Physical Entanglement Research Articles

Comprehensive Review of Hydrogel Synthesis, Characterization, and Emerging Applications

Hydrogels play a crucial role due to their high-water content and 3D structure, which make them ideal for various applications in biomedicine, sensing, and beyond. They can be prepared from a variety of biomaterials, polymers, and their combinations, allowing for versatility in properties and applications. Hydrogels include natural types derived from collagen, gelatin, alginate, and hyaluronic acid, as well as synthetic types based on polyethylene glycol (PEG), polyvinyl alcohol (PVA), and polyacrylamide (PAAm). Each type possesses distinct properties, such as mechanical strength, biodegradability, and biocompatibility, which can be tailored for applications such as wound healing, contact lenses, 3D bioprinting, and tissue engineering. The high-water content of hydrogels mimics natural tissue environments, promoting cell growth and allowing nutrient and waste exchange, which supports the development of functional tissues. They serve as scaffolds in tissue engineering applications, including wound healing, cartilage and bone regeneration, vascular tissue engineering, and organ-on-a-chip systems. Additionally, hydrogels can encapsulate and deliver therapeutic agents, such as growth factors or drugs, to specific target sites in the body. Hydrogels can be prepared through three primary methods: physical crosslinking, which relies on non-covalent interactions such as physical entanglements or hydrogen bonding; chemical crosslinking, which forms covalent bonds between polymer chains to create a stable structure; and irradiation-based crosslinking, where UV irradiation induces rapid hydrogel formation. The choice of crosslinking method depends on the desired properties and applications of the hydrogel. By providing a biomimetic environment, hydrogels facilitate cell growth and differentiation, support tissue formation, and aid in the regeneration of damaged or diseased tissues while delivering therapeutic agents. This review focuses on the critical advancements in processing routes for hydrogel development, summarizing the characterization and application of hydrogels. It also details key applications, including wound healing and cartilage and bone regeneration, as well as the challenges and future perspectives in the field.

Simultaneously enhancing the EMI shielding performances and mechanical properties of structure–function integrated CF/PEEK composites via chopped ultra-thin carbon fiber tapes and interfacial engineering with MXene

The functionalization of carbon fiber reinforced poly(ether-ether-ketone) (CF/PEEK) structural composites with high electromagnetic interference shielding efficiency (EMI SE) has important engineering application in the fields of aviation and aerospace. However, the simultaneous enhancement of interfacial properties and EMI SE in the CF/PEEK composite remains a significant concern. To address this issue, we have employed a continuous impregnation approach that involved synthesizing PFEEK as a binder and then utilizing mechanical spreading technology to prepare chopped ultra-thin CF tapes as the reinforcement phase. Subsequently, we deposited 2D MXene (Ti3C2Tx) on the CF tape surface to endow the interface properties and EMI SE for the CF/PEEK composites. As a result, when the MXene content was 1.0 mg/ml, the flexural strength, flexural modulus, and interlaminar shear strength (ILSS) of the obtained CF/PEEK composites achieved 17.6 %, 13.3 % and 36.6 % enhancement higher than that of the virgin CF/PEEK composites, respectively, which may be owing to the elevated interfacial properties via the hydrogen bonds, physical entanglement, π-π interactions, and mechanical interlocking with the incorporation of PFEEK and MXene. The optimal ILSS value and specific EMI SE/t value of the CF/PF-M1/PEEK composites can reach 113.7 MPa and 80.8 dB/mm, respectively. The enhancement in the EMI SE can be attributed to the enhancive reflection, the increased polarization losses, and multiple interlayer reflections of EM waves facilitated by the incorporation of MXene and multi ultra-thin CF/PF-MXene layers. This approach resulted in a structure–function integrated CF/PEEK composite, which holds promising application prospects across various cutting-edge domains.

Robust tetra-armed poly (ethylene glycol)-based hydrogel as tissue bioadhesive for the efficient repair of meniscus tears.

