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Smart Biobased Polymers and Composites: Current Challenges and Opportunities

A special issue of International Journal of Molecular Sciences (ISSN 1422-0067). This special issue belongs to the section "Materials Science".

Deadline for manuscript submissions: closed (31 July 2022) | Viewed by 29606

Special Issue Editor


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Guest Editor
1. Biorefining and Advanced Materials Research Centre, SRUC, Edinburgh EH9 3JG, UK
2. Enhanced Composites and Structures Center, School of Aerospace, Transport and Manufacturing, Cranfield University, Cranfield MK43 0AL, UK
Interests: biorefining, chemistry, nanotechnology, biomass, and waste; biomedical engineering; composites; sensors; manufacturing of functional materials; aerospace materials; nanomaterials; renewable energy; smart materials; surface engineering; water science and engineering; additive manufacturing of polymers and composites; multifunctional polymer composites and nanocomposites: self-healing, nanoelectronic materials; hydrogels; membranes; nanofiber; composites for extreme environments and manufacturing technology
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Special Issue Information

Dear Colleagues,

The 21st century poses vast challenges for researchers all around the globe, especially regarding the effective use of sustainable polymers and their materials for different applications. With this focus, sustainable polymers and composites from biorenewable sources are now rising as one of the most feasible alternatives to traditional synthetic polymers/materials for a variety of industrial applications.

This Special Issue of IJMS will cover the most recent advancements in the bio-based polymers and respective materials. Potential topics include, but are not limited to the following:

  • Biorefining and biorefineries
  • Biopolymers
  • Biocomposites; natural rubber
  • Biobased additives for polymers
  • Green chemicals precursors
  • Multifunctional or smart biobased polymers and composites
  • New insights into the sustainable polymers and their applications
  • Natural fiber-based polymers and composites
  • Polymer blends from natural resources
  • Rational design and understanding of sustainable polymers from different biorenewable resources
  • Synthesis and characterization of natural fiber-derived cellulosic materials (micro/nano)

Prof. Dr. Vijay Kumar Thakur
Guest Editor

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Keywords

  • analysis and characterization of bio-based polymers and composites
  • biomass
  • biodegradable polymers matrices
  • biodegradability
  • bio-based polymers and composites
  • bio-based resins
  • eco-friendly natural polymers
  • novel biocomposites
  • synthesis of bio-based polymers
  • sustainable materials

Published Papers (11 papers)

