Semi-interpenetrating Polymer Network Research Articles

Smart Crowding on pH-Induced Elasticity of Weakly Anionic poly(N-Isopropylacrylamide)-Based Semi-Interpenetrating Polymer Networks via Integration of Methacrylic Acid and Linear Polyacrylamide Chains.

Weakly anionic semi-interpenetrating polymer networks (semi-IPNs), comprised of copolymer poly(N-isopropylacrylamide-co-methacrylic acid) P(NIPA-MA) and linear poly(acrylamide) (LPA) chains as macromolecular crowding agent, are designed to evaluate pH-induced swelling and elasticity. Uniaxial compression testing after swelling in various pH-conditions is used to analyze the compressive elasticity as a function of swelling pH and LPA-content. The swelling of P(NIPA-MA)/LPA semi-IPNs is strongly pH-dependent due to MA units incorporated into the copolymer network which already exhibits temperature-sensitivity by presence of PNIPA counterpart. Since the behavior of semi-IPNs is a combination of PMA, LPA, and PNIPA moieties, the sensitivity of swelling to external pH can be modified with increasing swelling temperature. At high pH conditions, LPA-doped semi-IPNs show elasticity representing soft and loosely cross-linked structure. Elastic modulus is higher in acidic pH condition due to the less swelling tendency, while in basic pH, the modulus decreases significantly in coordination with swelling. Oscillatory swelling reveals how fast semi-IPNs can respond to environmental pH change (2.1-10.7). By describing adsorption potential of semi-IPNs for cationic methylene blue uptake by pseudo-first-order and Freundlich model, the designed poly(NIPA-MA)/LPA semi-IPNs emerge as promising smart materials in applications requiring rapid response to changes in temperature and pH via diffusional properties.

Robust liquid crystal semi-interpenetrating polymer network with superior energy-dissipation performance.

Liquid crystal networks (LCN) have attracted surging interest as extraordinary energy-dissipation materials owning to their unique dissipation mechanism based on the re-orientation of mesogens. However, how to integrate high Young's modulus, good dissipation efficiency and wide effective damping temperature range in energy-dissipation LCN remains a challenge. Here, we report a strategy to resolve this challenge by fabricating robust energy-dissipation liquid crystal semi-interpenetrating polymer network (LC-semi-IPN) consisting crystalline LC polymers (c-LCP). LC-semi-IPN demonstrates a superior synergistic performance in both mechanical and energy-dissipation properties, surpassing all currently reported LCNs. The crystallinity of c-LCP endows LC-semi-IPN with a substantial leap in Young's modulus (1800% higher than single network). The chain reptation of c-LCP also promotes an enhanced dissipation efficiency of LC-semi-IPN by 200%. Moreover, its effective damping temperature reaches up to 130 °C, which is the widest reported for LCNs. By leveraging its exceptional synergistic performance, LC-semi-IPN can be further utilized as a functional architected structure with exceptional energy-dissipation density and deformation-resistance.

Vinylic-addition Polynorbornene-based Anion-Exchange Membranes with Semi-Interpenetrating Polymer Networks for Water Electrolysis

Vinylic-addition Polynorbornene-based Anion-Exchange Membranes with Semi-Interpenetrating Polymer Networks for Water Electrolysis

Folic acid conjugated sodium alginate based redox responsive smart functional microgels as a potential targeted anticancer drug carrier

In this study, we have fabricated a sodium alginate-based redox-responsive, and cancer cell-targeted specific microgel using a water in oil (w/o) mini emulsion process and characterized it accordingly. Initially, we synthesized folic acid (FA)-grafted sodium alginate (SA), a biocompatible polysaccharide, followed by the preparation of a semi-interpenetrating polymer network (semi-IPN) microgel by crosslinking polyacrylamide (PAAm) with a disulfide crosslinker. The presence of disulfide linkages in the microgel formulation accelerated the release of the anti-cancer drug Doxorubicin (DOX) in the reducing domain of cancer cells (in vitro) (cumulative drug release amount 11 ± 3 %). Folic acid was incorporated into the microgels to enhance its targeting towards cancer cells due to the presence of the folate receptor on cancer cells. MTT (3-(4,5-dimethylthiazolyl-2)-2, 5-diphenyltetrazolium bromide) assay showed an IC50 of ∼30 μg/mL of the DOX-loaded microgels towards breast cancer cells (MDA-MB-231) and a nontoxic behaviour towards normal mouse fibroblast cells (L929). FACS (Fluorescence-Activated Cell Sorting) and cell uptake studies showed significant cell apoptosis upon application of the drug-loaded microgels. In our opinion, this type of microgel can be a potential drug delivery vector for cancer treatment.

