Interchain Hydrogen Bonds Research Articles

Investigation of the microscopic damage mechanisms in cotton fibers induced by mechanical friction

For the problem of friction damage in cotton fiber processing, a multi-scale combination of investigation methods is proposed. The surface of damaged cotton fiber is detected by relevant test means with damage features such as dislocations, defects and cracks. The internal pyranose ring and glycosidic bond fail, the crystallinity decreases, and the number of hydrogen bonds decreases. Anisotropy exists in the frictional properties of the microscopic surface of the cotton fiber. The results of molecular dynamics simulation showed that the cellulose main chain failed mainly at the glycosidic bond, and the side chain failed mainly at the hydroxymethyl functional group. Its interchain hydrogen bond O3H…O5 was the least damaged. The cellulose crystal (200) surfaces had poor abrasion resistance, and the frictional properties of each crystal surface were anisotropic. The results of the study provide a theoretical basis for improving friction and wear problems in cotton fiber processing.

Achieving the Birefringence Optimization by Methyl Modulation in Organic Nonlinear Optical Crystals

AbstractNon‐centrosymmetric organics are promising nonlinear optical (NLO) candidates, which always exhibit a short UV absorption cutoff edge, and a strong second harmonic generation (SHG) response, but an overlarge birefringence. Here, in order to optimize the birefringence, the methyl modulation of π‐conjugated organic planar units is proposed and implemented with the urea structure as a template. Thus, N‐methylurea and N,N'‐dimethylurea crystals are obtained by partially replacing hydrogen atoms with methyl groups. This replacement reduces hydrogen donors and weakens interchain hydrogen bonds, which facilitates the decreasing density and the parallel arrangement of π‐conjugated planar units. Hence, both N‐methylurea and N,N'‐dimethylurea crystals exhibit not only an optimized birefringence (N‐methylurea ≈0.099 and N,N'‐dimethylurea ≈0.072 at 546 nm) but also an enhanced SHG response (N‐methylurea ≈1.2 × β‐BaB2O4 and N,N'‐dimethylurea ≈1.9 × β‐BaB2O4), while maintaining a short UV absorption cutoff edge. Therefore, this work provides a novel strategy for the structural design and performance modulation of organic NLO crystals.

Flexible Artificial Tactility with Excellent Robustness and Temperature Tolerance Based on Organohydrogel Sensor Array for Robot Motion Detection and Object Shape Recognition.

Hydrogel-based flexible artificial tactility is equipped to intelligent robots to mimic human mechanosensory perception. However, it remains a great challenge for hydrogel sensors to maintain flexibility and sensory performances during cyclic loadings at high or low temperatures due to water loss or freezing. Here, a flexible robot tactility is developed with high robustness based on organohydrogel sensor arrays with negligent hysteresis and temperature tolerance. Conductive polyaniline chains are interpenetrated through a poly(acrylamide-co-acrylic acid) network with glycerin/water mixture with interchain electrostatic interactions and hydrogen bonds, yielding a high dissipated energy of 1.58MJ m-3, and ultralow hysteresis during 1000 cyclic loadings. Moreover, the binary solvent provides the gels with outstanding tolerance from -100 to 60°C and the organohydrogel sensors remain flexible, fatigue resistant, conductive (0.27 S m-1), highly strain sensitive (GF of 3.88) and pressure sensitive (35.8 MPa-1). The organohydrogel sensor arrays are equipped on manipulator finger dorsa and pads to simultaneously monitor the finger motions and detect the pressure distribution exerted by grasped objects. A machine learning model is used to train the system to recognize the shape of grasped objects with 100% accuracy. The flexible robot tactility based on organohydrogels is promising for novel intelligent robots.

Dissolution of denim waste in N-methyl morpholine-N-oxide monohydrate for fabrication of regenerated cellulosic film: Experimental and simulation study

Despite the significant amount of denim waste and its potential as a cellulose source, its use has been neglected. This study uses N-methyl morpholine-N-oxide, an eco-friendly solvent, to dissolve denim (including 100 % cotton) and create a denim film. Achieving a 10 % denim record solubility, a cellulosic film was also fabricated for comparison. Characterisation techniques were applied, and molecular dynamics simulations explored intramolecular interactions and the influence of indigo dye on dissolution process. FTIR spectra indicated no chemical reactions during dissolution and regeneration, though a shift in OH stretching suggested a change in crystallinity, confirmed by XRD results showing decreased crystallinity and a structural shift from cellulose I to cellulose II. 13C NMR analysis revealed disruptions in interchain hydrogen bonds after regeneration. TGA results showed lower decomposition temperatures for both films compared to the powders. Testing mechanical properties showed the denim film had higher elongation at break but lower tensile strength than the cellulose film. MD simulations indicated indigo dye did not significantly affect fundamental interactions but decreased denim solubility by reducing the diffusion coefficient. Rheological tests supported the simulation results, showing higher viscosity and molecular weight for the denim solution compared to cellulose.

