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Highlights • TFC membrane with an asymmetric separation layer was fabricated for nanofiltration. • The membrane was fabricated via IP process followed by secondary interface reaction. • High efficient nanofiltration of anionic dye aqueous solution was achieved. • Steady-state water flux was improved by at least 36.0%. • Steady-state flux decline was lowered by more than 23.5%. Abstract The development of high performance membrane is crucial for enhanced separation efficiency of nanofiltration process in treating wastewaters from dye and textile industries. In this work, a novel thin-film composite nanofiltration membrane with an asymmetric separation layer composed of relatively compact skin and loose body was designed and fabricated for improved perm-selectivity and antifouling property. Nascent composite membrane with loose poly(piperazine amide) (PA) separation layer was interfacially synthesized and performed with secondary surface reaction using an aqueous tannic acid (TA) solution. Membrane characterizations verified the formation of compact TA skin on top of the loose PA layer through forming covalent bonds via esterification reaction. Compared with the composite nanofiltration membrane with PA symmetric separation layer having the same glucose rejection of about 82.0%, the permeability to pure water of the composite membrane with PA/TA asymmetric separation layer was higher by 28.0%, the water fluxes to aqueous solutions dissolved with model anionic dyes of alizarin yellow R, sunset yellow and Congo red under steady state were higher by 50.3, 43.9 and 36.1%, and the steady-state flux declines were lowered by 27.8, 43.4 and 23.5%, respectively. Furthermore, the PA/TA-based membrane also exhibited better antifouling property and rejection ability to alizarin yellow R. [ABSTRACT FROM AUTHOR]

• Carbodiimide-assisted zwitterionic modification was performed with PA TFC membrane. • Irreversible depositions by dyes CR and VBB were lowered by 68.4 and 91.8 %. • Water permeabilities to CR and VBB aqueous solutions were enhanced by 62.3 and 95.2 %. • Permselectivity property was better than most of the reported zwitterionic membranes. • Separation performance to dye aqueous solutions was better than membrane NF270. In this work, a novel method of carbodiimide-assisted zwitterionic modification was proposed and implemented to incorporate zwitterionic moieties onto poly(piperazine amide) membrane for improved water permeability and anti-depositing property, which are crucial for highly efficient nanofiltration of dye-contained effluents. Carboxyl groups of polyamide layer were firstly transferred into N-acylurea using excess l-ethyl-3-(3-(dimethylamino)propyl)-carbodiimide. Zwitterions were then incorporated through ring-opening reaction between tertiary amine groups of N-acylurea and 1, 4-butanesultone. Carbodiimide-assisted zwitterionic modification was verified by ATR-IR and XPS analyses and was found to not affect membrane pore size but significantly enhance membrane's permeation and anti-dye-deposition performances. Compared with those of virgin membrane, water permeabilities of the desired zwitterionic membrane to pure water, Congo red aqueous solution and Victoria blue B aqueous solution were higher by 42.9, 62.3 and 95.2 %, respectively, hydraulic resistances from irreversible deposition of Congo red and Victoria blue B molecules were dramatically lowered by 68.4 and 91.8 %, respectively. Furthermore, the perm-selectivity performance of the desired zwitterionic membrane in terms of molecular weight cut-off and pure water permeability was better than most of the reported zwitterionic membranes, and the separation and anti-depositing performances to both anionic and cationic dye aqueous solutions were better than commercial membrane NF270. [ABSTRACT FROM AUTHOR]