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Research

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15 pages, 3401 KiB  
Article
Effect of Transglutaminase Post-Treatment on the Stability and Swelling Behavior of Casein Micro-Particles
by Ronald Gebhardt, Sahel Khanna, Jann Schulte and Md Asaduzzaman
Int. J. Mol. Sci. 2022, 23(19), 11837; https://doi.org/10.3390/ijms231911837 - 05 Oct 2022
Cited by 4 | Viewed by 1865
Abstract
Casein microparticles are produced by flocculation of casein micelles due to volume exclusion of pectin and subsequent stabilization by film drying. Transglutaminase post-treatment alters their stability, swelling behavior, and internal structure. Untreated particles sediment due to their size and disintegrate completely after the [...] Read more.
Casein microparticles are produced by flocculation of casein micelles due to volume exclusion of pectin and subsequent stabilization by film drying. Transglutaminase post-treatment alters their stability, swelling behavior, and internal structure. Untreated particles sediment due to their size and disintegrate completely after the addition of sodium dodecyl sulfate. The fact that transglutaminase-treated microparticles only sediment at comparable rates under these conditions shows that their structural integrity is not lost due to the detergent. Transglutaminase-treated particles reach an equilibrium final size after swelling instead of decomposing completely. By choosing long treatment times, swelling can also be completely suppressed as experiments at pH 11 show. In addition, deswelling effects also occur within the swelling curves, which enhance with increasing transglutaminase treatment time and are ascribed to the elastic network of cross-linked caseins. We propose a structural model for transglutaminase-treated microparticles consisting of a core of uncross-linked and a shell of cross-linked caseins. A dynamic model describes all swelling curves by considering both casein fractions in parallel. The characteristic correlation length of the internal structure of swollen casein microparticles is pH-independent and decreases with increasing transglutaminase treatment time, as observed also for the equilibrium swelling value of uncross-linked caseins. Full article
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24 pages, 18870 KiB  
Article
Formulation of Magneto-Responsive Hydrogels from Dually Cross-Linked Polysaccharides: Synthesis, Tuning and Evaluation of Rheological Properties
by Lenka Vítková, Lenka Musilová, Eva Achbergerová, Roman Kolařík, Miroslav Mrlík, Kateřina Korpasová, Leona Mahelová, Zdenka Capáková and Aleš Mráček
Int. J. Mol. Sci. 2022, 23(17), 9633; https://doi.org/10.3390/ijms23179633 - 25 Aug 2022
Cited by 7 | Viewed by 1741
Abstract
Smart hydrogels based on natural polymers present an opportunity to fabricate responsive scaffolds that provide an immediate and reversible reaction to a given stimulus. Modulation of mechanical characteristics is especially interesting in myocyte cultivation, and can be achieved by magnetically controlled stiffening. Here, [...] Read more.
Smart hydrogels based on natural polymers present an opportunity to fabricate responsive scaffolds that provide an immediate and reversible reaction to a given stimulus. Modulation of mechanical characteristics is especially interesting in myocyte cultivation, and can be achieved by magnetically controlled stiffening. Here, hyaluronan hydrogels with carbonyl iron particles as a magnetic filler are prepared in a low-toxicity process. Desired mechanical behaviour is achieved using a combination of two cross-linking routes—dynamic Schiff base linkages and ionic cross-linking. We found that gelation time is greatly affected by polymer chain conformation. This factor can surpass the influence of the number of reactive sites, shortening gelation from 5 h to 20 min. Ionic cross-linking efficiency increased with the number of carboxyl groups and led to the storage modulus reaching 103 Pa compared to 101 Pa–102 Pa for gels cross-linked with only Schiff bases. Furthermore, the ability of magnetic particles to induce significant stiffening of the hydrogel through the magnetorheological effect is confirmed, as a 103-times higher storage modulus is achieved in an external magnetic field of 842 kA·m1. Finally, cytotoxicity testing confirms the ability to produce hydrogels that provide over 75% relative cell viability. Therefore, dual cross-linked hyaluronan-based magneto-responsive hydrogels present a potential material for on-demand mechanically tunable scaffolds usable in myocyte cultivation. Full article
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17 pages, 4497 KiB  
Article
Maleic Anhydride-Grafted PLA Preparation and Characteristics of Compatibilized PLA/PBSeT Blend Films
by Hyunho Jang, Sangwoo Kwon, Sun Jong Kim and Su-il Park
Int. J. Mol. Sci. 2022, 23(13), 7166; https://doi.org/10.3390/ijms23137166 - 28 Jun 2022
Cited by 10 | Viewed by 2733
Abstract
Poly(butylene sebacate-co-terephthalate) (PBSeT) is a biodegradable flexible polymer suitable for melt blending with other biodegradable polymers. Melt blending with a compatibilizer is a common strategy for increasing miscibility between polymers. In this study, PBSeT polyester was synthesized, and poly(lactic acid) (PLA) was blended [...] Read more.
