Spherulitic Growth Research Articles

Correction to “Relation between Spherulitic Growth, Molecular Organization and Charge Carrier Transport in Meniscus‐Guided Coated Organic Semiconducting Films”

Correction to “Relation between Spherulitic Growth, Molecular Organization and Charge Carrier Transport in Meniscus‐Guided Coated Organic Semiconducting Films”

Optimization of polypropylene high-strength injection molding welding and interface structure analysis

Secondary injection molding is an effective method for joining polymer parts, where the weld interface plays a critical role in the overall performance of the part. This study discusses the influence of injection molding parameters on the interface strength of polypropylene and polypropylene (PP-PP) secondary injection molding and analyzes the welding interface structure. The injection molding parameters for PP-PP were optimized using the Taguchi method and the signal-to-noise ratio (S/N). The optimal injection molding parameters were determined to be a mold temperature of 120°C, injection temperature of 350°C, and injection speed of 100 mm/s. The interface tensile strength was measured at 33.42 MPa, corresponding to 98.1% of the tensile strength of the base material. Among these parameters, mold temperature has the greatest influence on the strength of the welding interface. Secondly, polarizing microscopy, scanning electron microscopy (SEM), and Fourier transform infrared spectroscopy (FTIR) were employed to observe and analyze the crystal structure and fracture failure modes at the interface. The results indicate that elevated injection molding parameters promote the formation of crystal nuclei and spherulite growth at the secondary melt interface, with the spherulite size at the interface significantly affecting the interface strength. This study offers valuable reference for the welding of other polymers and fiber-reinforced materials.

Preparation of tenofovir amibufenamide fumarate spherical particles to improve tableting performance and sticking propensity by designing a spherical crystallization process

Tenofovir amibufenamide fumarate (TMF) is the first oral drug developed in Asia for the treatment of adult patients with chronic viral hepatitis B, however, further applications are limited by poor tableting performance and high sticking propensity. In this work, the spherulitic growth process of TMF has been designed and explored with the help of molecular dynamics simulation and process analysis technologies (ATR-FTIR, FBRM and EasyViewer). The spherical particles with high bulk density, good flowability and uniform particle size distribution are prepared by a simple quenching process. More importantly, experimental results show that spherical particles have higher average tensile strength (100.8% increase), higher plastic deformability and lower amount of punch sticking (87.4% decrease in 30 tablets) compared to the commercial powder products. These contributions not only shed light on the design principle of drug spherulitic growth processes, but also provide guidance for the manufacture of high-quality tablet products.

Numerical simulation of spherulite and shish-kebab growth for semi-crystalline polymer melts via phase-field model

Polymer crystallization is an important research topic in materials sciences. The phase field model is employed to simulate the growth of spherulites and shish-kebabs for the semi-crystalline polymer under melt flows. Firstly, the phase field equation is discretized by the finite difference method(FDM), the energy equation is solved by the finite volume method(FVM), and the governing equation of viscous polymer melts is modeled and solved by the lattice Boltzmann method(LBM). And then the numerical simulations are conducted for the growth process of spherulites and shish-kebabs under the static and flowing conditions, respectively. Morever, the growth of shish-kebabs are simulated in two different mold cavities under melt flows and compared with each other. Finally, the growth of co-existed spherulites and shish-kebabs are simulated in both static and flowing states. Numerical results show that the coupled FD-FV-LB algorithm could successfully capture the growth interfaces of spherulites and shish-kebabs. The complex cavity makes the flow more complex, thereby changing the crystal morphologies. The melt flow makes the polymer crystals grow faster and densely towards the upstream direction, and increase the temperatures of the crystals.

Solvent‐free crystallization for fractionation of virgin coconut oil: Effect of process conditions on kinetics and crystal properties