Repair and preservation of the injured meniscus has become paramount in clinical practice. However, the complexities of various clinic stitching techniques for meniscus repair pose challenges for grassroots doctors. Hence, there is a compelling interest in innovative therapeutic strategies such as bioadhesives. An ideal bioadhesive must cure quickly in aqueous and blood environments, bind strongly, endure arthroscopic washing pressures, and degrade appropriately for tissue regeneration. Here, we present a tetra-poly (ethylene glycol) (PEG)-based hydrogel bioadhesive, boasting high biocompatibility, ultrafast gelation, facile injectable operation, and favorable mechanical strength. In view of the synergistic effects of chemical anchor and physical chain entanglement to tightly bind the meniscus, a seamless interface was formed between the surrounding meniscal tissues and hydrogels, enabling the longitudinal tear of the meniscus fused in situ to withstand large tensile force with the adhesive strength of 541.5±31.4kPa and arthroscopic washout resistance of 29.4kPa. Superior to existing commercial adhesives, ours allows sutureless application and arthroscopic assistance, without requiring specialized clinical skills. This research is expected to significantly impact our understanding of meniscal healing and ultimately promote a simpler process for achieving functional and structural recovery in torn menisci.

Cross‐Scale Interface Engineering for Fabricating Super‐Strong and Super‐Tough Aramid nanofiber film

AbstractPoly (p‐phenylene terephthalamide) (PPTA), known for its exceptional mechanical properties under the brand name Kevlar, finds extensive use in high‐performance applications despite the challenges it presents in processing and integration with other materials. Existing top–down methods for preparing PPTA composites result in significantly reduced strength (<200 MPa) and toughness (<10 MJ·m−3) due to insufficient interfacial interactions, limiting their application. Here, a cross‐scale interface engineering strategy is reported for fabricating super‐strong and super‐tough PPTA composite films. At the microscale, a synergistic crosslinking strategy of physical entanglement and hydrogen bonding to crosslink PPTA nanofibers is employed. At the macroscale, the network using a cyclic freeze–thaw and the stretch‐drying method is reinforced. The PPTA nanofiber composite film is super‐strong (854.6 MPa), super‐tough (106.2 MJ·m−3), and has a high‐temperature resistance (300 °C). Moreover, the bottom–up approach enables the direct synthesis of PPTA nanofibers, significantly reducing the preparation time from 7 days to 0.5 h. Furthermore, it is demonstrated that the composite film can be integrated into a robust and intelligent sensing‐display device that responds to external mechanical and heat injuries for firefighter's protection. This work provides an efficient strategy for fabricating high‐performance PPTA composites, paving the way for their practical use as durable protective materials.

Balancing stretchability and conductivity: Carbon nanotube layer-enhanced non-ionic conductive hydrogels with a sandwich structure

In non-ionic conductive hydrogels, conductivity often conflicts with mechanical properties, posing a challenge in creating hydrogels that strike a balance between conductivity and mechanical properties. Here, we addressed this issue by integrating carboxylated carbon nanotube (CNT) layers in a sandwich structure onto the surface of the cationic hydrogel (P(AM-co-DMDAAC), PAD), followed by dehydration for densification. This approach simultaneously improved the conductivity of the hydrogel while maintaining its stretchability. The stability of the composite structure was ensured through electrostatic interactions, hydrogen bonding, and physical entanglement between the PAD hydrogel and the CNT layer. Additionally, adjusting the water–solid ratio of the hydrogel allows fine-tuning of its conductivity and stretchability. Remarkably, at a 500 % water–solid ratio, the hydrogel achieved a conductivity of 2.3 S/m. By further reducing the water content, the conductivity could be increased to 25 S/m, significantly higher than similar hydrogels. The PAD-CNT hydrogel found applications in swelling response, tunable resistance wires, and as strain sensors. Notably, the sandwich structure enables the PAD-CNT hydrogel to output capacitive signals, exhibiting a more sensitive response in monitoring human movement. Overall, this study introduces a novel composite structure for conductive hydrogels, holding tremendous potential in flexible conductivity and smart response fields.

Removal of Surface Radioactive Uranium(Ⅵ) by Graphene Oxide Modified κ-carrageenan/Konjac Glucomannan Composite Hydrogel

Hydrogel is an effective surface decontamination technology. However, traditional colloid decontaminants face a long curing time and low decontamination rate. A peelable hydrogel coating composed of carrageenan, konjac glucan, and graphene oxide with excellent film-forming performance and decontamination efficiency was explored in this study. The results showed that the graphene oxide was effectively dispersed inside the hydrogel, improving the crosslink density and thermal stability of the hydrogel by forming hydrogen bonds with polysaccharide molecules. The graphene oxide can effectively enhance the decontamination performance of the hydrogel. For stainless steel, ceramic, glass, and rubber surfaces, the decontamination rates of the hydrogel for 30min were 96.95%, 87.6%, 96.27%, and 74.5%, respectively. The decontamination effect was stable to temperature. For cement surfaces, the hydrogel could reach a maximum decontamination rate of 70.68% after 24h. The decontamination efficiency of hydrogel was affected by porosity, surface roughness, and graphene oxide addition. The characterization results of XPS, FT-IR, and SEM/EDS showed that the decontamination process of the composite hydrogel may involve surface wetting, ion diffusion, electrostatic attraction, and physical entanglement.

