Recent progress in electrospun nanofibers and their applications in heavy metal wastewater treatment

doi:10.1007/s11705-022-2245-0

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (3) : 249-275 https://doi.org/10.1007/s11705-022-2245-0

REVIEW ARTICLE

Recent progress in electrospun nanofibers and their applications in heavy metal wastewater treatment

Xizi Xu¹, He Lv¹, Mingxin Zhang¹, Menglong Wang¹, Yangjian Zhou¹, Yanan Liu¹(

), Deng-Guang Yu^1,²(

)

¹. School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai 200093, China
². Shanghai Engineering Technology Research Center for High-Performance Medical Device Materials, Shanghai 200093, China

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Abstract

Novel adsorbents with a simple preparation process and large capacity for removing highly toxic and nondegradable heavy metals from water have drawn the attention of researchers. Electrospun nanofiber membranes usually have the advantages of large specific surface areas and high porosity and allowing flexible control and easy functionalization. These membranes show remarkable application potential in the field of heavy metal wastewater treatment. In this paper, the electrospinning technologies, process types, and the structures and types of nanofibers that can be prepared are reviewed, and the relationships among process, structure and properties are discussed. On one hand, based on the different components of electrospun nanofibers, the use of organic, inorganic and organic−inorganic nanofiber membrane adsorbents in heavy metal wastewater treatment are introduced, and their advantages and future development are summarized and prospected. On the other hand, based on the microstructure and overall structure of the nanofiber membrane, the recent progresses of electrospun functional membranes for heavy metal removal are reviewed, and the advantages of different structures for applications are concluded. Overall, this study lays the foundation for future research aiming to provide more novel structured adsorbents.

Keywords electrospinning heavy metal adsorption nanostructure wastewater

Corresponding Author(s): Yanan Liu,Deng-Guang Yu

Online First Date: 30 December 2022 Issue Date: 17 March 2023

Cite this article:

Xizi Xu,He Lv,Mingxin Zhang, et al. Recent progress in electrospun nanofibers and their applications in heavy metal wastewater treatment[J]. Front. Chem. Sci. Eng., 2023, 17(3): 249-275.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2245-0
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I3/249

Fig.1 Statistics of literature retrieved on the “Web of Science” platform and the themes “heavy metal removal” and “electrospinning nanofibers for heavy metal removal” respectively.

Fig.2 Typical applications of electrospun nanofibers.

Fig.3 A diagram of electrospinning and its jet motion.

Fig.4 Influence parameters of the electrospinning process.

Fig.5 Single-fluid electrospinning process: (a) blending electrospinning, (b) multi-nozzle electrospinning, and (c) multi-layer electrospinning.

Fig.6 Types of multi-fluid electrospinning spinnerets.

Fig.7 Different structures of nanofibers prepared by electrospinning: (a) A homogeneous composite prepared using a handheld electrospinning [61]. (b) A hybrid nanostructure with nano drug crystals distributing on the surfaces of PAN nanofibers [62]. (c) Two parallel core–shell nanofibers [63]. (d) A Janus nanofiber with one side contains oil and the other side loading AgNPs [64]. (e) A tri-layer Janus nano structure containing “A”, “B” and “C” three different nanocomposites, the bottom-left inset shows the Taylor cone during preparation. Reprinted with permission from Ref. [65], copyright 2022, Springer Nature. (f) An organized bi-layer structure with one layer of nanofibers and the other layer of casting films for biphasic drug release [66].

Fig.8 Types of electrospun nanofiber membranes.

Tab.1 Advantages and disadvantages of different kinds of natural polymer fiber membranes

Fig.9 Different modified natural polymers nanofibers and their heavy metal ions adsorption capacity: (a) Schematic diagram of the preparation process of thiol-functionalized cellulose nanofiber membrane and its removal capacity for heavy metals Cu²⁺, Cd²⁺, and Pb²⁺. Reprinted with permission from Ref. [84], copyright 2020, Elsevier. (b) Preparation of CS-PGMA-PEI electrospun membrane and its application principle in water purification, and its removal ability and reusability of heavy metals Cr⁶⁺, Cu²⁺ and Co²⁺. Reprinted with permission from Ref. [85], copyright 2019, Elsevier.

Tab.2 Properties of the electrospun nanofiber membranes of single-component polymers for the adsorption of heavy metals

Fig.10 Effect on cross-linked PVA nanofibers: (a) schematic diagram of macroscopic and microscopic morphology of metal ions adsorbed by nanofibers before and after cross-linking; (b) effect of crosslinking time on tensile strength of PVA nanofiber films; (c) effect of crosslinking time on the contact angle of PVA nanofiber films. Reprinted with permission from Ref. [88], copyright 2019, Elsevier.

