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We herein report the fabrication of a Velcro-mimicking surface based on polymer brushes. Using poly(ε-caprolactone) (PCL) as the model polymer, polymer loop brushes (PLBs) and singly tethered polymer brushes (STPBs) with nearly identical tethering point density and brush heights were synthesized using a polymer single crystal (PSC)-assisted grafting-to method. Atomic force microscopy-based single molecular force spectroscopy (AFM-SMFS) and macroscale lap-shear experiments both demonstrated that the PLBs led to strong adhesion that is up to ∼10 times greater than the STPBs, which is attributed to the enriched chain entanglement between the probing polymer and the brushes. We envisage that our results will pave the way towards a new materials design for strong adhesives and nanocomposites. 

Nanocomposite polymer electrolytes (CPEs) are promising materials for all-solid-state lithium metal batteries (LMBs) due to their enhanced ionic conductivities and stability to the lithium anode. MXenes are a new two-dimensional, 2D, family of early transition metal carbides and nitrides, which have a high aspect ratio and a hydrophilic surface. Herein, using a green, facile aqueous solution blending method, we uniformly dispersed small amounts of Ti 3 C 2 T x into a poly(ethylene oxide)/LiTFSI complex (PEO 20 -LiTFSI) to fabricate MXene-based CPEs (MCPEs). The addition of the 2D flakes to PEO simultaneously retards PEO crystallization and enhances its segmental motion. Compared to the 0D and 1D nanofillers, MXenes show higher efficiency in ionic conductivity enhancement and improvement in the performance of LMBs. The CPE with 3.6 wt% MXene shows the highest ionic conductivity at room temperature (2.2 × 10 −5 S m −1 at 28 °C). An LMB using MCPE with only 1.5 wt% MXene shows rate capability and stability comparable with that of the state-of-the-art CPELMBs. We attribute the excellent performance to the 2D geometry of the filler, the good dispersion of the flakes in the polymer matrix, and the functional group-rich surface. 

Incorporating solid polymer electrolyte (SPE) into lithium metal batteries has the benefit of employing the electrolyte as the electrode separator while inhibiting the growth of lithium dendrites. The two main models on lithium dendrite growth show that either ionic conductivity or mechanical property affect lithium dendrite nucleation and growth rate. In this work, with a well‐controlled hybrid network SPE as the model system, the modulus and conductivity of the hybrid SPEs are systematically tuned by plasticizing the network with low molecular with diluents. This systematic property control allows for establishing the correlation between mechanical/electrochemical properties of the SPEs with their propensity of lithium dendrite resistance using galvanostatic polarization and cycling experiments. It is further demonstrated that lithium metal batteries can be operated at 30 °C for the plasticized SPEs due to the dramatically improved conductivity.

 

Solid polymer electrolytes have shown to be a promising solution to suppressing dendrite growth for safer and higher performance lithium batteries. This article reports the fabrication and characterization of a series of nanostructured polymer electrolyte membranes (PEMs) comprised of poly(ethylene glycol)/bis(trifluoromethane)sulfonimide lithium electrolyte and acrylate–thiol‐ene crosslinked resin using a holographic polymerization (HP). Nanoscale long‐range order is observed and this unique structure imposes intriguing mechanical and ion‐conducting properties of the PEMs. The modulus of the holographically polymerized PEMs can be tuned to vary from 150 to 1300 MPa while room temperature conductivities of ≈2 × 10⁻⁵S cm⁻¹and 90 °C conductivity of ≈5 × 10⁻⁴S cm⁻¹are achieved. The HP nanostructure is also capable of directing ion transport either parallel or perpendicular to the membrane surface; an unprecedented ionic conductivity anisotropy as high as 3 × 10⁵is achieved. It is anticipated that these PEMs may be excellent candidates for lithium battery applications.

 

Solid polymer electrolytes (SPEs) are desirable in lithium metal batteries (LMBs) since they are nonflammable and show excellent lithium dendrite growth resistance. However, fabricating high performance polymer LMBs is still a grand challenge because of the complex battery system. In this work, a series of tailor‐designed hybrid SPEs are used to prepare LMBs with a LiFePO₄‐based cathode. High performance LMBs with both excellent rate capability and long cycle life are obtained at 60 and 90 °C. The well‐controlled network structure in this series of hybrid SPEs offers a model system to study the relationship between the SPE properties and the LMB performance. It is shown that the cycle life of the polymer LMBs is closely correlated with the SPE–Li interface ionic conductivity, underscoring the importance of the solid electrolyte interface in LMB operation. LMB performance is further correlated with the molecular network structure. It is anticipated that results from this study will shed light on designing SPEs for high performance LMB applications.