Reinforcement of C-NFO@GDY Membranes via the Synergistic Effect of the Graphdiyne Honeycomb Nanostructure and Electronegativity for High-Efficiency Oil-in-Water Emulsion Separation

Yanchun Pei , Xueyan Wu , Zhichao Ren , Yan Lv , Rui Xue , Jixi Guo , Dianzeng Jia

Advanced Fiber Materials ›› 2025, Vol. 7 ›› Issue (4) : 1195 -1207.

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Advanced Fiber Materials ›› 2025, Vol. 7 ›› Issue (4) : 1195 -1207. DOI: 10.1007/s42765-025-00549-2
Research Article
research-article

Reinforcement of C-NFO@GDY Membranes via the Synergistic Effect of the Graphdiyne Honeycomb Nanostructure and Electronegativity for High-Efficiency Oil-in-Water Emulsion Separation

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Abstract

Electrospun fiber membranes enable oil–water emulsion separation via tunable morphology and chemistry, yet most face an efficiency–permeability trade-off where enhancing one compromises the other. Herein, optimized membranes (C-NFO@GDY) are synthesized with a uniform honeycomb nanostructure of graphdiyne (GDY) on flexible coal-based preoxidized fibers (C-NFO) through the Glaser‒Hay coupling reaction. The honeycomb nanostructure of GDY effectively disperses external stress on the C-NFO fibers, increasing the tensile strength from 2.8 to 3.2 MPa. In addition, the nanostructure enhances hydration layer formation kinetics, achieving superhydrophilicity (0°) and underwater superoleophobicity (> 150°) of the membrane. When tested against three surfactant-stabilized emulsions (cetyltrimethylammonium bromide (CTAB), sodium dodecyl sulfate (SDS), and polyoxyethylene sorbitan monooleate (Tween 80)), the membranes demonstrated separation fluxes of 2936 L/(m2 h), 2149 L/(m2 h), and 1855 L/(m2 h), and the corresponding separation efficiencies were 99.6%, 96.6%, and 93.1%. For CTAB-stabilized emulsions, the C-NFO@GDY membrane (zeta potential: − 65.2 mV) exhibits strong electrostatic attraction with cationic surfactants, achieving a high flux of 2936 L/(m2 h) and a separation efficiency of 99.6%, surpassing those of recently reported MXene and PANI composites under identical conditions. Overall, the synergy between honeycomb nanostructure and electronegativity of GDY overcomes the flux–efficiency trade-off, offering new ideas for the preparation of oil–water separation membranes.

Keywords

Coal-based fiber membrane / Graphdiyne / Honeycomb nanostructure / Underwater superoleophobicity / Emulsion separation

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Yanchun Pei, Xueyan Wu, Zhichao Ren, Yan Lv, Rui Xue, Jixi Guo, Dianzeng Jia. Reinforcement of C-NFO@GDY Membranes via the Synergistic Effect of the Graphdiyne Honeycomb Nanostructure and Electronegativity for High-Efficiency Oil-in-Water Emulsion Separation. Advanced Fiber Materials, 2025, 7(4): 1195-1207 DOI:10.1007/s42765-025-00549-2

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References

[1]

LiMH, BaiL, JiangST, MikaS, HuangYP, LiuYB. Electrocatalytic transformation of oxygen to hydroxyl radicals via three-electron pathway using nitrogen-doped carbon nanotube-encapsulated nickel nanocatalysts for effective organic decontamination. J Hazard Mater, 2023, 452131352

[2]

LiC, RenLP, ZhangCH, XuWL, LiuX. TiO2 coated polypropylene membrane by atomic layer deposition for oil–water mixture separation. Adv Fiber Mater, 2021, 3138

[3]

JiangST, FangJ, LiuHY, TangXY, ZhuHY, ZongEM, CaiYT, ZhaoZT, CuoJB, LiuYB. Bioelectricity-driven, sulfurized Fe species anode in situ generate sulfate radicals from sulfates in antibiotic wastewater for enhanced ciprofloxacin hydrochloride removal: Performance and mechanism. Chem Eng J, 2024, 502157745

[4]

ZhuYQ, DuanGG, WuWJ, LiuYB, ZengSY, ZengSY, YangHQ, HanXS, HeSJ, ZhangCM, HanJQ, JiangSH. Ultrafast and energy-efficient flowthrough capture of antibiotics through a reusable MOF @ wood membrane adsorbent. J Membr Sci, 2025, 714123411

[5]

NurulSF, NurHO, NurHA, FauziahM, MohdHDO, AhmadFI, WoeiJL, KangL, TutukDK, IzumiI, MohammadMAS. A review on photothermal material and its usage in the development of photothermal membrane for sustainable clean water production. Desalination, 2021, 517115259

[6]

CaiDL, MaPC. Electrospun polyacrylonitrile membrane in situ modified with cellulose nanocrystal anchoring TiO2 for oily wastewater recovery. Adv Fiber Mater, 2023, 52023