AbstractThis research was aimed to conduct solvent‐free crystallization and fractionation of virgin coconut oil (VCO). This study investigated the effect of surface contact area‐to‐volume ratio and mixing conditions on crystal characteristics. Commercially available VCO samples, extracted by different methods, were analyzed for fatty acid and triacylglycerol composition using GC–MS and UPLC–ELSD. VCO extracted through enzyme and chilling–thawing cycles exhibited higher medium chain fatty acids and medium chain triacylglycerols, which was selected for crystallization studies. Isothermal crystallization of VCO at 21°C assessed the effect of scale of crystallizer tube on cooling rate using Newton's law of cooling equation. The smaller tube (20 mm diameter) with a higher surface contact area‐to‐volume ratio produced 4.1‐fold faster cooling and a higher crystallization yield (44%) compared to the 80 mm diameter tube when no agitation was applied. Whereas mixing with a magnetic stirrer produced a large number of nuclei, generating intense crystallization heat, and rendering the crystals inseparable from liquid fraction. The process of VCO crystallization was also studied for kinetics and crystal growth mechanism using the Avrami model employing angled rotation of sample tube during non‐isothermal crystallization. Angled rotary mixing produced stable crystals and significantly increased the crystallization rate (t1/2 = 26.86 min) with polyhedral or spherulitic crystal growth (n = 3.25) compared to non‐mixing condition (t1/2 = 161.87 min) with restricted linear growth (n = 1.64). DSC analysis of VCO and its fractions obtained after crystallization using the 20 mm tube with angled rotary mixing indicated shifts in their thermogram peaks, suggesting differences in triacylglycerol compositions.Practical applicationsVirgin coconut oil (VCO) is well recognized for its health‐beneficial properties, yet its application is limited due to its complex triglyceride composition. The solvent‐free crystallization method facilitates VCO fractionation into phases with different melting points without hazardous solvents. The efficacy of this process is highly dependent on temperature, cooling rate, and agitation, which affects crystal morphology and growth kinetics. This study addresses these challenges in the scarcely investigated area of VCO crystallization. The resulting fractions can be customized for specific applications based on their altered functional properties in producing baking and confectionery coatings, salad dressings, and so on. The olein fraction obtained in this study can be utilized in nutraceutical formulations targeting digestive and cognitive health, as it is reported to be rich in medium chain triglycerides. This research optimizes process conditions, suggesting an efficient method for dry‐fractionating VCO, which is significantly associated with the food and pharmaceutical industries.

Influence of non-linear diffusion controlled phenomena on the sorption capability of PEO-Salt-SiO2 composite electrolyte: A study on property optimization

The present research, reports the hygrothermal behavior of poly [ethylene oxide] (PEO) based composite film (500 and1000 μm) containing NH4I and KBr (5–20 wt%) as the mobile phase and non-reactive silica (15 wt%) as the filler. These are termed as PK/NSiO2-series for solvent sorbed and (PK/NSiO2)NS for non-swelled film. The novelty of the research lies in the analyses of non-Fickian solvent diffusion trait of films using python programming. The presence of ions and its variable polarizable nature is found to influence the number density of bonded and free solvent content along with the extend of cross linkage. Introduction of silica is found to enhance the ionic conductivity (about one order higher) of the film irrespective of the type of charge carrier owing to the improved dispersion within the matrix. Non-Fickian diffusion is found to influence the ionic conductivity of P2K20SiO2 (10−5Scm−1 to 10−2 Scm−1) minimizing the degradation to 0.2 %ΔC/1000 h (>1 %ΔC/1000 h, tested for 2000 h) compared to P2N20NSiO2. In contrast, ion migration in P2NSiO2 is guided by Rice and Roth model and being more polarizable ions, the mobility is significant which maximizes the conductivity to ∼10−1 Scm−1. Microstructural study shows heterogenous nucleation to be more pronounced upon addition of silica filler wherein the homogeneity, inter fibrillar interaction and grain growth of spherulites is higher. This tends to extend amorphous regions thereby propagating the ion migration path. The influence of sorption process is studied in terms of electrochemical impedance, dielectric analyses and long term cyclability (20,000 h) in terms of loss tangent.

Change in Concentration of Amorphous Region Due to Crystallization in PTT/PET Miscible Blends.

In a miscible crystalline/crystalline blend of poly(trimethylene terephthalate) (PTT) and poly(ethylene terephthalate) (PET), the PET spherulites grew at 240 °C when the PTT content was 30 wt% or less. The growth rate of PET spherulites decreased with time due to the exclusion of PTT from the growth front of PET spherulites into the amorphous region, resulting in a three-stage crystallization process. Due to the exclusion, the spherulite growth stopped before the volume filling of the PET spherulites, causing the formation of an excluded PTT amorphous region. When the temperature was lowered from 240 °C to 210 °C, the PTT spherulites grew in the excluded PTT amorphous region. The spherulite growth rate of PTT in the excluded PTT amorphous region was equivalent to that of a blend of 60-70 wt% PTT in 30/70 PTT/PET. These results suggest a significant change in the PTT concentration in the amorphous region, from the initial PTT content of 30 wt% to 60-70 wt%, due to the exclusion of PTT during the melt crystallization of PET at 240 °C.