Poly(butylene sebacate-co-terephthalate) (PBSeT) is a biodegradable flexible polymer suitable for melt blending with other biodegradable polymers. Melt blending with a compatibilizer is a common strategy for increasing miscibility between polymers. In this study, PBSeT polyester was synthesized, and poly(lactic acid) (PLA) was blended with 25 wt% PBSeT by melt processing with 3–6 phr PLA-grafted maleic anhydride (PLA-g-MAH) compatibilizers. PLA-g-MAH enhanced the interfacial adhesion of the PLA/PBSeT blend, and their mechanical and morphological properties confirmed that the miscibility also increased. Adding more than 6 phr of PLA-g-MAH significantly improved the mechanical properties and accelerated the cold crystallization of the PLA/PBSeT blends. Furthermore, the thermal stabilities of the blends with PLA-g-MAH were slightly enhanced. PLA/PBSeT blends with and without PLA-g-MAH were not significantly different after 120 h, whereas all blends showed a more facilitated hydrolytic degradation rate than neat PLA. These findings indicate that PLA-g-MAH effectively improves PLA/PBSeT compatibility and can be applied in the packaging industry. Full article
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13 pages, 2435 KiB  
Article
A Novel Method of Endotoxins Removal from Chitosan Hydrogel as a Potential Bioink Component Obtained by CO2 Saturation
by Adrianna Banach-Kopeć, Szymon Mania, Joanna Pilch, Ewa Augustin, Iwona Gabriel and Robert Tylingo
Int. J. Mol. Sci. 2022, 23(10), 5505; https://doi.org/10.3390/ijms23105505 - 14 May 2022
Cited by 3 | Viewed by 2039
Abstract
The article presents a new approach in the purification of chitosan (CS) hydrogel in order to remove a significant amount of endotoxins without changing its molecular weight and viscosity. Two variants of the method used to purify CS hydrogels from endotoxins were investigated [...] Read more.
The article presents a new approach in the purification of chitosan (CS) hydrogel in order to remove a significant amount of endotoxins without changing its molecular weight and viscosity. Two variants of the method used to purify CS hydrogels from endotoxins were investigated using the PyroGene rFC Enzymatic Cascade assay kit. The effect of the CS purification method was assessed in terms of changes in the dynamic viscosity of its hydrogels, the molecular weight of the polymer, microbiological purity after refrigerated storage and cytotoxicity against L929 cells based on the ISO 10993-5:2009(E) standard. The proposed purification method 1 (M1) allows for the removal of significant amounts of endotoxins: 87.9–97.6% in relation to their initial concentration in the CS hydrogel without affecting the solution viscosity. Moreover, the final solutions were sterile and microbiologically stable during storage. The M1 purification method did not change the morphology of the L929 cells. Full article
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15 pages, 7623 KiB  
Article
Treatment of Critical Size Femoral Bone Defects with Biomimetic Hybrid Scaffolds of 3D Plotted Calcium Phosphate Cement and Mineralized Collagen Matrix
by Anna Carla Culla, Corina Vater, Xinggui Tian, Julia Bolte, Tilman Ahlfeld, Henriette Bretschneider, Alexander Pape, Stuart B. Goodman, Michael Gelinsky and Stefan Zwingenberger
Int. J. Mol. Sci. 2022, 23(6), 3400; https://doi.org/10.3390/ijms23063400 - 21 Mar 2022
Cited by 5 | Viewed by 3243
Abstract
To treat critical-size bone defects, composite materials and tissue-engineered bone grafts play important roles in bone repair materials. The purpose of this study was to investigate the bone regenerative potential of hybrid scaffolds consisting of macroporous calcium phosphate cement (CPC) and microporous mineralized [...] Read more.
To treat critical-size bone defects, composite materials and tissue-engineered bone grafts play important roles in bone repair materials. The purpose of this study was to investigate the bone regenerative potential of hybrid scaffolds consisting of macroporous calcium phosphate cement (CPC) and microporous mineralized collagen matrix (MCM). Hybrid scaffolds were synthetized by 3D plotting CPC and then filling with MCM (MCM-CPC group) and implanted into a 5 mm critical size femoral defect in rats. Defects left empty (control group) as well as defects treated with scaffolds made of CPC only (CPC group) and MCM only (MCM group) served as controls. Eight weeks after surgery, micro-computed tomography scans and histological analysis were performed to analyze the newly formed bone, the degree of defect healing and the activity of osteoclasts. Mechanical stability was tested by 3-point-bending of the explanted femora. Compared with the other groups, more newly formed bone was found within MCM-CPC scaffolds. The new bone tissue had a clamp-like structure which was fully connected to the hybrid scaffolds and thereby enhanced the biomechanical strength. Together, the biomimetic hybrid MCM-CPC scaffolds enhanced bone defect healing by improved osseointegration and their differentiated degradation provides spatial effects in the process of critical-bone defect healing. Full article
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23 pages, 9774 KiB  
Article
Characterization of a Novel Aspect of Tissue Scarring Following Experimental Spinal Cord Injury and the Implantation of Bioengineered Type-I Collagen Scaffolds in the Adult Rat: Involvement of Perineurial-like Cells?
by Haktan Altinova, Pascal Achenbach, Moniek Palm, Istvan Katona, Emmanuel Hermans, Hans Clusmann, Joachim Weis and Gary Anthony Brook
Int. J. Mol. Sci. 2022, 23(6), 3221; https://doi.org/10.3390/ijms23063221 - 16 Mar 2022
Cited by 1 | Viewed by 2151
Abstract