Green synthesis of multifunctional responsive hydrogel embedded with silver, based on xanthan gum, N-isopropylacrylamide, vinyl imidazole, and Luffa cylindrica for wound healing

In this study, a pH- and temperature-responsive smart hydrogel was developed by utilizing Xanthan Gum (XG), N-Isopropylacrylamide (NIPAM), Vinyl Imidazole (VI), and Luffa cylindrical (LC). Semi-interpenetrating polymer networks (semi-IPNs) were created using free radical polymerization with N,N′-methylenebisacrylamide (MBA) as the cross-linker and ammonium persulfate (APS) as the initiator. Silver nanoparticles (AgNPs) were synthesized within semi-IPN hydrogel network structures to impart antibacterial properties. Malva sylvestris (MS) aqueous leaf extract was used as a reducing and stabilizing agent for the green synthesis of the AgNPs. The semi-IPN hydrogels exhibited pH- and temperature-responsive swelling behavior, which also enabled the controlled release of the drug. After 11 h, the cumulative release reached approximately 73% at pH 7.2 and 87% at pH 8.3. Additionally, the sustained release mechanism of the Trimethoprim drug was described using the Korsmeyer-Peppas model and was governed by Fickian diffusion. The drug-loaded semi-IPN@Ag nanocomposite hydrogel has demonstrated effective antibacterial activity against various Gram-negative and Gram-positive bacteria, indicating its promising potential as a wound dressing material for reducing infection risk.

Antibacterial Biocomposite Based on Chitosan/Pluronic/Agarose Noncovalent Hydrogel: Controlled Drug Delivery by Alginate/Tetracycline Beads System.

Designing a wound dressing with controlled uptake, antibacterial, and proper biocompatibility is crucial for the appropriate wound healing process. In this study, alginate/tetracycline (Alg/TC) beads were produced and embedded into chitosan/pluronic/agarose semi-interpenetrating polymer network hydrogel, which serves as a potential biocompatible dressing for treating skin wounds. The effect of pluronic content on the porosity, swelling, mechanical characteristics, and degradation of the hydrogel was investigated. Furthermore, the impact of Alg beads on TC release was subsequently examined. In the absence of Alg beads, faster release was observed. However, after incorporating beads into the hydrogels, the release was sustained. Particularly, the hydrogel containing Alg beads exhibited a nearly linear release, reaching 74% after 2 days in acidic media. The antimicrobial activity and biocompatibility of the hydrogel were also evaluated to assess the capability of the TC-loaded hydrogels for wound dressing applications. The hydrogel demonstrated efficient antibacterial features against Gram-positive and Gram-negative bacteria. Additionally, the sample behavior was evaluated against exposure to yeast. Furthermore, based on biocompatibility studies using HFF2 cells, the TC-loaded hydrogel exhibited remarkable biocompatibility. Overall, this novel composite hydrogel shows remarkable biocompatibility and antibacterial activities which can be used as a great potential wound dressing to prevent wound infections due to its effective inhibition of bacterial growth.

Electrically conductive functionalization of cured polyether ether ketone with improved bioactivity by surface-polymerization of polyaniline

The electrically conductive polyether ether ketone (PEEK) holds great promise for antibacterial and cell growth promotion under electrical stimulation, making it a promising material for next-generation implants. However, it is a significant challenge for electrically conductive functionalization of PEEK, especially for cured or shaped PEEK. In addition, PEEK’s bioactivity is still underdeveloped at present. Here, an electrically conductive PEEK with improved bioactivity is prepared through surface-polymerization of polyaniline (PANI) in the shell layer of cured PEEK. Impressively, an extremely high conductivity of 5.2 × 10−2 S/cm is achieved for the conductive PEEK among all the reported PANI/PEEK composites or blends with the optimal conductivity of 3.0 × 10−4 S/cm. It has been demonstrated that the conductive shell layer of the conductive PEEK features a PANI/PEEK semi-interpenetrating polymer network structure, explaining its conductivity. Improved cell proliferative activity is also disclosed for the conductive PEEK compared to that of the pure PEEK, and good biocompatibility and osteogenesis properties are further confirmed for the fabricated conductive PEEK scaffold. This conductive functionalization approach offers a significant advancement for developing next-generation biological implants and could be applied to other cured polymers as well.