Preparation mixed matrix membranes with different types of Al2O3-NOHMs for enhancing CO2 separation performance

ABSTRACT Nano-organic hybrid materials (Al2O3-NOHMs) were synthesized with nano-alumina as the core, γ-(2,3-epoxypropyl) propyl trimethoxysiane (KH560) as the corona, and three of polyetheramine M2070, D2000, M1000 as the canopy, respectively. Al2O3-NOHMs were used as fillers to prepare MMMs with Pebax as substrate to improve the CO2 separation performance. The Al2O3-NOHMs were characterized by TEM and rheological properties. The results showed that the synthesized Al2O3-NOHMs were liquid-like and had a core-shell structure, which can effectively reduce Al2O3 agglomeration in the membrane. FT-IR analysis of MMMs showed that Al2O3-NOHMs and Pebax were physically blended, TGA indicated that Al2O3-NOHMs do not affect the thermal stability of the membrane, and XRD indicated that the addition of Al2O3-NOHMs destroyed the interchain hydrogen bond of Pebax and reduced the crystallinity of MMMs. The gas permeability of the membrane was tested under ideal gas conditions, compared with pure membrane, the CO2 permeability of Al2O3-NOHM(M2070)/Pebax MMMs and Al2O3-NOHM(D2000)/Pebax MMMs reached 137.15 Barrer (24.68%) and 147.52 Barrer (34.11%), and the selectivity of CO2/N2 reached 77.82 (58.84%) and 72.31 (47.59%) at 30°C and 0.3 MPa, respectively, surpassing 2008 Robeson upper bound.

Crystal structure of polymeric bis-(3-amino-1H-pyrazole)-cadmium diiodide.

The reaction of cadmium iodide with 3-amino-pyrazole (3-apz) in ethano-lic solution leads to tautomerization of the ligand and the formation of crystals of the title compound, catena-poly[[di-iodido-cadmium(II)]-bis-(μ-3-amino-1H-pyrazole)-κ2 N 2:N 3;κ2 N 3:N 2], [CdI2(C3H5N3)2] n or [CdI2(3-apz)2] n . Its asymmetric unit consists of a half of a Cd2+ cation, an iodide anion and a 3-apz mol-ecule. The Cd2+ cations are coordinated by two iodide anions and two 3-apz ligands, generating trans-CdN4I2 octa-hedra, which are linked into chains by pairs of the bridging ligands. In the crystal, the ligand mol-ecules and iodide anions of neighboring chains are linked through inter-chain hydrogen bonds into a di-periodic network. The inter-molecular contacts were qu-anti-fied using Hirshfeld surface analysis and two-dimensional fingerprint plots, revealing the relative qu-anti-tative contributions of the weak inter-molecular contacts.

Impact of Sacrificial Hydrogen Bonds on the Structure and Properties of Rubber Materials: Insights from All-Atom Molecular Dynamics Simulations.

The inclusion of sacrificial hydrogen bonds is crucial for advancing high-performance rubber materials. However, the molecular mechanisms governing the impact of these bonds on material properties remain unclear, hindering progress in advanced rubber material research. This study employed all-atom molecular dynamics simulations to thoroughly investigate how hydrogen bonds affect the structure, dynamics, mechanics, and linear viscoelasticity of rubber materials. As the modified repeating unit ratio (β) increased, both interchain and intrachain hydrogen bond content rose, with interchain bonds playing a predominant role. This physical cross-linking network formed through interchain hydrogen bonds restricts molecular chain movement and relaxation and raises the glass transition temperature of rubber. Within a certain content of hydrogen bonds, the mechanical strength increases with increasing β. However, further increasing β leads to a subsequent decrease in the mechanical performance. Optimal mechanical properties were observed at β = 6%. On the other hand, a higher β value yields an elevated stress relaxation modulus and an extended stress relaxation plateau, signifying a more complex hydrogen-bond cross-linking network. Additionally, higher β increases the storage modulus, loss modulus, and complex viscosity while reducing the loss factor. In summary, this study successfully established the relationship between the structure and properties of natural rubber containing hydrogen bonds, providing a scientific foundation for the design of high-performance rubber materials.