Numerous intervention strategies have been developed to promote functional tissue repair following experimental spinal cord injury (SCI), including the bridging of lesion-induced cystic cavities with bioengineered scaffolds. Integration between such implanted scaffolds and the lesioned host spinal cord is critical for supporting regenerative [...] Read more.
Numerous intervention strategies have been developed to promote functional tissue repair following experimental spinal cord injury (SCI), including the bridging of lesion-induced cystic cavities with bioengineered scaffolds. Integration between such implanted scaffolds and the lesioned host spinal cord is critical for supporting regenerative growth, but only moderate-to-low degrees of success have been reported. Light and electron microscopy were employed to better characterise the fibroadhesive scarring process taking place after implantation of a longitudinally microstructured type-I collagen scaffold into unilateral mid-cervical resection injuries of the adult rat spinal cord. At long survival times (10 weeks post-surgery), sheets of tightly packed cells (of uniform morphology) could be seen lining the inner surface of the repaired dura mater of lesion-only control animals, as well as forming a barrier along the implant–host interface of the scaffold-implanted animals. The highly uniform ultrastructural features of these scarring cells and their anatomical continuity with the local, reactive spinal nerve roots strongly suggest their identity to be perineurial-like cells. This novel aspect of the cellular composition of reactive spinal cord tissue highlights the increasingly complex nature of fibroadhesive scarring involved in traumatic injury, and particularly in response to the implantation of bioengineered collagen scaffolds. Full article
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25 pages, 4946 KiB  
Article
Cyprinus carpio Skeleton Byproduct as a Source of Collagen for Gelatin Preparation
by Robert Gál, Pavel Mokrejš, Jana Pavlačková and Dagmar Janáčová
Int. J. Mol. Sci. 2022, 23(6), 3164; https://doi.org/10.3390/ijms23063164 - 15 Mar 2022
Cited by 1 | Viewed by 2401
Abstract
Byproducts obtained from fish processing account for up to 70% of their live weight and represent a large amount of unused raw materials rich in proteins, fats, minerals, and vitamins. Recently, the management of the use of predominantly cold-water fish byproducts has become [...] Read more.
Byproducts obtained from fish processing account for up to 70% of their live weight and represent a large amount of unused raw materials rich in proteins, fats, minerals, and vitamins. Recently, the management of the use of predominantly cold-water fish byproducts has become a priority for many processing companies. This paper describes the biotechnological processing of byproducts of warm-water Cyprinus carpio skeletons into gelatins. A Taguchi experimental design with two process factors (HCl concentration during demineralization of the starting material and the amount of enzyme during enzyme conditioning of the collagen) examined at three levels (0.5, 1.0 and 2.0 wt%; 0.0, 0.1 and 0.2 wt% respectively) was used to optimize the processing of fish tissue into gelatin. Depending on the preparation conditions, four gelatin fractions were prepared by multi-stage extraction from the starting material with a total yield of 18.7–55.7%. Extensive characterization of the gel-forming and surface properties of the prepared gelatins was performed. Gelatins belong to the group of zero–low-medium Bloom value (0–170 Bloom) and low–medium viscosity (1.1–4.9 mPa·s) gelatins and are suitable for some food, pharmaceutical, and cosmetic applications. During processing, the pigment can be isolated; the remaining solid product can then be used in agriculture, and H3PO4Ca can be precipitated from the liquid byproduct after demineralization. The carp byproduct processing technology is environmentally friendly and meets the requirements of zero-waste technology. Full article
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17 pages, 1941 KiB  
Article
Oxidation of Various Kraft Lignins with a Bacterial Laccase Enzyme
by Sebastian A. Mayr, Raditya Subagia, Renate Weiss, Nikolaus Schwaiger, Hedda K. Weber, Johannes Leitner, Doris Ribitsch, Gibson S. Nyanhongo and Georg M. Guebitz
Int. J. Mol. Sci. 2021, 22(23), 13161; https://doi.org/10.3390/ijms222313161 - 06 Dec 2021
Cited by 12 | Viewed by 3287
Abstract
Modification of kraft lignin (KL), traditionally uses harsh and energy-demanding physical and chemical processes. In this study, the potential of the bacterial laccase CotA (spore coating protein A) for oxidation of KL under mild conditions was assessed. Thereby, the efficiency of CotA to [...] Read more.
Modification of kraft lignin (KL), traditionally uses harsh and energy-demanding physical and chemical processes. In this study, the potential of the bacterial laccase CotA (spore coating protein A) for oxidation of KL under mild conditions was assessed. Thereby, the efficiency of CotA to oxidize both softwood and hardwood KL of varying purity at alkaline conditions was examined. For the respective type of wood, the highest oxidation activity by CotA was determined for the medium ash content softwood KL (MA_S) and the medium ash content hardwood KL (MA_H), respectively. By an up to 95% decrease in fluorescence and up to 65% in phenol content coupling of the structural lignin units was indicated. These results correlated with an increase in viscosity and molecular weight, which increased nearly 2 and 20-fold for MA_H and about 1.3 and 6.0-fold for MA_S, respectively. Thus, this study confirms that the CotA laccase can oxidize a variety of KL at alkaline conditions, while the origin and purity of KL were found to have a major impact on the efficiency of oxidation. Under the herein tested conditions, it was observed that the MA_H KL showed the highest susceptibility to CotA oxidation when compared to the other hardwood KLs and the softwood KLs. Therefore, this could be a viable method to produce sustainable resins and adhesives. Full article