Facile fabrication of robust and tight PIMs-based TFC hollow fiber membranes with a semi-interpenetrating polymer network via liquid phase cross-linking for organic solvent nanofiltration

Resource recovery and reuse are essential for sustainable development, particularly for high-value resources such as homogeneous (photo)catalysts, active pharmaceutical ingredients, and high-value natural compounds, which can offer economic benefits. Recently, organic solvent nanofiltration (OSN) for resource recovery has gained significant attention owing to its advantages including low energy consumption and seamless integration with other processes. Polymers of intrinsic microporosity (PIMs) have great potential as membrane materials for OSN, owing to their excellent pore properties and solution processability. However, swelling and dissolution of PIMs in organic solvents can impede the filtration performance of PIMs-based OSN membranes. In this study, we fabricated thin-film composite hollow fiber membranes for OSN based on PIMs with improved organic solvent stability using a semi-interpenetrating polymer network (semi-IPN) formed by cross-linking Matrimid with 1,6-hexanediamine within the PIMs through the liquid phase cross-linking method. Semi-IPNs mitigate swelling and tighten the pores of PIMs-based membranes, enabling excellent filtration and molecular separation performance. Furthermore, the fabricated PIMs with a semi-IPN membrane exhibited excellent rejection performance (>96 %) for homogeneous photocatalysts, allowing successful concentration and recovery via OSN. Therefore, PIMs-based membranes with a semi-IPN hold great promise as OSN membranes for the recovery of valuable resources.

Injectable and 3D Extrusion Printable Hydrophilic Silicone-Based Hydrogels for Controlled Ocular Delivery of Ophthalmic Drugs.

While silicone elastomers have found widespread use in the biomedical industry, 3D printing them has proven to be difficult due to the material's slow drying time, low viscosity, and hydrophobicity. Herein, we arrested the hydrophilic silicone (HS) macrochains into a semi-interpenetrating polymer network (semi-IPN) via an in situ photogelation-assisted 3D microextrusion printing technique. The flow behavior of the pregel solutions and the mechanical properties of the printed HS hydrogels were tested, showing a high elastic modulus (approximately 15 kPa), a low tan δ, high elasticity, and delayed network rupturing. The uniaxial compression tests demonstrated a nearly negligible permanent deformation, suggesting that the printed hybrid hydrogel maintained its elastic properties. Drug loading and diffusion in the microporous hydrogel are shown via the non-Fickian anomalous transport mechanism, leading to highly tunable loading/releasing profiles (approximately 20% cumulative release) depending on the HS concentration. The drug encapsulation exhibits exceptional stability, remaining intact without any degradation even after a storage period of 1 month. As far as we know, this is the first soft biomaterial based on HS that functions as an exceptional controlled drug delivery device.

Semi-IPN polysaccharide-based hydrogels for effective removal of heavy metal ions and dyes from wastewater: a comprehensive investigation of performance and adsorption mechanism.

The escalating issue of environmental pollutants necessitates efficient, sustainable, and innovative wastewater treatment technologies. This review comprehensively analyzes the mechanisms and isotherms underlying the adsorption processes of semi-interpenetrating polymer network (semi-IPN) polysaccharide-based hydrogels to remove heavy metal ions and dyes from wastewater. Polysaccharides are extensively utilized in hydrogel synthesis due to their biocompatibility, cost-effectiveness, and non-toxic nature. The synthesis of these hydrogels as semi-IPNs enhances their mechanical and structural robustness and adsorption capacity. This review explores the key parameters affecting adsorption performance, including pH, temperature, contact time, and adsorbent dosage. Findings highlight that semi-IPN polysaccharide-based hydrogels exhibit remarkable adsorption capabilities through electrostatic interactions, ion exchange, and surface complexation. Furthermore, this review highlights the distinct advantages of semi-IPNs over other polymer networks. Semi-IPNs offer improved mechanical stability, higher adsorption efficiencies, and better reusability, making them a promising solution for wastewater treatment. Detailed isotherm models, including Langmuir and Freundlich isotherms, were studied to understand these hydrogels' adsorption behavior and capacity for different pollutants. This study highlights the potential of semi-IPN polysaccharide-based hydrogels as effective adsorbents forheavy metals and dyes and as a promising solution for mitigating environmental pollution. The insights provided herein contribute to developing advanced materials forenvironmental remediation, aligning with global sustainability goals, and advancing wastewater treatment technology.