Honey induces changes in the molecular structure and microstructure of gluten in wheat-rye sourdoughs.

Chemical oxidizers and redox enzymes have traditionally been used to enhance the quality of baked goods. However, consumers now seek natural and clean-label ingredients, avoiding those with chemical-sounding names. Honey, a natural source of glucose oxidase (GOX), represents a promising alternative to purified enzymes for baking purposes. This study aimed to evaluate the effect of honey on the molecular structure and microstructure of gluten proteins in sourdough fermented by different lactic acid bacteria (LAB) strains. Four wheat-rye (1:1) sourdoughs were prepared, each supplemented with honey and inoculated with a different LAB strain. Additionally, two uninoculated doughs, one with honey (honey dough) and the other without (control dough), were prepared under identical conditions. Electronic paramagnetic resonance spectroscopy revealed the presence of hydrogen peroxide in honey solutions, indicating its role as an active source of GOX. Raman spectroscopy showed that honey addition altered the molecular structure of gluten by increasing the proportion of random coils at the expense of α-helix structures. This change is likely attributed to the competition between honey sugars and gluten proteins for water molecules in this system. Moreover, honey led to a decrease in the free sulfhydryl content of gluten compared to the control dough, suggesting an increase in disulfide crosslinking points. These enhanced protein-protein interactions were observed in scanning electron microscopy micrographs as a coarse gluten network composed of interconnected strands and fibrils. All LAB strains exhibited optimal acidification (pH < 4.3) in honey-supplemented sourdoughs, promoting the hydrolysis of gluten proteins into smaller fragments. Overall, honey-supplemented sourdoughs showed a gradual increase in the β-sheet content while decreasing the proportion of random coils over time. This trend suggests that the polypeptide fragments interacted through interchain hydrogen bonds, leading to a more ordered structure, which likely contributes to providing dough with good baking aptitude.

Effect of incorporated amide blocks on the glass transition in polyesteramides

Incorporation of amide blocks is a common strategy used to promote the thermal and mechanical performances of polyesteramides. Meanwhile, glass transition temperature (Tg) is often used as one of the key parameters for measuring their physiochemical properties. Using a classical molecular dynamics approach, the Tg values of polyesteramides with a varying amide content are predicted by distinguishing their density variations with temperature. The predicted Tg values are in agreement with the measurements with an overestimation of about 2.6–6.5%. The incorporation of amide blocks favors the formation of interchain hydrogen bonds (HB). Although the relationship between Tg and HB formation has been well established, our simulations reveal that the entanglement of polyesteramide backbones leads to the Tg reduction at a high amide content, which is caused by the interplay between inter- and intra-chain HB numbers. The revealed molecular mechanism of Tg dependence on amide addition is helpful for the molecular design of functional polyesteramides.

Study of Cellulose Dissolution in ZnO/NaOH/Water Solvent Solution and Its Temperature-Dependent Effect Using Molecular Dynamics Simulation.

Cellulose is a biopolymer with numerous advantages that make it an ecological, economical, and high-performing choice for various applications. To fully exploit the potential of cellulose, it is often necessary to dissolve it, which poses a current challenge. The aqueous zinc oxide/sodium hydroxide (ZnO/NaOH/Water) system is a preferred solvent for its rapid dissolution, non-toxicity, low cost, and environmentally friendly nature. In this context, the behavior of cellulose chains in the aqueous solution of ZnO/NaOH and the impact of temperature on the solubility of this polymer were examined through a molecular dynamics simulation. The analysis of the root means square deviation (RMSD), interaction energy, hydrogen bond curves, and radial distribution function revealed that cellulose is insoluble in the ZnO/NaOH solvent at room temperature (T = 298 K). Decreasing the temperature in the range of 273 K to 268 K led to a geometric deformation of cellulose chains, accompanied by a decrease in the number of interchain hydrogen bonds over the simulation time, thus confirming the solubility of cellulose in this system between T = 273 K and T = 268 K.