[7]

LuXC, ShenLG, LinHJ, HanL, DuJR, ChenC, TengJH, LiBS, YuW, XuYC. An efficient solution based on the synergistic effects of nickel foam in NiFe-LDH nanosheets for oil/water separation. J Hazard Mater, 2024, 469133973

[8]

SanjayR, NagarajanP, SabyasachiG, SubhadipM, SuryasarathiB, NarayanCD. Porous graphene-based membranes: preparation and properties of a unique two-dimensional nanomaterial membrane for water purification. Sep Purif Rev, 2021, 262282

[9]

XueJJ, WuT, DaiYQ, XiaYN. Electrospinning and electrospun nanofibers: methods, materials, and applications. Chem Rev, 2019, 1195298

[10]

WangD, YangHY, WangQX, LuJ, YanJ, ChengWL, RojasOJ, HanGP. Composite membranes of polyacrylonitrile cross-linked with cellulose nanocrystals for emulsion separation and regeneration. Compos Part A, 2023, 164107300

[11]

SuY, FanTT, CuiWY, LiYA, RamakrishnaS, LongYZ. Advanced electrospun nanofibrous materials for efficient oil/water separation. Adv Fiber Mater, 2022, 4938

[12]

GeJL, ZongDD, JinQ, YuJY, DingB. Biomimetic and superwettable nanofibrous skins for highly efficient separation of oil-in-water emulsions. Adv Funct Mater, 2018, 281705051

[13]

LiH, ZhangJQ, ZhuL, LiuHL, YuSF, XueJW, ZhuX. Reusable membrane with multifunctional skin layer for effective removal of insoluble emulsified oils and soluble dyes. J Hazard Mater, 2021, 415125677

[14]

WangR, ShiMS, XuFY, QiuY, ZhangP, ShenKL, ZhaoQ, YuJG, ZhangYF. Graphdiyne-modified TiO2 nanofibers with osteoinductive and enhanced photocatalytic antibacterial activities to prevent implant infection. Nat Commun, 2020, 114465

[15]

KhanK, TareenAK, IqbalM, ShiZ, ZhangH, GuoZY. Novel emerging graphdiyne based two dimensional materials: synthesis, properties and renewable energy applications. Nano Today, 2021, 39101207

[16]

GaoX, ZhouJY, DuR, XieZQ, DengSB, LiuR, LiuZF, ZhangJ. Robust superhydrophobic foam: a graphdiyne-based hierarchical architecture for oil/water separation. Adv Mater, 2016, 28168

[17]

LiXD, WangN, HeJJ, YangZ, ZhaoFH, WangK, HuangCS. One-step preparation of highly durable superhydrophobic carbon nanothorn arrays. Small, 2020, 161907013

[18]

ZhouJY, GaoX, LiuR, XieZQ, YangJ, ZhangSQ, ZhangGM, LiuHB, LiYL, ZhangJ, LiuZF. Synthesis of graphdiyne nanowalls using acetylenic coupling reaction. J Am Chem Soc, 2015, 1377596

[19]

MatsuokaR, SakamotoR, HoshikoK, SasakiS, MasunagaH, NagashioK, NishiharaH. Crystalline graphdiyne nanosheets produced at a gas/liquid or liquid/liquid interface. J Am Chem Soc, 2017, 1393145

[20]

ChenHL, LiuX, GongD, ChangZ, LiuGJ, FanJR, WuP, LiZ, PanYC, ShiGS, SunYH, ZengGF. Ultrahigh-water-flux desalination on graphdiyne membranes. Nat Water, 2023, 1800

[21]

LvY, WuXY, LinH, LiJX, ZhangHB, GuoJX, JiaDZ, ZhangHM. A novel carbon support: few-layered graphdiyne decorated carbon nanotubes capture metal clusters as effective metal-supported catalysts. Small, 2021, 172006442

[22]

LiangN, WuXY, LvY, GuoJX, ZhangXL, ZhuYF, LiuHB, JiaDZ. A graphdiyne oxide composite membrane for active electrolyte enhanced supercapacitors with super long self-discharge time. J Mater Chem C, 2022, 102821

[23]

LvY, WuXY, JiaW, GuoJX, ZhangHB, LiuHB, JiaDZ, ZhangHM, TongFL. Graphdiyne-anchored ultrafine NiFe hydroxide nanodots electrocatalyst for water oxidation with high mass activity and superior durability. Carbon, 2020, 16945

[24]

JiaSJ, WuJL, RanL, YangWS, DuanGG, YangHQ, ShiFS, ChenYH, HuJP, JiangSH. Electrospun nanofibers membranes of La (OH)3/PAN as a versatile adsorbent for fluoride remediation: performance and mechanisms. E-Polymers, 2024, 2420240083

[25]