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22 pages, 7477 KiB  
Article
Lignin and Xylan as Interface Engineering Additives for Improved Environmental Durability of Sustainable Cellulose Nanopapers
by Sergejs Beluns, Oskars Platnieks, Sergejs Gaidukovs, Olesja Starkova, Alisa Sabalina, Liga Grase, Vijay Kumar Thakur and Gerda Gaidukova
Int. J. Mol. Sci. 2021, 22(23), 12939; https://doi.org/10.3390/ijms222312939 - 29 Nov 2021
Cited by 18 | Viewed by 2707
Abstract
Cellulose materials and products are frequently affected by environmental factors such as light, temperature, and humidity. Simulated UV irradiation, heat, and moisture exposure were comprehensively used to characterize changes in cellulose nanopaper (NP) tensile properties. For the preparation of NP, high-purity cellulose from [...] Read more.
Cellulose materials and products are frequently affected by environmental factors such as light, temperature, and humidity. Simulated UV irradiation, heat, and moisture exposure were comprehensively used to characterize changes in cellulose nanopaper (NP) tensile properties. For the preparation of NP, high-purity cellulose from old, unused filter paper waste was used. Lignin and xylan were used as sustainable green interface engineering modifiers for NP due to their structural compatibility, low price, nontoxic nature, and abundance as a by-product of biomass processing, as well as their ability to protect cellulose fibers from UV irradiation. Nanofibrillated cellulose (NFC) suspension was obtained by microfluidizing cellulose suspension, and NP was produced by casting films from water suspensions. The use of filler from 1 to 30 wt% significantly altered NP properties. All nanopapers were tested for their sensitivity to water humidity, which reduced mechanical properties from 10 to 40% depending on the saturation level. Xylan addition showed a significant increase in the specific elastic modulus and specific strength by 1.4- and 2.8-fold, respectively. Xylan-containing NPs had remarkable resistance to UV irradiation, retaining 50 to 90% of their initial properties. Lignin-modified NPs resulted in a decreased mechanical performance due to the particle structure of the filler and the agglomeration process, but it was compensated by good property retention and enhanced elongation. The UV oxidation process of the NP interface was studied with UV-Vis and FTIR spectroscopy, which showed that the degradation of lignin and xylan preserves a cellulose fiber structure. Scanning electron microscopy images revealed the structural formation of the interface and supplemented understanding of UV aging impact on the surface and penetration depth in the cross-section. The ability to overcome premature aging in environmental factors can significantly benefit the wide adaption of NP in food packaging and functional applications. Full article
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19 pages, 5557 KiB  
Article
A Comparison Study on the Magneto-Responsive Properties and Swelling Behaviors of a Polyacrylamide-Based Hydrogel Incorporating with Magnetic Particles
by Chanchan Xu, Bin Li and Xiaojie Wang
Int. J. Mol. Sci. 2021, 22(22), 12342; https://doi.org/10.3390/ijms222212342 - 15 Nov 2021
Cited by 3 | Viewed by 1852
Abstract
This work investigates the mechanical properties, microstructures, and water-swelling behavior of a novel hydrogel filled with magnetic particles. The nanoparticles of magnetite (Fe3O4) and the micro-particles of carbonyl iron (CI) were selected and filled into a polyacrylamide (PAAM) hydrogel [...] Read more.
This work investigates the mechanical properties, microstructures, and water-swelling behavior of a novel hydrogel filled with magnetic particles. The nanoparticles of magnetite (Fe3O4) and the micro-particles of carbonyl iron (CI) were selected and filled into a polyacrylamide (PAAM) hydrogel matrix to create two types of magnetic hydrogels. The isotropy and anisotropy of magnetic hydrogels are also presented in this study. The isotropic samples were cured without applying a magnetic field (MF), and the anisotropic samples were cured by applying an MF in the direction perpendicular to the thickness of the samples. The effects of the size, content, and inner structures of magnetic particles on the magneto-responsive and swelling properties of magnetic hydrogels were investigated. It was found that the magnetorheological (MR) effect of anisotropic samples was apparently higher than that of isotropic samples, and the hydrogels with CI exhibited a noticeable MR effect than those with Fe3O4. The storage modulus can be enhanced by increasing the filler content and size, forming an anisotropic structure, and applying an external MF. In addition, the magnetic hydrogels also have a swelling ability that can be tuned by varying the content and size of the particle fillers. Full article
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Review