Preparation and characterization of Pickering emulsion gel stabilized by WPI/SPI composite particles and encapsulation of milk-derived peptide FDRPFL

In this study, Pickering emulsion (PE) stabilized by whey protein isolate/soybean protein isolate (WPI/SPI) composite particles were used as a template to construct Pickering emulsion gel (PEG). The results showed that the PE stabilized by WPI/SPI composite particles had good centrifugal and storage stability at 4 °C (at least 4 months). Furthermore, When SA concentration was 3% and PE:SA ratio of 5:1, the obtained PEG with water-in-oil type exhibited a smaller droplet size, a denser network structure, and solid-like behavior in the linear viscoelastic region using a laser particle size analyzer, rheometer, and confocal laser scanning microscopy. Moreover, the increase of hydrogen bonds after SA addition confirmed that increased of β-sheet in WPI/SPI by Fourier-transform infrared spectroscopy, as β-sheet structure was stabilized by interchain hydrogen bonds, thus forming a denser network structure. In addition, PEGs could effectively encapsulate peptide FDRPFL, with a highest encapsulation efficiency of 72.8%. In vitro digestion behavior revealed that PEGs could improve the bioaccessibility of peptide FDRPFL and mainly followed the release mechanism of non-Fickian superstate II. Taken together, the present findings provide a theoretical framework for the development and application of PEGs stabilized by WPI/SPI composite particles.

Molecular Simulation Study of the Kinetics and Mechanism of Micellization of Charged and Uncharged Block Copolymer in Aqueous Solution: Polystyrene-Block-Poly(acrylic acid) PS-b-PAA

The micellization kinetics, dynamics, and diffusional properties of poly(styrene)-block-poly(acrylic acid) copolymer chains in salt-free aqueous solution have been investigated as a function of the copolymer composition (XPS ) for the cases of un-ionized (charge density f = 0) and ionized PAA blocks (charge density f = 1), for the first time to our knowledge via atomistic molecular dynamic simulations. The micelle formation mechanism was inspected by tracking the population of unimers and clusters across the simulation trajectory; it confirmed that the asymmetric copolymer micelle formation followed a combined approach of unimer insertion and cluster fusion mechanisms, while symmetric micelle formation followed the unimer insertion method exclusively. Micelle formation took a longer time for copolymers having charged (ionized) PAA blocks (f > 0) and relatively short PS blocks (number fraction of PS repeat units in copolymer XPS < 0.5) due to the presence of a greater number of hydrophobic groups, in agreement with the micellization kinetics observed for model copolymer micelles via DPD (Dissipative Particle Dynamics) simulation studies in literature. The conformational dynamics were studied using the relaxation of backbone dihedral angles and radius of gyration, for the core and corona blocks, respectively, showed that the PS blocks relaxed slower as compared to the soluble PAA blocks in solution due to their hydrophobic nature. The conformational relaxation time increased linearly for the PS blocks and was invariant for the PAA blocks with respect to XPS. The interaction dynamics of the PS-b-PAA copolymer micelles studied via the relaxation times of the PAA-PAA inter-chain (τHB,PP) and PAA-water inter-molecular hydrogen bonds (τHB,PW) showed the increase of τHB,PP, and the decrease of τHB,PW in solution with the increase in XPS. The PAA-water H-bond relaxes slower at f = 1 than that at f = 0 due to the stronger affinity of ionized PAA units with water molecules. The diffusivity of the copolymer chains decreased exponentially with an increase in XPS value, which is in agreement with the theoretical and experimental observations described in the literature.

Cross-linking manipulation of waterborne biodegradable polyurethane for constructing mechanically adaptable tissue engineering scaffolds.

Mechanical adaptation of tissue engineering scaffolds is critically important since natural tissue regeneration is highly regulated by mechanical signals. Herein, we report a facile and convenient strategy to tune the modulus of waterborne biodegradable polyurethanes (WBPU) via cross-linking manipulation of phase separation and water infiltration for constructing mechanically adaptable tissue engineering scaffolds. Amorphous aliphatic polycarbonate and trifunctional trimethylolpropane were introduced to polycaprolactone-based WBPUs to interrupt interchain hydrogen bonds in the polymer segments and suppress microphase separation, inhibiting the crystallization process and enhancing covalent cross-linking. Intriguingly, as the crosslinking density of WBPU increases and the extent of microphase separation decreases, the material exhibits a surprisingly soft modulus and enhanced water infiltration. Based on this strategy, we constructed WBPU scaffolds with a tunable modulus to adapt various cells for tissue regeneration and regulate the immune response. As a representative application of brain tissue regeneration model in vivo, it was demonstrated that the mechanically adaptable WBPU scaffolds can guide the migration and differentiation of endogenous neural progenitor cells into mature neurons and neuronal neurites and regulate immunostimulation with low inflammation. Therefore, the proposed strategy of tuning the modulus of WBPU can inspire the development of novel mechanically adaptable biomaterials, which has very broad application value.