Preparation of high-performance antibacterial/antifungal citric acid–starch adhesives based on physical entanglement and chemical crosslinking

Starch-based wood adhesives are widely used as environmentally friendly and formaldehyde-free alternatives in the manufacturing of wood products. However, their poor water resistance and inability to inhibit bacterial/fungal growth limit their practicality. To address this issue, a physicochemical double-crosslinked network structure between citric acid, starch, and wood was prepared in this study by physically entangling the wood structure and chemically crosslinking the starch molecules, with citric acid preventing the activity of various enzymes and denatured proteins within microbial cells, thereby inhibiting bacterial and fungal growth. In water resistance cycling tests, the resulting esterified starch plywood demonstrated a 47.6 % and 13.2 % increase in water resistance compared with starch plywood and commercially available phenolic resin plywood, respectively. In addition, the tighter intermolecular bonding in the crosslinked structure results in a 31 % increase in heat resistance. The physical “nailing” and chemical crosslinking between the adhesive and the wood improved considerably the bonding strength to 98.36 %. The dual role of the physicochemical crosslinking of starch adhesives provides a straightforward strategy for the preparation of inexpensive, water-resistant, and fungal/bacterial-resistant starch adhesives, thus contributing to the promotion of starch adhesives.

The effect of graphene properties on the extrusion of a shape memory epoxy vitrimer

Thermoset polymers exhibit very appealing mechanical and functional properties. Direct ink writing (DIW) could open new possibilities in the design and fabrication of intricate thermoset parts, but it often requires the use of additives such as fumed silica or nanoclays to modify the rheology of uncured epoxies. However, relatively large concentrations are usually needed what can be detrimental to properties. Graphene-derived additives are an appealing alternative, but we need to understand the key physicochemical characteristics that define an optimum graphene rheology modifier. Here we compare the effect of three different carbon fillers on the viscoelastic response of a reprocessable epoxy vitrimer with shape memory capabilities, graphene oxide (GO), reduced graphene oxide (rGO), and graphene powder (GP), and assess the effect of their chemistry and morphology. The analysis shows that large (∼20 μm in size) rGO flakes enable the formation of strong, printable gels, through Van der Waals interactions and physical entanglement. The vitrimer could be successfully printed by incorporating 5 wt% of rGO. The printed parts exhibit tensile strengths (30–60 MPa), moduli (2–3 GPa), strength recovery after reprocessing (∼80 %), shape-memory properties comparable to the pure epoxy, and improved water resistance due to the introduction of hydrophobic rGO.

Sliding on Slide-Ring Gels

Recent investigations have pointed to physical entanglements that greatly outnumber chemical crosslinks as key sources of energy dissipation and low friction in hydrogel networks. Slide-ring gels are an emerging class of hydrogels described by their mobile crosslinks, which are formed by rings topologically constrained to slide along linear polymer chains within the network. These materials have enjoyed decades of study by polymer chemists but have been underexplored by the tribology community. In this work, we synthesized a pseudo-rotaxane crosslinker from poly(ethylene glycol) diacrylate (PEG-diacrylate) and α-cyclodextrin-acrylate followed by hydrogel networks by connecting the sliding crosslinks with polyacrylamide chains. The mechanical and tribological properties of slide-ring hydrogels were investigated using a custom-built microtribometer. Slide-ring hydrogels exhibit unique behavior compared to conventional covalently crosslinked polyacrylamide hydrogels and offer a vast design space for future investigations.Graphical

Polymer Gels from Physical Entanglements of Ultrahigh–Molecular Weight Polymers in Ionic Liquids

Polymer Gels from Physical Entanglements of Ultrahigh–Molecular Weight Polymers in Ionic Liquids

Fabrication of edible nanocellulose chitosan bi-component film based on a novel “swell-permeate” approach