An Algorithm for Modeling Thermoplastic Spherulite Growth Using Crystallization Kinetics.

Crystallization kinetics were used to develop a spherulite growth model, which can determine local crystalline distributions through an optimization algorithm. Kinetics were used to simulate spherulite homogeneous nucleation, growth, and heterogeneous nucleation in a domain discretized into voxels. From this, an overall crystallinity was found, and an algorithm was used to find crystallinities of individual spherulites based on volume. Then, local crystallinities within the spherulites were found based on distance relative to the nucleus. Results show validation of this model to differential scanning calorimetry data for polyether ether ketone at different cooldown rates, and to experimental microscopic images of spherulite morphologies. Application of this model to various cooldown rates and the effect on crystalline distributions are also shown. This model serves as a tool for predicting the resulting semi-crystalline microstructures of polymers for different manufacturing methods. These can then be directly converted into a multiscale thermomechanical model.

Improving Powder Performances of d-Ribose through Spherulitic Growth

Improving Powder Performances of <scp>d</scp>-Ribose through Spherulitic Growth

Constructing Porous Energetic Spherulites via Solvation-Growth Coupling for Enhanced Combustion.

The fabrication of materials with hierarchical structures has garnered great interest, owing to the potential for significantly enhancing their functions. Herein, a strategy of coupling molecular solvation and crystal growth is presented to fabricate porous spherulites of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (CL-20), an important energetic material. With the addition of polyvinylpyrrolidone in the antisolvent crystallization, the metastable solvate of CL-20 is formed and grows spherulitically, and spontaneously desolvates to obtain the porous spherulite when filtration, in which the characteristic peak of the nitro group of CL-20 shifts detected by the in situ micro-confocal Raman spectroscopy. The effect of polyvinylpyrrolidone is thought to induce the solvation of CL-20, confirmed by density functional theory calculations, meanwhile acting on the (020) face of CL-20 to trigger spherulitic growth, demonstrated through infrared spectroscopy and Rietveld refinement of powder X-ray diffraction. Moreover, compared to common CL-20 crystals, porous spherulites exhibit enhanced combustion with increases of 6.24% in peak pressure, 40.21% in pressurization rate, and 9.63% in pressure duration effect, indicating the capability of hierarchical structures to boost the energy release of energetic crystals. This work demonstrates a new route via solvation-growth coupling to construct hierarchical structures for organic crystals and provides insight into the structure-property relations for material design.

Origin and Nucleation Kinetics of Transcrystalline Layer in Bamboo fiber@nano‐TiO2/Polypropylene Composite

AbstractHerein origin and nucleation kinetics of transcrystalline layer (TCL) in bamboo fiber deposited with nano‐TiO2 (BF@TiO2)/polypropylene (PP) composite is studied. Firstly, the surface morphology, roughness, and energy, as well as crystalline structure (e. g., crystal face indices (hkl)) of BF@TiO2 are analyzed to clarify the origin of TCL in the composite. Subsequently, the nucleation kinetics of TCL in BF@TiO2/PP composite at different crystallization temperatures (Tc) are investigated through polarized optical microscopy. The results find that the surface roughness and energy of BF@TiO2 increase by 47.55 % and 2.41 % compared with untreated BF, respectively. Interestingly, the mismatch rates (MRs) of hkl(BF) vs. hkl(PP) are &gt;320 %. In comparison, the MRs of (101)(BF@TiO2)TiO2 vs. (hkl)(PP) are dramatically decreased to &lt;25 %, suggesting a similar crystal plane between BF@TiO2 and PP matrix. These results indicate that the TCL formation in the composite is more facile in BF@TiO2 than in the untreated BF. During isothermal crystallization, the nucleation and spherulite growth rates decrease as the Tc increases. The interface free energy difference (▵σ) between BF@TiO2 and PP is calculated based on the heterogeneous nucleation theory. The ▵σ is 1.54±0.11 J cm−2, highlighting that the BF@TiO2 strongly induces the PP nucleation.