Terahertz spectroscopy of interchain hydrogen bond changes of poly (L-lactic acid)/poly (D-lactic acid) blends during solution crystallization

The blending of poly (L-lactic acid) (PLLA) and poly (D-lactic acid) (PDLA) achieves an effective transformation of properties based on the formation of interchain hydrogen bonds. Therefore, it is important to study the stereo-complex (SC) system. We studied the solution crystallization of PLLA/PDLA blends based on the sensitivity of terahertz (THz) spectroscopy to hydrogen bonds. The results revealed an abnormal red-shift in the characteristic peak frequency of the blends with the increase of PLLA, which is attributed to the difference in chain stacking of the main components in the blends. Moreover, we believe that the peak height of the SC at 1.43 THz is an accurate index reflecting the interchain hydrogen bonds in the case of blending ratio changes. When the blend ratio is determined, we found that the blue shift of this peak frequency corresponded to the weakening of interchain hydrogen bonds. The results show that THz spectroscopy can effectively observe the solution crystallization behavior of blends, and its different characteristic indexes contain the information of interaction and aggregation structure.

Crystal structure of polymeric bis-(3-amino-1H-pyrazole)-cadmium dibromide.

The reaction of cadmium bromide tetra-hydrate with 3-amino-pyrazole (3-apz) in ethano-lic solution leads to tautomerization of the ligand and the formation of crystals of the title compound, catena-poly[[di-bromido-cadmium(II)]-bis-(μ-3-amino-1H-pyrazole)-κ2 N 3:N 2;κ2 N 2:N 3], [CdBr2(C3H5N3)2]n or [CdBr2(3-apz)2]n. Its asymmetric unit consists of a half of a Cd2+ cation, a bromide anion and a 3-apz mol-ecule. The Cd2+ cations are coordinated by two bromide anions and two 3-apz ligands, generating trans-CdN4Br2 octa-hedra, which are linked into chains by pairs of the bridging ligands. In the crystal, the ligand mol-ecules and bromide anions of neighboring chains are linked through inter-chain hydrogen bonds into a two-dimensional network. The inter-molecular contacts were qu-anti-fied using Hirshfeld surface analysis and two-dimensional fingerprint plots, revealing the relative qu-anti-tative contributions of the weak inter-molecular contacts.

Understanding the Molecular Mechanisms of Polyphenol Inhibition of Amyloid β Aggregation.

Alzheimer's disease (AD) is highly associated with self-aggregation of amyloid β (Aβ) proteins into fibrils. Inhibition of Aβ aggregation by polyphenols is one of the major therapeutic strategies for AD. Among them, four polyphenols (brazilin, resveratrol, hematoxylin, and rosmarinic acid) have been reported to be effective at inhibiting Aβ aggregation, but the inhibition mechanisms are still unclear. In this work, these four polyphenols were selected to explore their interactions with the Aβ17-42 pentamer by molecular dynamics simulation. All four polyphenols can bind to the pentamer tightly but prefer different binding sites. Conversion of the β-sheet to the random coil, fewer interchain hydrogen bonds, and weaker salt bridges were observed after binding. Interestingly, different Aβ17-42 pentamer destabilizing mechanisms for resveratrol and hematoxylin were found. Resveratrol inserts into the hydrophobic core of the pentamer by forming hydrogen bonds with Asp23 and Lys28, while hematoxylin prefers to bind beside chain A of the pentamer, which leads to β-sheet offset and dissociation of the β1 sheet of chain E. This work reveals the interactions between the Aβ17-42 pentamer and four polyphenols and discusses the relationship between inhibitor structures and their inhibition mechanisms, which also provides useful guidance for screening effective Aβ aggregation inhibitors and drug design against AD.

Fully atomistic molecular dynamics simulation of chemically modified natural rubber with hydrogen-bonding network