The fabrication of multi-component film with colloidal particles could be inconvenient. A novel “swell-permeate” (SP) strategy was proposed to form homogeneous multi-component films. The SP strategy allows colloidal particles to fit into the polymer network by stretching the polymer chains assisted by water. We demonstrated the strategy by creating films with polysaccharide substrates as β-cyclodextrin grafted chitosan (CS) with nanocellulose. The addition of nanocellulose significantly increased the mechanical properties and the barrier performance of the films. The size of nanocellulose particles in affecting mechanical properties was investigated by applying different length of cellulose nanocrystal (CNC), the longer of which, due to denser physical entanglements, showed a better increase to the film in the elastic modulus and tensile strength to 4.54-fold and 5.71-fold, respectively. The films were also loaded with ethyl-p-coumarate (EpCA) and had an enhanced performance in anti-microbial for Altenaria alternata, Salmonella typhi, and Escherichia coli. The anti-oxidative property was increased as well, and both effects were valid both in vitro and in ready-to-eat apples. The strategy provides a practical and convenient method for fabricating colloidal particle containing films, and the novel idea of “swell-permeate” is potentially regarded as a new solution to the challenge of ready-to-eat food quality maintenance.

Hydrogels with high sacrifice efficiency of sacrificial bonds and with high strength and toughness due to dense entanglements of polymer chains

Introducing sacrificial bonds is a common method for increasing the toughness of hydrogels. Many sacrificial bonds have been extensively investigated, but the sacrifice efficiency has never been studied. In this study, polyacrylamide hydrogels with highly entangled polymer chains containing carboxyl–zirconium (–COO−–Zr4+) sacrificial bonds are prepared to study the effect of polymer chain entanglement on the sacrificial bond efficiency. Unlike chemical crosslinking points, the dense physical entanglements do not affect the toughness (∼43 MJ/m3) of hydrogels but significantly improve the tensile strength (by two times) and Young’s modulus (by six times). Physical entanglements enable the chains to slide and adjust the network structure under stress, which enables more polymer chains and sacrificial bonds to participate in the deformation process. Therefore, dense entanglements will greatly improve the sacrifice efficiency. However, a high density of chemical crosslinking points will limit the improvement in the sacrifice efficiency, which is attributed to the sliding limitations because of physical entanglement. The highly entangled polyacrylamide hydrogels toughened by –COO−–Zr4+ have an excellent load-bearing capacity. This study provides a novel strategy for designing hydrogels with ultra-high strength and toughness, which paves the way for the development of many hydrogels used in engineering materials.

Reducing the number of qubits in quantum simulations of one dimensional many-body Hamiltonians

We investigate the Ising and Heisenberg models using the block renormalization group method (BRGM), focusing on its behavior across different system sizes. The BRGM reduces the number of spins by a factor of 1/2 (1/3) for the Ising (Heisenberg) model, effectively preserving essential physical features of the model while using only a fraction of the spins. Through a comparative analysis, we demonstrate that as the system size increases, there is an exponential convergence between results obtained from the original and renormalized Ising Hamiltonians, provided the coupling constants are redefined accordingly. Remarkably, for a spin chain with 24 spins, all physical features, including magnetization, correlation function, and entanglement entropy, exhibit an exact correspondence with the results from the original Hamiltonian. The study of the Heisenberg model also shows this tendency, although complete convergence may appear for a size much larger than 24 spins, and is therefore beyond our computational capabilities. The success of BRGM in accurately characterizing the Ising model, even with a relatively small number of spins, underscores its robustness and utility in studying complex physical systems, and facilitates its simulation on current NISQ computers, where the available number of qubits is largely constrained.

Deciphering the structure-function-quality improvement role of starch gels by wheat bran insoluble dietary fibers obtained from different fermentation patterns and its potential mechanisms

Insoluble dietary fiber (IDF) isolated through co-fermented bran from probiotics may improve starch gel-based foods. This work aimed to elucidate the comprehensive impact of different IDF samples (CK, unfermented; NF, natively fermented; YF, yeast fermented; LF, Lactobacillus plantarum fermented; and MF, mix-fermented) and their addition ratios (0.3–0.9%) on gel structure-property function. Results indicated that IDF introduction altered the starch pasting behavior (decreased the viscosity and advanced the pasting time). Also, YF, LF, and MF showed less effect on gel multiscale morphology (SEM and CLSM); however, their excessively high ratio resulted in network structure deterioration. Moreover, FT-IR, XRD, and Raman characterization identified the composite gels interaction mechanisms mainly by hydrogen bonding forces, van der Waals forces, water competition, and physical entanglement. This modulation improved the composite gel water distribution, rheological/stress-strain behavior, textural properties, color, stability, and digestive characteristics. The obtained findings may shed light on the construction and development of whole-grain gel-based food products with new perspectives.

