Study of Dye Adsorption Properties of Cellulose-Based Nanocellulose Aerogels

doi:10.12141/j.issn.1000-565X.240587

Abstract

Abstract:

The issue of water pollution is becoming increasingly severe, highlighting the urgent need to develop efficient and sustainable methods for pollutant removal. This study proposed the use of ambient pressure drying to prepare a nanocellulose-based aerogel with high adsorption capacity for both anionic and cationic pollutants. Polyethyleneimine (PEI) was first attached to a carboxymethylated cellulose nanofiber (CNF) framework through electrostatic interactions. Then, γ-aminopropyltriethoxysilane (APTES) and glutaraldehyde (GA) were used for chemical crosslinking to form a hydrogel. Finally, through solvent exchange and ambient pressure drying, a low-density (18.80 mg/cm³) and high-porosity (92.06%) CNF/PEI composite aerogel (CPA) was obtained. This aerogel demonstrated excellent structural stability in water. Owing to the coexistence of anionic carboxymethyl and cationic amino groups, the aerogel exhibited strong adsorption capacity of aerogel per gram for both cationic and anionic dyes in complex wastewater environments. The maximum adsorption capacities of aerogel per gram for methylene blaue (MB) and Congo red (CR) were 516 mg and 2 090 mg, respectively,with removal rates of over 98% for both anionic and cationic dyes. In addition, the aerogel exhibited good structural stability and fatigue resistance. After soaking in an alkaline solution for a week, it remained intact, and after 10 cycles of compression in the wet state, its elasticity recovery rate remained at 60%. Compared to similar adsorption materials, CPA shows significant advantages in terms of adsorption capacity, amphoteric adsorption ability, and reusability. The preparation method proposed in this study is time-efficient and highly effective, making it suitable for large-scale production, with promising potential for application in industrial wastewater treatment.

Key words: nanocellulose, aerogel, surface modification, dye adsorption, water treatment technology

CLC Number:

TB34

CHEN Gang, AO Jie, HE Yingying, WANG Chunyu, ZHANG Cheng. Study of Dye Adsorption Properties of Cellulose-Based Nanocellulose Aerogels[J]. Journal of South China University of Technology(Natural Science Edition), 2025, 53(8): 149-157.