The incorporation of sacrificial hydrogen bonds is critical for the development of rubber materials with exceptional properties. However, the molecular-level mechanism by which sacrificial hydrogen bonds affect material properties is still poorly understood, significantly hindering the advancement of high-performance rubber materials. In this study, we employ fully atomistic molecular dynamics simulations to elucidate the impact of hydrogen bonds on structure, mechanical properties and linear viscoelasticity. Increasing the modified repeating unit ratio α leads to a rise in hydrogen bond content, particularly inter-chain hydrogen bonds, and the modified groups cluster due to hydrogen bonds. This hydrogen bond crosslinking network constrains the movement of the molecular chains, increasing the glass transition temperature. Surprisingly, the mechanical properties show an initial increase followed by a decrease as α increases, and the system with α=6% exhibits the optimal mechanical properties. This trend is due to the regulation of mechanical properties by the non-bond energy increment and bond orientation, with the system with α=6% exhibiting the maximum non-bonded energy increment and bond orientation. Increasing the self-healing temperature and time improves self-healing efficiency, essentially governed by the diffusion of molecular chains. The system with higher α exhibits a higher stress relaxation modulus and more extended stress relaxation plateau, attributable to a more complex hydrogen bond crosslinking network. Additionally, higher α values result in higher energy storage modulus, loss modulus, and complex viscosity but can effectively reduce the loss factor. Therefore, adjusting α can achieve a material with robust mechanical properties and low mechanical losses. Overall, we successfully establish the relationship between structure and properties and guide the designing and synthesizing of rubber materials with even better properties.

Bridging Biocondensation and Biomimetic Fibrillation by Regulating Intra- And Interchain Hydrogen Bonds in Artificial Biomacromolecular Condensates.

Utilizing biocondensates as feedstocks can be a state-of-the-art strategy for emulating natural silk spinning. Although current biocondensates can form solid fibers using a biomimetic draw spinning method, the fibrillation is primarily achieved through evaporation of highly concentrated biocondensates rather than structural conversion in natural spinning. Current artificial biocondensates lack biomimetic features of stress-induced fibrillation since they are unable to replicate the structural complexity of native proteins in the dope. Herein, we successfully achieved biomimetic fibrillation at significantly reduced concentrations by constructing artificial biocondensates using naturally derived silk fibroin. The biomimetic features of stress-induced fibrillation in native proteins are replicated in our artificial biocondensates by tailoring multivalent interactions in biocondensation. Our findings unravel the fundamental correlations between biocondensation and stress-induced fibrillation. This work can not only provide a framework for designing artificial biocondensates in biomimetic spinning but also improve the molecular insights into natural spinning.

Secondary structure in polymorphic forms of alpha-synuclein amyloids.

Numerous Alpha-synuclein amyloid structures available in PDB enable their comparative analysis. They are all characterized by a flat structure of each individual chain with an extensive network of inter-chain hydrogen bonds. The identification of such amyloid fibril structures requires determining the special conditions imposed on the torsion angles. Such conditions have already been formulated by the Authors resulting in the model of idealised amyloid. Here, we investigate the fit of this model in the group of A-Syn amyloid fibrils. We identify and describe the characteristic supersecondary structures in amyloids. Generally, the amyloid transformation is suggested to be the 3D to 2D transformation engaging mostly the loops linking Beta-structural fragments. The loop structure introducing the 3D organisation of Beta-sheet change to flat form (2D) introduces the mutual reorientation of Beta-strands enabling the large-scale H-bonds generation with the water molecules. Based on the model of idealised amyloid we postulate the hypothesis for amyloid fibril formation based on the shaking, an experimental procedure producing the amyloids.

High intrinsic thermal conductive polymer films by engineered interchain hydrogen bond interactions

AbstractA series of polyvinyl alcohol (PVA) composite films containing different hydrogen bond acceptors 4,4′‐dihydroxydiphenyl (BP), 1,1′‐biphenyl‐4,4′‐diyl dihexanoate (DHB) and benzene‐1,3,5‐triyl tribenzoate (TBB) were prepared by casting method. Due to the existence of strong intermolecular interaction, the highest in‐plane thermal conductivity of the above films is 1.298 Wm−1 K−1, which is about 65% higher than pure PVA films. Fourier Transform infrared spectroscopy (FT‐IR) and wide‐angle X‐ray diffraction (WXAD) demonstrated that the TBB acts as a thermal bridge to enhance the internal interaction force and make the internal structure more regular. Strong molecular contact forces were demonstrated by mechanical tensile testing. The thermal expansion rate of the system was explored through molecular dynamics. Thermal expansion experiments proved that hydrogen bond can effectively reduce the free volume. Molecular dynamics simulations were also performed in this work. The number and density of hydrogen bonds inside different polymers were calculated, and the phonon thermal transport was quantitatively analyzed. The thermal bridge and intermolecular contact force were discovered to effectively restrict the molecular chain's activity and reduce its free volume. The results of the experiments and molecular dynamics reveal that strong intermolecular interactions and thermal bridges can significantly improve polymer intrinsic thermal conductivity.