A non-classical crystallization mechanism of microbially-induced disordered dolomite

Non-classical crystallization pathways, involving the formation of complex precursors prior to nucleation, have been observed during the calcification process of invertebrate skeletons and shells. However, these pathways were rarely documented in microbially-induced carbonate precipitation. In this study, we presented experimental evidence demonstrating that a halophilic bacterium (Halomonas sp. strain JBHLT-1) catalyzed the biomineralization of disordered dolomite through an amorphous calcium-magnesium carbonate (ACMC) with a stoichiometry near that of dolomite. During the ACMC formation, strain JBHLT-1 significantly enhanced the incorporation of Mg2+ ions compared to abiotic ACMC that was synthesized without any microbial biomass. In the stage of ACMC crystallization, the presence of microbial biomass reduced the dissolution-reprecipitation rate and induced bias towards a solid-state reaction pathway. This observation was supported by the negligible loss of structural Mg2+ ions in the presence of cells of strain JBHLT-1. The microbially-induced growth of disordered dolomite appeared to follow a spherulitic growth mechanism, as evidenced by its hierarchical structure composed of coalesced nano-spheres, eventually growing into micron-sized spheroids and dumbbells with extended incubation times. Since disordered dolomite is considered as a crucial crystalline precursor of ordered sedimentary dolomite, the findings of this study have important implications for understanding the formation mechanism of natural dolomite.

Polymer Crystallization Kinetics and Thermodynamics of Some Industrial Polyamides

A comprehensive non-isothermal kinetics study on polymer crystallization processes taking place in a set of industrial polyamides comprising nylon 6, nylon 6,6, nylon 11 and nylon 12, individually, is reported. The kinetics studies elucidated that the phenomena of nucleation/diffusion underlying the nylons crystallization go to completion in a single-step. Notwithstanding, the nylons diffusion activation energies do not correspond to the universal value of segmental jump activation energy signifying polymer chains diffusion processes. The polymer chain transport phenomenon was probably the slowest one in the case of nylon 6 and nylon 6,6, and the fastest in the case of nylon 12, while intermediate for nylon 11. Furthermore, the nucleation barrier during the course of polymer crystallization was the highest for nylon 6,6, followed by nylon 6, nylon 11 and nylon 12. Our kinetics studies further predict that the crystallization of nylon 12 and nylon 11 follows, respectively, diffusion-controlled 2D growth of spherulites and a somewhat complicated nucleation/growth phenomenon. The thermodynamics of the nylons crystallization suggests that the highest structural orientation of the activated complex was attained in the case of the nylon 12 crystallization process. Interestingly, while the thermodynamics and majority of the kinetic parameters of nylon 6 and nylon 6,6 were similar/comparable, the two follow widely differing crystallization mechanisms. The most probable physical meanings of the obtained kinetics and thermodynamics parameters and their practical significance are given and discussed.

Optimizing bonding performance in CF/PEKK composites: The role of IR heating and press consolidation

Bonding performance of carbon fiber/polyetherketoneketone (CF/PEKK) laminates is closely related to crystallinity and is influenced by growth, formation, and density of spherulites. Press consolidation, with its ability to adjust pressure, exhibits superior quality compared to oven consolidation. However, bonding and production of CF/PEKK laminates using Press consolidation exhibit significant variations in quality depending on forming conditions. While research on producing CF/PEKK laminates using press consolidation is currently active, there is a lack of studies on co-consolidation for CF/PEKK laminates. Thus, in this study, establishment of forming process variables for press consolidation was conducted to achieve excellent bonding performance for CF/PEKK. Furthermore, IR heating-assisted surface heat treatment was employed to enhance bonding performance of CF/PEKK laminates by controlling crystallinity and spherulites. To analyze bonding performance, short bean shear testing was conducted to obtain interlaminar shear strength (ILSS). Results showed that surface modification through IR heating led to an increase in crystallinity and a noticeable growth in size of spherulites. In specific conditions, improved bonding performance was observed. This is judged to be primarily due to increase in spherulite size and crystallinity at bonding interface, attributed to specific conditions of both surface treatment through IR heating and Press consolidation.

Chemical compositions and crystallization characteristics of SOS‐rich fats

AbstractSOS‐rich fats have been developed to improve heat stable properties and fat bloom‐resistant abilities of chocolates, which is highly connected with their crystallization behaviors. Shea butter stearin (SBS) and mango kernel fat (MKF) are the typical SOS‐rich fats. Both contained high levels of stearic acid (45.06%–59.67%) and oleic acid (31.85%–39.97%), while 77.00%–86.88% of the oleic acid were distributed at the sn‐2 positions of triacylglycerol molecules, contributing to forming 78.04% of SOS in SBS and 47.85% of SOS in MKF. Their SOS levels were significantly higher than that in cocoa butter (CB, 25.43%). However, MKF contained the highest levels of SOO (15.59%), which was about six to eight times as likely that in SBS and CB (1.76%–2.66%). Further crystallization tests revealed that SBS and MKF exhibited similar rod‐like growth from instantaneous nuclei at 4°C. The former was then changed to become more spherulitic growth at 20°C significantly. Specifically, large feather‐like crystals corresponding to β form were observed in SBS at the final stage of crystallization at 20 and 30°C, while MKF exhibited smaller crystals. The higher concentration of SOO in MKF was considered as the softening factor. It was further supposed that constant crystallization at 20°C may be difficult for some fats (e.g., SOS &lt; 30%) to form adequate amounts of β crystals. The results will provide information on making cocoa butter blends and chocolate tempering.