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29 pages, 5964 KiB  
Review
Magnetic Fluorescent Quantum Dots Nanocomposites in Food Contaminants Analysis: Current Challenges and Opportunities
by Jincheng Xiong, Huixia Zhang, Linqian Qin, Shuai Zhang, Jiyue Cao and Haiyang Jiang
Int. J. Mol. Sci. 2022, 23(8), 4088; https://doi.org/10.3390/ijms23084088 - 07 Apr 2022
Cited by 16 | Viewed by 2995
Abstract
The presence of food contaminants can cause foodborne illnesses, posing a severe threat to human health. Therefore, a rapid, sensitive, and convenient method for monitoring food contaminants is eagerly needed. The complex matrix interferences of food samples and poor performance of existing sensing [...] Read more.
The presence of food contaminants can cause foodborne illnesses, posing a severe threat to human health. Therefore, a rapid, sensitive, and convenient method for monitoring food contaminants is eagerly needed. The complex matrix interferences of food samples and poor performance of existing sensing probes bring significant challenges to improving detection performances. Nanocomposites with multifunctional features provide a solution to these problems. The combination of the superior characteristics of magnetic nanoparticles (MNPs) and quantum dots (QDs) to fabricate magnetic fluorescent quantum dots (MNPs@QDs) nanocomposites are regarded as an ideal multifunctional probe for food contaminants analysis. The high-efficiency pretreatment and rapid fluorescence detection are concurrently integrated into one sensing platform using MNPs@QDs nanocomposites. In this review, the contemporary synthetic strategies to fabricate MNPs@QDs, including hetero-crystalline growth, template embedding, layer-by-layer assembly, microemulsion technique, and one-pot method, are described in detail, and their advantages and limitations are discussed. The recent advances of MNPs@QDs nanocomposites in detecting metal ions, foodborne pathogens, toxins, pesticides, antibiotics, and illegal additives are comprehensively introduced from the perspectives of modes and detection performances. The review ends with current challenges and opportunities in practical applications and prospects in food contaminants analysis, aiming to promote the enthusiasm for multifunctional sensing platform research. Full article
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