Material	Preparation method	Type of metal ions	Adsorption capacity	Ref.
PVA/CS	Blend electrospinning	Pb²⁺, Cd²⁺	266.12, 148.79 mg·g^–1	[106]
PAA/PVA	Blend electrospinning	Cu²⁺	49.3 mg·g^–1	[107]
PVA/PAA	Blend electrospinning	Pb²⁺, Cd²⁺	159, 102 mg·g^–1	[108]
PVA/PAN	Two-nozzle electrospinning and surface modification	Cr⁶⁺, Cd²⁺	66.5, 33.6 mg·g^–1	[109]
PVA/PEI	Blend electrospinning	Cr⁶⁺	150 mg·g^–1	[110]
PAN/CA	Hydrolysis and amidoximation modification	Fe³⁺, Cu²⁺, Cd²⁺	7.47, 4.26, 1.13 mmol·g^–1	[111]
PA-66/PAN	Twin-spinneret electrospinning and amidoxime modified	Cu²⁺, Pb²⁺	67.5, 75.4 mg·g^–1	[112]
CS/CA	Treatment by neutralization of CS and deacetylation of CA	As⁵⁺, Pb²⁺, Cu²⁺	39.4, 57.3, 112.6 mg·g^–1	[113]
CS/PEO (polyethylene oxide)	Diethylenetriaminepentaacetic acid-modified	Cu²⁺, Pb²⁺, Ni²⁺	177, 142, 56 mg·g^–1	[114]
CS/phosphorylated nanocellulose	Phosphate groups ( $P O 4 2 ?$ ) formed on the surface of electrospun nanofibers	Cd²⁺	232.55 mg·g^–1	[115]
PAN/PEI	Aminated PAN nanofibers followed by grafting branched PEI	Cu²⁺	149.8 mg·g^–1	[116]
SF/CA	Blend electrospinning and ethanol treatment	Cu²⁺	22.8 mg·g^–1	[117]
PVDF (polyvinylidene fluoride)/PAN	Treatment of electrospun PVDF/AOPAN nanofibers with KOH	Pb²⁺, Cu²⁺, Ni²⁺	72.5, 30.1, 52.8 mg·g^–1	[118]
PAN/PDA (polydopamine)	Coating PAN nanofibers with PDA	Cr⁶⁺	61.65 mg·g^–1	[89]
PLA/PDA/CS	CS-grafted porous P-PLLA (porous poly(L-lactic acid)) nanofiber by using PDA as an intermediate layer	Cu²⁺	270.27 mg·g^–1	[119]

Tab.3 Properties of electrospun multi-component nanofibers for heavy metals adsorption

Tab.4 Properties of electrospun inorganic nanofibers for heavy metals adsorption

Fig.11 Preparation and application of electrospun inorganic nanofibers: (a) Transmission electron microscope (TEM) photos of Al₂O₃?Fe₂O₃ mixed nano-composite fiber and its removal percentage and adsorption capacity changing with time (min) when adsorbing various metal ions. Reprinted with permission from Ref. [129], copyright 2013, Elsevier. (b) Preparation of ACNFs/MnO₂ nano-composite fiber and its removal efficiency and adsorption capacity at different Pb²⁺ concentrations. Reprinted with permission from Ref. [130], copyright 2020, Elsevier.

Fig.12 Functional composite nanofibers prepared by electrospinning combined with hydrothermal method and their application: (a) the schematic diagram of the preparation of b-PEI-FePAN nanofibers; (b) scanning electron microscopy images of pure PAN (Pannels I and II) and b-PEI-FePAN (Pannels III and IV) nanofibers; (c) removal performances of different adsorbents for Cr⁶⁺; (d) removal mechanism. Reprinted with permission from Ref. [147], copyright 2017, Elsevier.