Molecular, Crystalline, and Microstructures of Lipids from Astrocaryum Species in Guyana and Their Thermal and Flow Behavior

The phase behavior of lipids extracted from Astrocaryum vulgare (AV) and Astrocaryum aculeatum (AA) pulp and kernels and their microstructural, thermal and flow properties were studied. The lipid profiles, crystal structures, microstructures, thermal stabilities and flow behaviors of these lipids provided important structure–function information that are useful to assess potential applications in the food, cosmetic and pharmaceutical industries. AV and AA fruits were sourced from the lowlands and rainforests, respectively, of Guyana. AV and AA pulp oils (AVP and AAP) were distinguished from each other in composition and unsaturation, with AVP oils being predominated by a di-unsaturated TAG (2-(palmitoyloxy)propane-1,3-diyl dioleate (POO)) and AAP oils predominated by propane-1,2,3-triyl trioleate (OOO); there were unsaturation levels of 65% and 80%, respectively. The main fatty acids in AVP oils were oleic, palmitic and stearic; for AAP, these were oleic, linoleic, palmitic and stearic. The kernel fats of AV and AA were similar in composition and had saturation levels of 80%, being mainly comprised of tri-saturated TAGs propane-1,2,3-triyl tridodecanoate (LLL) and 3-(tetradecanoyloxy)propane-1,2-diyl didodecanoate (LML). The onset of mass loss (T5%on) of AV and AA pulp oils were similar at 328 ± 6 °C, which were 31 °C ± 9 higher compared to that of the kernel fats, which demonstrated similar T5%on = 293 ± 7 °C. AA and AV pulp oils were liquid at room temperature, with melting points of −5 ± 1 °C and 3 ± 1 °C, respectively; both kernel fats were solid at room temperature, packing in β′ (90% of crystals) and β (10% of crystals) polymorphic forms and melting almost identically at 30 ± 1 °C. Pulp oils demonstrated sporadic nucleation at the onset of crystallization with slow growth into rod-shaped crystallites, leading to an approximately 50% degree of crystallization at undercooling of approximately 40K. Nucleation for kernel fats was instantaneous at undercooling of approximately 23K, demonstrating a spherulitic growth pattern incorporating crystalline lamella and a 90% degree of crystallization. Kernel fats and pulp oils demonstrated Newtonian flow behavior and similar dynamic viscosity in the melt, approximately 28.5 mPa·s at 40 °C. The lipid profiles of AVP and AAP oils were dominated by unsaturated TAGs, suggesting potential nutrition and health benefits, particularly compared to other tropical oils with higher saturation levels, such as palm oil. AAP oil in particular is as unsaturated as olive oil, contains high levels of beta carotene and provides a unique flavor profile. The AAK and AVK lipid profiles and phase transformation indicate potential for applications where a high solid fat content and medium-chain fatty acids are required. Their high lauric and myristic acid content makes them similar to industrially important tropical oils (coconut and palm kernel), suggesting their use in similar formulations. The melting point and plasticity of the kernel fats are similar to that of cocoa and shea butters, suggesting use as replacements in cosmetics, foods and confections. There is, however, the need to better understand their nutritional status and effects on health.

Polyethylene oxide mixtures with thymol: Unusual thermal behavior and morphology due to a crystallizable hydrogen-bonded complex

Formation of cocrystals in polymer-containing systems attracts a lot of attention lately due to their promise in pharmaceutics, being a poorly studied phenomenon in polymer science. For the first time, we report on the cocrystallization in mixtures of polyethylene oxide and thymol and study in detail the structure and thermal behavior of the mixtures by differential scanning calorimetry, optical microscopy, wide angle X-ray scattering, attenuated total reflection Fourier-transformed infrared spectroscopy, and quantum chemical simulation. The results are summarized into the experimental phase diagram that describes well all the transformations of the systems during their heating and cooling. On the molecular level, we conclude the existence of noncovalent-bonded complexes composed of three monomeric units of polyethylene oxide and two molecules of thymol, which might become structural units of cocrystals upon cooling. This results in a growth of huge centimeter-sized spherulites in the stoichiometric mixture and to the coexistence of two types of spherulites in the mixtures of other compositions. The peculiarities of thymol release from the complexes into different media are also investigated.