Functional Semi-Interpenetrating Polymer Networks.

Semi-interpenetrating polymer networks (SIPNs) have garnered significant interest due to their potential applications in self-healing materials, drug delivery systems, electrolytes, functional membranes, smart gels and, toughing. SIPNs combine the characteristics of physical cross-linking with advantageous chemical properties, offering broad application prospects in materials science and engineering. This perspective introduces the history of semi-interpenetrating polymer networks and their diverse applications. Additionally, the ongoing challenges associated with traditional semi-interpenetrating polymer materials are discussed and provide an outlook on future advancements in novel functional SIPNs.

Shape memory and mechanical properties of ESO modified epoxy/polyurethane semi-interpenetrating polymer networks for smart plaster

While numerous studies have explored the potential of shape memory materials in medical applications, the current research output is not enough for significant productivity in industrial products. In this research, a type of shape memory orthopedic plaster was fabricated by using epoxy/polyurethane interpenetrating networks modified with epoxidized soybean oil (ESO) and then compared with some commercial plasters. Polymer networks that were produced could be tailored to have glass transition temperatures (Tgs) within the range of 70–90 °C by changing the percentage composition of polyurethane and soybean oil. Shape recovery and fixity ratios in all samples were above 95 and 97 %. DMA results showed that IPNs with variable amount of soybean oil had lower glass transition temperature (Tg) and cross-link densities compared to IPNs without soybean oil. Based on the tensile test results, most samples exhibited an elastic modulus in the range of 280–400MPa, a level deemed somewhat acceptable when compared to commercial samples. Light microscope images had shown that the increase of polyurethane led to the phase separation of polymers, which was improved by the addition of soybean oil.

Temperature-Regulated Synthesis of Hyaluronic Acid-Interpenetrated Polyacrylamide/Poly(Acrylic Acid Sodium Salt) Semi-Interpenetrated Polymer Network Gel for the Removal of Methyl Violet.

An alternative synthetic pathway was proposed for the optimization of synthesis to find a better correlation between the swelling and elasticity of hyaluronic acid-interpenetrated gels via temperature regulation. An experimental design methodology was presented for the synthesis of polyacrylamide/poly(acrylic acid sodium salt)/hyaluronic acid, PAAm/PSA/HyA, gels by modifying the one-pot procedure using free radical crosslinking copolymerization of AAm with the addition of anionic linear PSA chains in the presence of various amount of HyA, ranging between 0.05% and 0.20% (w/v). Semi-interpenetrated polymer network (IPN)-structured gels were designed with tunable elasticity, in which the extent of covalent crosslinking interactions is controlled by polymerization temperature ranging between -18 and 45 °C. Depending on the HyA content added in the synthesis and the polymerization temperature, the swelling ratio could be controlled. The addition of 0.05% (w/v) HyA increased the swelling of semi-IPNs, while the elastic modulus increased with increasing HyA content and decreased with the polymerization temperature. PAAm/PSA/HyA semi-IPNs showed the typical pH-sensitive swelling of anionic gels, and the swelling reached a maximum at a pH of 11.2. PAAm/PSA/HyA gels were tested for the removal of methyl violet from wastewater. Adsorption kinetics were shown to be well-fitted with the pseudo-second-order model using linear and nonlinear regression analysis. With the clear relationship between increased modulus and composition, this study enabled the fine-tuning of semi-IPN interactions by varying the polymerization temperature.

Enhancing mechanical and thermal properties of blends with novel phenylethynyl-terminated siloxane-containing ortho-hydroxy polyimide

A novel phenylethynyl-terminated siloxane-containing ortho-hydroxy polyimide (O-SPI) was synthesized and physically blended with thermoplastic polyimide (PI) to enhance both the thermal and mechanical properties of polyimide, addressing the growing demand for high-performance materials in harsh environments. The blend underwent conversion to semi-Interpenetrating Polymer Networks ( semi-IPNs) and benzoxazole structures through thermal curing of reactive phenylethynyl groups and thermal rearrangement of ortho-hydroxy imide units. The trends in thermal and mechanical properties were investigated in relation to the chemical structures and varying mass fraction of O-SPI. The covalent incorporation of semi-IPNs and rigid benzoxazole structures restrict segmental motion while the backbone linkage confers the toughness of the blends. These synergistic effects insure the cured blends with high glass transition temperatures (472.51°C) and tensile strength (117.81 MPa) simultaneously, demonstrating their potential for applications in challenging conditions.