WangDD, HuangLK, FangHX, LiSF, WangGZ, ZhouSM, ZhaoR, SunXY. Activated carbon fibers functionalized with superhydrophilic coated PDA/TiO2/SiO2 with photoluminescent self-cleaning properties for efficient oil–water separation. J Hazard Mater, 2024, 465133373

[26]

LiangN, WuXY, ZhangXL, LvY, GuoJX, GuoRH, ZhuYF, LiuHB, JiaDZ. A graphdiyne based separator toward high performance activated electrolyte-enhanced supercapacitors. J Mater Chem A, 2024, 124695

[27]

OhSB, BangJ, JinHJ, KwakHW. Green fabrication of underwater superoleophobic biopolymeric nanofibrous membranes for effective oil–water separation. Adv Fiber Mater, 2023, 5603

[28]

ZhengLJ, WuXD, LouZ, WuD. Superhydrophobicity from microstructured surface. Chin Sci Bull, 2004, 491779

[29]

GaoXF, JiangL. Water-repellent legs of water striders. Nature, 2004, 43236

[30]

WangYW, MengFX, HanL, LiuXY, GuoF, LuH, ChengDH, WangWB. Constructing a highly tough, durable, and renewable flexible filter by epitaxial growth of a glass fiber fabric for high flux and superefficient oil–water separation. J Hazard Mater, 2023, 448130807

[31]

LiuYH, BaiTB, ZhaoSX, ZhangZL, FengMJ, ZhangJB, LiDM, FengLB. Sugarcane-based superhydrophilic and underwater superoleophobic membrane for efficient oil-in-water emulsions separation. J Hazard Mater, 2024, 461132551

[32]

LiSH, HuangJY, ChenZ, ChenGQ, LaiYK. A review on special wettability textiles: theoretical models, fabrication technologies and multifunctional applications. J Mater Chem A, 2017, 531

[33]

ZengQQ, ZhouXL, ShenLG, ZhaoDL, KongN, LiYB, QiuXF, ChenC, TengJH, XuYC, LinHJ. Exceptional self-cleaning MXene-based membrane for highly efficient oil/water separation. J Membr Sci, 2024, 700122691

[34]

SuHW, HuH, LiZY, YanGL, WangL, XiangD, ZhaoCX, WuYP, ChenJY, WangC. Pre-oxidized PAN nanofibrous membrane to efficiently and continuously separate large-scale viscous oil-in-water emulsions under harsh conditions with ultra-long-term oil-fouling recovery. Adv Fiber Mater, 2023, 6852

[35]

LiZK, ZhangTC, MokobaT, YuanS. Superwetting Bi2MoO6/Cu3(PO4)2 nanosheet-coated copper mesh with superior anti-oil-fouling and photo-fenton-like catalytic properties for effective oil-in-water emulsion separation. Acs Appl Mater Interfaces, 2021, 1323662

[36]

YangYX, DongJS, WangR, LinZA, CaiZW. Urchin-like fluorinated covalent organic frameworks decorated fabric for effective self-cleaning and versatile oil/water separation. J Hazard Mater, 2023, 459132149

[37]

ZhangWB, ZhuYZ, LiuX, WangD, LiJY, JinJ. Salt-induced fabrication of superhydrophilic and underwater superoleophobic PAA-g-PVDF membranes for effective separation of oil-in-water emulsions. Angew Chem Int Ed, 2014, 53856

[38]

WangJ, MaXY, SuLY, ZhangCH, DongXF, TengC, JiangL, YuCM. Eco-friendly perforated kelp membrane with high strength for efficient oil/water separation in a complex environment. Sep Purif Technol, 2022, 282120114

[39]

TieL, GuoZ, LiuW. pH-manipulated underwater-oil adhesion wettability behavior on the micro/nanoscale semicircular structure and related thermodynamic analysis. ACS Appl Mater Interfaces, 2015, 710641

[40]

SuB, TianY, JiangL. Bioinspired interfaces with superwettability: from materials to chemistry. J Am Chem Soc, 2016, 1381727

[41]

ZhangWF, LiXY, QuRX, LiuYN, WeiY, FengL. Janus membrane decorated via a versatile immersion-spray route: controllable stabilized oil/water emulsion separation satisfying industrial emission and purification criteria. J Mater Chem A, 2019, 74941

[42]

KocherginskyNM, TanCL, LuWF. Demulsification of water-in-oil emulsions via filtration through a hydrophilic polymer membrane. J Membr Sci, 2003, 220117

[43]

LiZQ, WangML, LiY, RenJM, PeiCH. Effect of cellulose nanocrystals on bacterial cellulose hydrogel for oil–water separation. Sep Purif Technol, 2023, 304122349

Funding

Innovative Research Group Project of the National Natural Science Foundation of China(U2003307)

Science and Technology Department of Xinjiang Uygur Autonomous Region(2022TSYCLJ0043)

RIGHTS & PERMISSIONS

Donghua University, Shanghai, China

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