Materials	Preparation method	Heavy metal ion	Adsorption capacity	Ref.
CS/TiO₂	Different doping forms of TiO₂: coating method and entrapped method	Pb²⁺, Cu²⁺	(1) 710.3, 579.1 mg·g^–1(2) 526.5, 475.5 mg·g^–1	[149]
CS/graphene oxide (GO)	Blending electrospinning	Cu²⁺, Pb²⁺, Cr⁶⁺	461.3, 423.8, 310.4 mg·g^–1	[150]
CS/HAp	Blending electrospinning	Pb²⁺, Ni²⁺, Co²⁺	296.7, 213.8, 180.2 mg·g^–1	[151]
CA/montmorillonite	Composite nanofibers with organically modified montmorillonite and followed by deacetylation	Cr⁶⁺	20 mg·g^–1	[152]
CA/HAp	Blending electrospinning	Fe³⁺, Pb²⁺	46.93, 45.825 mg·g^–1	[153]
PAN/FeCl₂	Blending electrospinning	Cr⁶⁺	108 mg·g^–1	[154]
PAN/MWCNTs (multiwalled carbon nanotubes)	PEI modified MWCNT as a novel additive in PAN nanofiber membrane	Pb²⁺, Cu²⁺	232.7, 112.5 mg·g^–1	[155]
PAN/ZIF-8 (zeolitic imidazolate framework-8)	ZIF-8 nanoparticles are uniformly decorated on PAN nanofibers by hot-pressing method	Cu²⁺	Cu²⁺ removal rate of ZIF-8/PAN NF can highly reach 34.1% in 4 min	[156]
PAN/ZnO	Blending electrospinning	Pb²⁺, Cd²⁺	322, 166 mg·g^–1	[157]
PAN/MgO	Coaxial electrospinning and post-treatment	Cu²⁺	354 mg·g^–1	[158]
PAN/boehmite	Combination of electrospinning process, chemical modification and hydrothermal reaction	Pb²⁺, Cu²⁺, Cd²⁺	180.83, 48.68, 114.94 mg·g^–1	[159]
PAN/CS/ZnO	Electrospun PAN nanofibrous membranes were functionalized with zinc oxide nanoparticles and coated with a layer of electrospun CS	Cr³⁺	116.5 mg·g^–1	[160]
PVA/SiO₂	Composite nanofibers were functionalized by mercapto groups via the hydrolysis polycondensation	Cu²⁺	489.12 mg·g^–1	[161]
PVA/zeolite	Blending electrospinning	Ni²⁺, Cd²⁺	342.8, 838.7 mg·g^–1	[162]
PVA/TiO₂/ZnO	Blending electrospinning	Th⁴⁺	333.3 mg·g^–1	[163]
PVA/clay and PCL (polycaprolactone)/clay	Blending electrospinning	Cd²⁺, Cr³⁺, Cu²⁺, Pb²⁺	14.58, 17.36, 16.46, 16.50 mg·g^–1 and 29.59, 27.23, 25.36, 32.88 mg·g^–1	[164]
PA-6/Mg(OH)₂	Electrospinning technique combined with hydrothermal strategy	Cr⁶⁺	296.4 mg·g^–1	[165]
PCL/clay/zeolite	Blending electrospinning	Pb²⁺	19.531 mg·g^–1	[166]
PEO/CS/AC	Blending electrospinning	Cr⁶⁺, Fe³⁺, Cu²⁺, Zn²⁺, Pb²⁺	261.1, 217.4, 195.3, 186.2, 176.9 mg·g^–1	[167]
CS/PVA/zeolite	Hydrolyzed CS solution was blended with PVA and zeolite	Cr⁶⁺, Fe³⁺, Ni²⁺	8.84, 6.16, 1.77 mg·g^–1	[168]
PVA/PAA/SiO₂	Blending electrospinning and crosslink through heat treatment	Cu²⁺	125.47 mg·g^–1	[169]
PE/PAA/PAH	Blending electrospinning and thermal crosslinking	Pb²⁺, Cd²⁺, Cu²⁺	70%, 98%, 92% romoval at pH 7.4	[170]
PVP/CeO₂/TMPTMS (3-mercaptopropyltrimethoxysilane)	Surface modification of CeO₂ and blending electrospinning	Pb²⁺, Cu²⁺	90.9, 88.3 mg·g^–1	[171]
PMMA (polymethylmethacrylate)/rhodanine	Blending electrospinning	Ag⁺, Pb²⁺	125.7, 140.2 mg·m^–2	[172]
PU/phytic acid	Blending electrospinning	Pb²⁺	136.52 mg·g^–1	[173]
Alginate/GO	Blending electrospinning	Pb²⁺	386.2 mg·g^–1	[174]

Tab.5 Properties of electrospun organic/inorganic composite nanofibers for the adsorption of heavy metals

Fig.13 Preparation of porous nanofibers by electrospinning: (a) one-step electrospinning (solvent-induced phase separation), (b) multi-step electrospinning method.

Fig.14 Founctional P-PLLA-based nanofibers and their application: (a) schematic representation showing the membrane sample preparation and metal ion absorption; (b) SEM image of P-PLLA nanofibers; (c) SEM images of P-PLLA/PDA-6 nanofibers; (d) SEM image of porous P-PLLA/PDA-6/CS nanofibers coated with PDA and grafted with CS; (e) adsorption capacity of Cu²⁺ at different concentrations; (f) adsorption capacity at different time. Reprinted with permission from Ref. [119], copyright 2021, Elsevier.

Fig.15 Influence of core–shell structure on the properties of nanofibers and their application: (a) the preparation method and TEM images of modified nylon-PAN/PANI core–shell nanofiber; (b) measurement of water contact angle of different fibers; (c) stress-strain curves of unmodified and modified membranes; (d) maximum adsorption capacities of Pb and Cd metal ions for unmodified and modified membranes. Reprinted with permission from Ref. [188], copyright 2018, Elsevier.

Fig.17 One-step synthesis of hollow hybrid nanofibers by electrospinning and their application: (a) schematic illustrations of the preparation of hollow Fe(OH)₃@cellulose hollow nanofiber membranes; (b) SEM (photoes I and II) and TEM (photo III) images of Fe(OH)₃@cellulose hollow nanofibers; (c) schematic illustration of the water permeation and pollutant adsorption process; (d) effect of pH values on the adsorption performance of Cr⁶⁺ by Fe(OH)₃@cellulose hollow nanofibers. Reprinted with permission from Ref. [195], copyright 2012, American Chemical Society.

Fig.18 A sandwich multilayer nanofiber membrane prepared by electrospinning and bioelectrospraying: the fabrication processes and synergistic effect of Saccharomyces cerevisiae layers and nanofiber layers for absorbing Zn²⁺ and Cd²⁺. Reprinted with permission from Ref. [198], copyright 2019, Elsevier.

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