Rational Design of Hybrid Electrolyte for All-Solid-State Lithium Battery Based on Investigation of Lithium-Ion Transport Mechanism

Lithium-ion batteries (LIBs) are widely used in various applications, including personal electronic devices, electric vehicles, and energy storage systems. Given the increasing demand for LIBs, there is need to develop rechargeable batteries with high energy densities, long cycle life, and enhanced safety. Lithium all-solid-state batteries (ASSBs) could improve operational safety by eliminating flammable liquid electrolytes and using non-flammable solid electrolytes. Among the various types of solid electrolytes explored, solid polymer electrolytes (SPEs) have garnered significant attention owing to their desirable properties, such as good processability, light weight, flexibility, and favorable interfacial contact with the electrodes. To develop practical battery systems using SPEs, improving the ionic conductivity mechanism of lithium-ion (Li+) in SPEs is crucial. Li+ transport mechanism of SPE is typically known as segmentation motion and ion hopping. In SPE, crystalline and amorphous phases coexist, and movement of Li+ occurs mainly in the amorphous phase. Therefore, the use of SPE at high temperatures improves ionic conductivity, but still that have limitation by low ionic conductivity (10-7~ 10-8 S cm-1) at ambient temperatures, low Li+ transference numbers, a restricted electrochemical window, and low mechanical strength. Hybrid polymer electrolytes (HPEs) combine an inorganic ceramic electrolyte (ICE) and SPE to create a ceramic-in-polymer or a polymer-in-ceramic hybrid and have improved ionic conductivity and mechanical stability compared to SPE. Ceramic materials of HPE can be classified into oxide-based materials and NASICON-type materials. Oxide-based materials such as SiO2, Al2O3, etc. induce an increase in the amorphous area of PEO and improve segmental mobility by preventing recrystallization of the polymer, thereby increasing ionic conductivity. NASICON-type materials, such as Li7La3Zr2O12 (LLZO), Li1+xAlxTi2-x(PO4)3 (LATP), etc. are promising candidates for improving ionic conductivity by increasing the mobility of Li+ because they form ionic conductive channels within the ceramic bulk. However, despite the observed improvements in performance, the Li+ ion transport mechanism in HPEs and its correlation with the electrochemical cell results remain unclear.In this study, we present a new approach to improve the performance of ASSB by establishing the Li+ transport mechanism through a designed HPE system proven through experimental results and density functional theory (DFT) calculations. To achieve high energy density ASSB, LiNi0.8Co0.1Mn0.1O2 (NCM811) Li ASSB cell was applied, and through a combination of experiment and DFT calculation, HPE was manufactured by PEO-based semi-interpenetrating polymer network (semi-IPN) SPE and Li1+xAlxTi2-x(PO4)3 (LATP) of NASICON-type. As a result, we confirmed that Li+ migrates through the interface of SPE and LATP, which has a significant effect on the improved ionic conductivity (7.23 × 10-4 S cm-1 at 45 ℃). In addition, it was confirmed that Li dendrites were suppressed and cycle performance were improved due to the improved physical strength of the electrolyte with the addition of ceramics. This suggests a promising design strategy for high-performance Li ASSB.

Semi-Interpenetrating Polymer Network Anion Exchange Membranes Based on Quaternized Polybenzoxazine and Poly(Vinyl Alcohol-Co-Ethylene) for Acid Recovery by Diffusion Dialysis.

Acid recovery from acidic waste is a pressing issue in current times. Chemical methods for recovery are not economically feasible and require significant energy input to save the environment. This study reported a semi-interpenetrating polymer network (semi-IPN) anion exchange membranes (AEMs) for acid recovery by diffusion dialysis with excellent dimensional stability, high oxidation stability, good acid dialysis coefficient (UH +) and high separation factor (S). Semi-IPN AEMs are prepared by ring-open cross-linked quaternized polybenzoxazine (AQBZ) with poly(vinyl alcohol-co-ethylene), where AQBZ is obtained by Mannich reaction and Menshutkin reaction. All four proportions of semi-IPNs exhibit clear micro-phase separation, which is conducive to ion transport. The water uptake (WU) of the four semi-IPNs ranges from 14.2 % to 19.2 %, while the swelling ratio (SR) remains between 8.7 % and 11.3 %. These results indicate that the cross-linked structure in the designed semi-IPNs effectively control swelling and ensure dimensional stability. The thermal degradation temperature (Td5) of semi-IPN4:6 to semi-IPN7:3 varies from 309 °C to 289 °C, with an oxidation stability weight loss rate (WOX) ranging from 91.5 % to 93.5 %, demonstrating excellent thermal stability and oxidation stability. The semi-IPNs also show good UH + values ranging from 11.9-16.3*10-3 m/h and high S values between 38.6 and 45.9, indicating the promising potential of the semi-IPNs.