A super-stretchable and anti-fatigue silicone gel by regulating chain entanglement and cross-link density

Applications of silicone gel in flexible devices and soft machines require it to maintain excellent stretchability and antifatigue. However, the reported fatigue threshold of traditional silicone gels is in the range of 1–100 J m−2 and the stretchability below 2000 %. Herein, we report a simple strategy for constructing soft polydimethylsiloxane gels, which possesses high stretchability up to 8300 %, and high fatigue resistance (321 J m−2). This is achieved by controlling the ratio of chemical crosslinking and physical entanglement in the polydimethylsiloxane gels. The symbiotic relationship of this combination includes: extending the polymer chains helps them unfold to increase softness and intrinsic toughness; controlling the physical entanglement and chemical cross-linking helps to further increase the tensile rate and fatigue threshold, and adding small-molecule dimethyl PDMS as a solvent further increases fatigue resistance and tensile properties. This work provides a facile approach for developing super-stretchable and anti-fatigue silicone gel, which promises wide range of applicant in flexible devices and soft machines.

Exploring the influence of native minerals in coal gangue on CG/PE composite manufacturing and performance: Examining SiO2's role in interfacial compatibility

AbstractThis study delves into the influence of inherent minerals within coal gangue (CG) on the preparation and performance of coal gangue /polyethylene (CG/PE) composites, focusing on the role of SiO2 in interfacial compatibility. A systematic examination unveils the consequences of varying SiO2 content on physical, mechanical, thermal, and microstructural attributes of the composites. SiO2 incorporation significantly improves physical properties, boosting density and hardness but impacting tensile strength negatively. It enhances bending strength and modulus while diminishing tensile strength. Judicious SiO2 addition enhances thermal stability, but excess SiO2 may compromise thermal decomposition. Microstructural analysis, including SEM and FTIR, elucidates SiO2‐PE interactions, primarily through physical entanglement. SiO2 introduction promotes more ordered PE molecular chain arrangements, elevating composite crystallinity. In summary, this study provides in‐depth insights into SiO2's mechanistic impact on CG/PE composite properties, laying a robust foundation for designing environmentally friendly composites. These findings hold promise for advancing sustainable materials science and engineering. Future research may explore SiO2 optimization for specific applications and synergistic effects with other fillers in composites.Highlights SiO2 greatly improves the properties of CG/PE composites with detailed exploration. Reveals the specific SiO2‐PE interaction mechanism for a better comprehension. Performs structural analysis via XRD with valuable findings presented. Promotes pioneering advancements in eco‐friendly materials with broad significance.

Controlled dissolution of physically cross-linked locust bean gum – κ-carrageenan hydrogels

Most hydrogels swell but do not dissolve in water since their chains are tied to each other. Nevertheless, some hydrogels disintegrate under physiological conditions, a property that could be beneficial in emerging applications, including sacrificial materials, 3D bioprinting, and wound dressings. This paper proposes a novel approach to control the dissolution rate of hydrogels based on the integration of kappa carrageenan nanoparticles (KCAR-NPs) into kappa carrageenan (KCAR) and locust bean gum (LBG) hydrogels to obtain a three-component hybrid system. KCAR and LBG are known to have synergistic interactions, where physical interactions and chain entanglements lead to their gelation. We hypothesized that integrating the bulky nanoparticles would disturb the three-dimensional network formed by the polysaccharide chains and enable manipulating the dissolution rate. Compression, water absorption, rheology, and cryo-scanning electron microscopy measurements were performed to characterize the physical properties and structure of the hydrogels. The hybrid hydrogels displayed much faster dissolution rates than a control system without nanoparticles, which did not completely dissolve within 50 days and offered a cutting-edge means to finely adjust hydrogel dissolution through modulation of KCAR and KCAR-NPs concentrations. The new hydrogels also exhibited shear-thinning and self-healing properties resulting from the weak and reversible nature of the physical bonds.