Figures/Tables 5

References 30

[1]	LIU Y， KE Y， SHANG Q，et al ．Fabrication of multifunctional biomass-based aerogel with 3D hierarchical porous structure from waste reed for the synergetic adsorption of dyes and heavy metal ions［J］．Chemical Engineering Journal，2023，451（3）：138934/1-15.
[2]	CHENG S， ZHAO S， XING B，et al ．Preparation of magnetic adsorbent-photocatalyst composites for dye removal by synergistic effect of adsorption and photocatalysis［J］．Journal of Cleaner Production，2022，348：131301/1-11.
[3]	QIAO A， CUI M， HUANG R，et al ．Advances in nanocellulose-based materials as adsorbents of heavy metals and dyes［J］．Carbohydrate Polymers，2021，272：11847/1-15.
[4]	GAO X， REN P， WANG J，et al ．Fabrication of visible-light responsive Tio 2 @c photocatalyst with an ultra-thin carbon layer to efficiently degrade organic pollutants［J］．Applied Surface Science，2020，532：147482/1-10.
[5]	WANG K， LIU X， TAN Y，et al ．Two-dimensional membrane and three-dimensional bulk aerogel materials via top-down wood nanotechnology for multibehavioral and reusable oil/water separation［J］．Chemical Engineering Journal，2019，371：769-780.
[6]	NASROLLAHZADEH M， SAJJADI M， IRAVANI S，et al ．Green-synthesized nanocatalysts and nanomate-rials for water treatment：current challenges and future perspectives［J］．Journal of Hazardous Materials，2021，401：123401/1-24.
[7]	刚恺悦，张宝浩，马宁，等．基于静电作用选择性吸附染料的超分子凝胶剂［J］．精细化工，2022，39（11）：2328-2336.
	GANG Kaiyue， ZHANG Baojie， MA Ning，et al ．Supramolecular gels for selective adsorption of dyes based on electrostatic interaction［J］．Fine Chemicals，2022，39（11）：2328-2336.
[8]	GUO J， ZHOU S， MA X，et al ．Regenerated cellulose/polyethyleneimine composite aerogel for efficient and selective adsorption of anionic dyes［J］．Separation and Purification Technology，2024，330：125480/1-14.
[9]	YU J， TIAN S， YAO A，et al ．Compressible polydopamine modified pomelo peel powder/poly（ethyleneimine）/k-carrageenan aerogel with pH-tunable charge for selective removal of anionic and cationic dyes［J］．Carbohydrate Polymers，2024，323：121377/1-17.
[10]	MA X， ZHAO S， TIAN Z，et al ．MOFs meet wood：reusable ragnetic hydrophilic composites toward efficient water treatment with super-high dye adsorption capacity at high dye concentration［J］．Chemical Engineering Journal，2022，446（1）：136851/1-9.
[11]	QIN W， LI M X， ZHANG Y，et al ．High capacity and selective adsorption of congo red by cellulose-based aerogel with mesoporous structure：adsorption properties and statistical data simulation［J］．International Journal of Biological Macromolecules，2024，259（1）：129137/1-15.
[12]	PARALE V G， KIM T， CHOI H，et al ．Mechanically strengthened aerogels through multiscale，multicompositional，and multidimensional approaches：a review［J］．Advanced Materials，2024，36（18）：2307772/1-47.
[13]	庄杰，徐朝阳．纤维素基气凝胶吸附性能的研究进展［J］．高分子材料科学与工程，2022，38（3）：144-150.
	ZHUANG Jie， XU Chaoyang ．Advances in the adsorption properties of cellulose-based aerogels［J］．Polymeric Materials Science and Engineering，2022，38（3）：144-150.
[14]	DAS R， LINDSTROM T， SHARMA P R，et al ．Nanocellulose for sustainable water purification［J］．Chemical Reviews，2022，122（9）：8936-9031.
[15]	欧阳志宇．戊二醛-聚乙烯亚胺/羧甲基壳聚糖荷电纳滤膜的制备及性能研究［D］．南京：南京理工大学，2019.
[16]	XU H， ZHANG Z， JIANG W，et al ．Multifunctional amphibious superhydrophilic-oleophobic cellulose nanofiber aerogels for oil and water purification［J］‍．Carbohydrate Polymers，2024，330：121774/1-12.
[17]	WANG Z， HE Y， WANG C，et al ．A moisture-absorbing cellulose nanofibril-based foam via ambient drying for high-performance dehumidification［J］．Chemical Engineering Journal，2024，486：150063/1-9.
[18]	WU N， YANG Y， WANG C，et al ．Ultrathin cellulose nanofiber assisted ambient-pressure-dried，ultralight，mechanically robust，multifunctional Mxene aerogels［J］．Advanced Materials，2023，35（1）：2207969/1-12.
[19]	HU X， ZHANG S， YANG B，et al ．Preparation of ambient-dried multifunctional cellulose aerogel by freeze-linking technique［J］．Chemical Engineering Journal，2023，477：147044/1-10.
[20]	李方，雷春发，陈港．基于抄纸法制备羧甲基改性高强纤维素膜及性能研究［J］．造纸科学与技术，2021，40（1）：23-28.
	LI Fang， LEI Chunfa， CHEN Gang ．Preparat-ion of carboxymethyl-modified high-strength cellulose membranes based on paper copying method and study of their properties［J］．Paper Science and Technology，2021，40（1）：23-28.
[21]	ZHU P， YU Z， SUN H，et al ．3D printed cellulose nanofiber aerogel scaffold with hierarchical porous structures for fast solar-driven atmospheric water harvesting［J］．Advanced Materials，2024，36（1）：2306653/1-9.
[22]	QIU C， LI Y， LIU H，et al ．A novel crosslinking strategy on functional cellulose-based aerogel for effective and selective removal of dye［J］．Chemical Engineering Journal，2023，463：142404/1-10.
[23]	LI D， SUN L， YANG L，et al ．Adsorption behavior and mechanism of modified pinus massoniana pollen microcarriers for extremely efficient and rapid adsorption of cationic methylene blue dye［J］．Journal of Hazar-dous Materials，2024，465：133308/1-15.
[24]	LOREVICE M V， CLARO P I C， ALEIXO N A，et al ．Designing 3D fractal morphology of eco-friendly nanocellulose-based composite aerogels for water remediation［J］．Chemical Engineering Journal，2023，462：142166/1-14.
[25]	LI B， ZHAO Y ．Facile synthesis and ultrastrong adsorption of a novel polyacrylamide-modified diatomite/cerium alginate hybrid aerogel for anionic dyes from aqueous environment［J］．International Journal of Biological Macromolecules，2023，253（5）：127114/1-14.
[26]	DU N， HUANG L， XIONG Y，et al ．Micro-mechanism insights into the adsorption of anionic dyes using quaternary ammonium-functionalised chitosan aerogels［J］．Carbohydrate Polymers，2023，313：120855/1-17.
[27]	ZENG X， ZHU J， ZHANG G，et al ．Molecular-level understanding on complexation-adsorption-degradation during the simultaneous removal of aqueous binary po-llutants by magnetic composite aerogels［J］．Chemical Engineering Journal，2023，468：143536/1-16.
[28]	LEE J， MATHUR S， SHEN S，et al ．MoSe₂ nanoflowers for highly efficient industrial wastewater treatment with zero discharge［J］．Advanced Science，2021，8（23）：2102857/1-8.
[29]	VARAMESH A， ABRAHAM B D， WANG H，et al ．Multifunctional fully biobased aerogels for water remediation：applications for dye and heavy metal adsorption and oil / water separation［J］．Journal of Hazardous Materials，2023，457：131824/1-18.
[30]	XIA N N， WU Q， BI S L ．Ultra efficient removal of heavy-metal ions and dyes using a novel cellulose-based three-dimensional network［J］．Cellulose，2024，31（6）：3747-3761.