Preparation and characterization of agarose-sodium alginate hydrogel beads for the co-encapsulation of lycopene and resveratrol nanoemulsion

In the study, lycopene and resveratrol nanoemulsion hydrogel beads were prepared by using agarose‑sodium alginate as a carrier and the semi-interpenetrating polymer network technique, characteristics and morphologies were evaluated by scanning electron microscopy, fluorescence microscopy, rheological measurement. The synergistic antioxidant effect of lycopene and resveratrol was confirmed, the best synergistic antioxidant performance is achieved when the ratio of 1:1. To increase the solubility and improve the stability, the lycopene was prepared as solid dispersion added to the nanoemulsion. The encapsulation rate of lycopene and resveratrol reached 93.60 ± 2.94 % and 89.30 ± 1.75 %, respectively, and the cumulative release showed that the addition of agarose slowed down the release rate of the compound, which improves the applicability of lycopene and resveratrol and development of carriers for the delivery of different bioactive ingredients.

Dimensionally stable cellulose acetate-chitosan semi-interpenetrating polymer network as fuel cell anion exchange membrane

Dimensionally stable cellulose acetate-chitosan semi-interpenetrating polymer network as fuel cell anion exchange membrane

Dual crosslinked interpenetrating polymer network-based porous hydrogel membrane for solid-state supercapacitor applications

Hydrogel membranes have emerged as promising candidates for solid-state supercapacitors (SSCs), overcoming limitations associated with traditional liquid electrolytes like leakage, thermal hazards, and flammability. However, single-network hydrogels often suffer from poor mechanical properties, making them inadequate for wearable applications. Herein, solution casting technique is used to develop a novel dual-crosslinked semi-interpenetrating polymer network (semi-IPN) hydrogel membrane through in-situ polymerisation of acrylic acid (AA) in a polyvinyl alcohol (PVA) matrix, followed by doping with KOH solution. By adjusting the composition between PVA and AA, the phase separation pathway is controlled, resulting in a homogeneously distributed porous architecture that enhances ion-conductive pathways. The hydrogel exhibited excellent properties, including high ionic conductivity (174 mS cm−1), considerable tensile strength (5 MPa), and significant elongation at break (460 %). Dielectric studies confirmed its significantly improved capacitive behaviour and low conductivity relaxation characteristics. Additionally, the resulting pseudocapacitor assembled with graphite-silvernanowire-polyaniline based composite electrode demonstrated a high specific capacitance (302 F g−1 at 0.2 A g−1) with outstanding capacity retention (75 % up to 500 cycles). Overall, the incorporation of this novel material provides great potential for high-performance SSC applications.

Morphology-controlled metal–organic frameworks as molecular traps for enhanced ion dynamics in practical semi-solid lithium metal batteries

Controlling electrostatic interactions between charged molecules is crucial to enabling advanced batteries with reliable lithium (Li)-ion conductors. To address this issue, herein, we present a class of morphology-controlled metal–organic frameworks (MOFs) that serve as Li+ boosting molecular traps for fast Li+ conduction. A rod-like MOF is incorporated into semi-interpenetrating polymer networks to construct Li+ boosting fluidic nanochannels, which enable fast Li+ transport (σ = 1.5 mS cm−1, tLi+ = 0.76) through the ionic pathway. Molecular dynamics simulations further elucidate the Li+ transport mechanism in these MOF-based molecular traps. This unusual Li+ conduction behavior of MOF-based semi-solid electrolytes suppresses the anion-triggered ion concentration gradient and facilitates the electrochemical reaction kinetics at the electrodes, ultimately improving the rate performance and cycling retention of Li-metal cells (consisting of LiNi0.7Co0.2Mn0.1O2 cathodes and Li-metal anodes). Notably, a scalable pouch-type semi-solid Li-metal cell provides stable cycling performance for realistic batteries, exceeding those of previously reported Li batteries including porous crystalline frameworks.