Superabsorbent ZnO/rubber-based hydrogel composite for removal and photocatalytic degradation of methylene blue

A superabsorbent hydrogel was prepared by the free-radical copolymerization of natural rubber (NR) latex with poly(acrylic acid) (PAA) at NR loadings up to 50 wt%. An NR/PAA hydrogel containing 40 wt% of NR (NR-40) had a water absorption capacity of 214 g/g (21,400 %) of its dry weight. The compressive modulus increased 512 % and sample integrity was improved due to the physical entanglement of NR chains. NR-40 hydrogel removed 97 % of methylene blue (MB) from the aqueous solution in 1 h (at initial concentrations of 10–1000 mg/L) and produced a maximum removal of 1191 mg MB/g of hydrogel at an initial MB concentration of 4500 mg/L. The adsorption of MB was an endothermic process. Fourier transform infrared spectroscopy indicated that hydrogen bonding and electrostatic interaction drove the process. After the in-situ incorporation of ZnO into NR-40, absorbed energy from sunlight generated active species that could photocatalytically degrade adsorbed MB in the hydrogel matrix. The scavenger tests indicated that superoxide radical anions and hydroxyl radicals were the main species for this process. The hydrogel composite material showed good stability and could be regenerated and reused over 10 cycles, degrading >80 % of the adsorbed dye. This novel natural-based hydrogel provides double functions of adsorption and photodegradation of toxic dyes without the requirement of chemicals and a separation process.

Enhancing the strength and toughness of polylactic acid-based composites through one-step co-deposition of active coating onto wood fiber

A facial strategy of co-deposition is proposed to enhance the interfacial bonding in wood fiber (WF)/polylactic acid (PLA) composites. Dopamine or tannic acid (TA) was co-deposited with 3-aminopropyltriethoxysilane (APTES) onto the WF surface to create active coatings. These coatings were formed through Michael addition and Schiff base reactions and effectively attached to the WF through a combination of hydrogen and covalent bonding. Such active coatings facilitated the connection between WF and PLA through both covalent bonds and physical entanglements, thereby enhancing the interfacial interactions and compatibility between the two components. The co-deposition of TA with APTES was found to be more effective than with dopamine, leading to a dramatic improvement in the tensile strength and elongation at break of the composites by 33.4 % and 185.9 %, respectively. This work offers a facile method to prepare high performance plant fiber reinforced PLA composites, thereby broadening the potential applications of PLA.

Preparation of poly(lactic acid) grafted glycidyl neodecanoate by solid phase grafting and its compatibilization for poly(lactic acid)/poly(butylene adipate‐co‐terephthalate) composite

AbstractPoly(lactic acid) (PLA) grafted glycidyl neodecanoate (GND) with a single epoxy group (PLA‐GND) is prepared in this paper by solid phase grafting, and the effects of different reaction conditions on the grafting percentage of PLA‐GND are investigated. Furthermore, PLA‐GND is used as a nonreactive compatibilizer to prepare PLA‐GND/PLA/poly(butylene adipate‐co‐terephthalate) (PBAT) composite by melt blending. The results show that PLA‐GND has the highest grafting percentage of 2.15% when the feed weight ratio of GND to PLA is 0.2, the feed weight ratio of triphenylphosphine to PLA is 0.02, the additive amount of xylene is 1 mL, the reaction temperature is 120°C, and the reaction time is 115 min. The GND segments of PLA‐GND and PBAT segments could form a physical entanglement microdomain because of the similar aliphatic chain of GND and PBAT, which would improve the compatibility of PLA and PBAT. PLA‐GND/PLA/PBAT composite has the highest tensile strength, elongation at break, impact strength, crystallinity, heat deformation temperature, and melt flow rate at a PLA‐GND content of 5%, which are 38.54 MPa, 118.65%, 15.83 kJ/m2, 5.71%, 65.3°C, and 36.3 g/10 min, 14.53%, 390.90%, 68.94%, 224.43%, 16.19%, and 224.40% higher than those of PLA/PBAT composite, respectively.Highlights PLA grafted GND with a single epoxy group is prepared by solid phase grafting. PLA‐GND as a non‐reactive compatibilizer compatibilizes PLA/PBAT composite. The similar chain of GND and PBAT is helpful to form the physical entanglement. The physical entanglement is essential to improve compatibility of PLA and PBAT. PLA/PBAT composite has excellent overall performance at a PLA‐GND content of 5 wt%.