Numerical simulation of macroscopic viscoelastic melt filling and mesoscopic spherulite growth

Abstract In this work, a non-isothermal viscoelastic computational framework is proposed for macroscopic polymer melt filling and mesoscopic spherulite growth. Firstly, the macroscopic viscoelastic governing equation is solved by coupled level set immersed boundary and finite-volume (LS-IB-FV) method. The melt-air interface is captured by the coupled level-set and volume-of-fluid (CLSVOF) method. And the mesoscopic crystallization behavior is predicted by the phase field model. Then, the numerical simulation for melt filling process is compared with experimental one to validate the coupled method. And it is simulated that the melt filling stage in a complex annular cavity with 17 small solid discs for the semi-crystalline polymer of isotactic polystyrene, and it is studied that the impacts of three different injection velocities on the flow modes, temperature distribution and solidified layers. Finally, in the regions of solidified layers, the growth of spherulites is simulated with/without melt flows at two different points. Numerical results show that the injection velocities can affect the flow modes and temperature distribution significantly. The morphology of polymer spherulite that is consistent with the experimental result can be observed clearly. With flow fields, the spherulites grow faster and densely towards the upstream direction.

Trace polymer coated clarithromycin spherulites: Formation mechanism, improvement in pharmaceutical properties and development of high-drug-loading direct compression tablets

Clarithromycin (CLA) is a high dose antibiotic drug exhibiting poor flowability and tabletability, making the tablet development challenging. This study aims to develop spherulitic CLA by introducing trace amount of polymer in crystallization solution. Its formation mechanism, physicochemical properties and potential for the direct compression (DC) tablets development were also investigated. Morphological analyses and the in situ observation on crystallization process revealed that the CLA spherulites are formed by fractal branching growth from both sides of the threadlike precursor fibers. 1H NMR analysis and nucleation time monitoring indicated that the existence of hydroxypropyl cellulose in solution slowed down the crystal nucleation and growth rate by forming hydrogen bonding interactions with CLA molecules, making the system maintain high supersaturation, providing high driving forces for CLA spherulitic growth. In comparison to commercial CLA, the CLA spherulites exhibit profoundly improved flowability, tabletability and dissolution behaviors. XPS, contact angle and Raman mapping analysis confirmed the presence of a thin HPC layer on the surfaces and interior of CLA spherulitic particles, resulting in increasing powder plasticity, interparticulate bonding strength and powder wettability, thus better tabletability and dissolution performances. The improved flowability and tabletability of CLA spherulites also enabled the successful development of DC tablet formulation with a high CLA loading (82.8 wt%) and similar dissolution profiles to reference listed drug. This study provides a novel solid form of CLA with superior manufacturability for further development.

Solid polymer nanocomposite electrolytes based on poly(ε‐caprolactone)‐based waterborne polyurethane–polyethylene oxide and fluorine‐doped carbon quantum dot‐MXene

AbstractThe need for higher energy storage capability has encouraged researchers to move toward lithium‐metal batteries (LMBs). Due to the safety issue associated with liquid electrolytes, solid polymer electrolytes (SPEs) the main focus on polyethylene oxide (PEO) were at the center of the research. However, high crystallization, fast decomposition, and low thermomechanical stability has limited its application. Low lithium‐ion transference number () is another issue leading to polarization of the SPEs and consequently, triggering dendrite nucleation and growth. Here, we developed a series of SPEs based on PEO‐waterborne polyurethane (WPU) and nanoparticles of fluorine‐doped carbon quantum dot (fCQD) and MXene. The host polymer matrix was a blend of poly(ε‐caprolactone) (PCL)‐based WPU and PEO. The use of WPU and the nanoparticles increased the thermomechanical stability and suppressed PEO crystallinity through disrupting the spherulites growth and reducing the thermal stability of the crystallites. Using the WPU led to significant increase in () compared with previous reports. The prepared SPEs showed high‐electrochemical stability and ionic conductivity at and based on the results of cycling performance, a discharge capacity of 120.58 mAh/g and coulombic efficiency of 99.1% was achieved after 200 cycles.