.纤维素/壳聚糖共混纳滤膜的制备及其染料脱盐性能研究[J].膜科学与技术,2018,38(4):27-32.
	Chen H J,Ji X S,Chen X X,et al.Preparation of CEL/CS blend nanofiltration membranes for dye desalination[J].Membrane Science and Technoloy,2018,38(4):27-32.
6	Xu Y Q,Lin J,Gao C,et al.Preparation of high-flux nanoporous solvent resistant PAN membrane with potential fractionation of dyes and Na₂SO₄[J].Industrial & Engineering Chemistry Research,2017,56(41):11967-11976.
7	Ye W,Lin J,Borrego R,et al.Advanced desalination of dye/NaCl mixures by a loose nanofiltration membrane for digital ink-jet printing[J].Separation & Purification Technology,2018,197:27-35.
8	Lin J,Ye W,Baltaru M C,et al.Tight ultrafiltration membranes for enhanced separation of dyes and Na₂SO₄ during textile wastewater treatment[J].Journal of Membrane Science,2016,514:217-228.
9	周丰,黄慧敏,钱飞跃,等.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 F,Huang H M,Qian F Y,et al.Effects of carbon nanotubes mats structure on rejection performance of composite membranes [J].CIESC Journal,2018,69(5):2318-2326.
10	Huang L,Huang S T,Venna S R,et al.Rightsizing nanochannels in reduced graphene oxide membranes by solvating for dye desalination[J].Environmental Science & Technology,2018,52(21):12649-12655.
11	Xu Y Q,Wu M Y,Yu S Y,et al.Ultrathin and stable graphene oxide filmviaintercalation polymerization of polydopamine for preparation of digital inkjet printing dye[J].Journal of Membrane Science,2019,586:15-22.
12	陶文,严晓菊,霍璐,等.硼酸盐交联的层层自组装氧化石墨烯膜的研究[J].当代化工,2019,48(8):1642-1644.
	Tao W,Yan X J,Huo L,et al.Research on layer-by-layer self-assembled graphene oxide films crosslinked by borate[J].Contemporary Chemical Industry,2019,48(8):1642-1644.
13	张润楠,李亚飞,苏延磊,等.氨基化氧化石墨烯界面聚合制备超薄复合纳滤膜[J].化工学报,2018,69(1):435-445.
	Zhang R N,Li Y F,Su Y L,et al.Preparation of thin-film composite nanofiltration membranes with amino-functionalized graphene oxide by interfacial polymerization[J].CIESC Journal,2018,69(1):435-445.
14	Liu G P,Jin W Q.Graphene oxide membrane for molecular separation: challenges and opportunities[J].Science China Materials,2018,61(8):1021-1026.
15	刘阳,顾平,张光辉.氧化石墨烯分离膜的制备及其水处理领域的应用进展[J].化工进展,2017,36(11):230-238.
	Liu Y,Gu P,Zhang G H.Fabrication of graphene oxide-assisted membranes and its applications in water treatment and purification[J].Chemical Industry and Engineering Progress,2017,36(11):230-238.
16	Huang H,Song Z,Wei N,et al.Ultrafast viscous water flow through nanostrand-channelled graphene oxide membranes[J].Nature Communications,2013,4(2979):1-9.
17	Wang X L,Zhang C H,Ouyang P.The possibility of separating saccharides from a NaCl solution by using nanofiltration in diafiltration mode[J].Journal of Membrane Science,2002,204:271-281.
18	Lui C H,Liu L,Mak K F,et al.Ultraflat graphene[J].Nature,2009,462:339-341.
19	Ferrari A C,Meyer J C,Scardaci V,et al.Raman spectrum of graphene and graphene layers[J].Physical Review Letters,2006,97(18):187401.
20	Krishnamoorthy K,Veerapandian M,Yun K,et al.The chemical and structural analysis of graphene oxide with different degrees of oxidation [J].Carbon,2013,53:38-49.
21	Wei G.The Chemistry of graphene oxide[J].Chemical Society Reviews,2009,39:228-240.
22	Akbari A,Sheath P,Shinde D B,et al.Large-area graphene-based nanofiltration membranes by shear alignment of discotic nematic liquid crystals of graphene oxide[J].Nature Communications,2016,7(10891):1-12.
23	Stobinski L,Lesiak B,Malolepszy A,et al.Graphene oxide and reduced graphene oxide studied by the XRD, TEM and electron spectroscopy methods[J].Journal of Electron Spectroscopy & Related Phenomena,2014,195:145-154.
24	Wei Y,Zhang Y,Gao X,et al.Declining flux and narrowing nanochannels under wrinkles of compacted graphene oxide nanofiltration membranes[J].Carbon,2016,108:568-575.
25	Qiu,R Y,Xiao J,Dong X,et al.The effects of edge functional groups on water transport in graphene oxide membranes[J].Applied Materials & Interfaces,2019,11(8):8483-8491.
26	Yu S,Gao C,Su H,et al.Nanofiltration used for desalination and concentration in dye production[J].Desalination,2001,140(1):97-100.
27	Mohammad A W,Teow Y H,Ang W L,et al.Nanofiltration membranes review: recent advances and future prospects[J].Desalination,2015,356:226-254.
28	Yi H,Jiang Y,Chao G.High-flux graphene oxide nanofiltration membrane intercalated by carbon nanotubes[J].Applied Materials & Interfaces,2015,7(15):8147-8155.
29	Childress A E,Elimelech M.Relating nanofiltration membrane performance to membrane charge (electrokinetic) characteristics[J].Environmental Science & Technology,2000,34(17):3710-3716.
30	Nilsson M,Trägårdh G,Östergren K.The influence of pH, salt and temperature on nanofiltration performance [J].Journal of Membrane Science,2008,312:97-106.
31	Freger V,Arnot T C,Howell J A.Separation of concentrated organic/inorganic salt mixtures by nanofiltration [J].Journal of Membrane Science,2000,178:185-193.
32	Lin J,Tang C Y,Ye W,et al.Unraveling flux behavior of superhydrophilic loose nanofiltration membranes during textile wastewater treatment[J].Journal of Membrane Science,2015,493:690-702.
33	Fikar M,Kovács Z,Czermak P.Dynamic optimization of batch diafiltration processes[J].Journal of Membrane Science,2010,355:168-174.
34	Bowen W R,Mohammad A W.Diafiltration by nanofiltration: prediction and optimization[J].AIChE Journal,1998,44(8):1799-1812.

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用于喷墨印花染料纯化的自组装GO/TiO₂复合纳滤膜的制备

Preparation of self-assembled graphene oxide / nano TiO₂ composite nanofiltration membrane for inkjet printing dye

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