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Figure 1. Structural design and morphological analysis of the PHLM-CSE composite solid-state electrolyte. (a) Schematic illustration of the three-dimensional architecture of the PHLM-CSE and the proposed mechanism by which MOF facilitates Li⁺ transport; (b) SEM image of the PVDF-HFP/LLZTO nanofiber membrane (PHL), scale bar : 2 ï¿½ï¿½m; (c) SEM image of the PHL-Zn nanofiber membrane after Zn²⁺ ion adsorption, scale bar: 2 ï¿½ï¿½m; (d) SEM image of the PHLM nanofiber membrane following in situ MOF growth, scale bar: 1 ï¿½ï¿½m; (e, f) TEM images of the PHLM nanofiber membrane highlighting internal structure; (g) SEM image of the surface morphology of the PHLM-CSE electrolyte, scale bar: 2 ï¿½ï¿½m. Inset: photograph image of the as-prepared membrane; (h) Nitrogen adsorption-desorption isotherm of the as-prepared ZIF-8 measured at 77.3 K; (i) XRD patterns of the PHLM-CSE electrolyte, PHLM and PHL membranes, pristine PVDF-HFP, ZIF-8, and LLZTO. Key diffraction peaks for PVDF-HFP, LLZTO, and ZIF-8 are indicated by dotted lines and arrows for clarity; (j) Fourier transform infrared (FTIR) spectra of the PHL, ZIF-8, and PHLM nanofiber membranes.

Figure 2. Structural features and electrochemical performance of the PHLM-CSE composite electrolyte membranes. (a) Differential scanning calorimetry (DSC) curves of PHL-CSE and PHLM-CSE electrolytes, highlighting their glass transition temperature (T_g) ; (b) DSC curves of PHL-CSE and PHLM-CSE in the higher-temperature region, illustrating thermal stability; (c) Stress-strain curves of PHL-CSE, PHLM-CSE, and PEO-LiTFSI electrolytes, revealing mechanical strength and flexibility; (d) Frequency-dependent dielectric constant (ï¿½ï¿½_r) of PEO-LiTFSI, PHL-CSE, and PHLM-CSE electrolytes; (e) FTIR spectra of PHL, PHLM and pristine PVDF-HFP membranes, demonstrating polymer phase characteristics and structural features; (f) Arrhenius plots of ionic conductivity (ï¿½ï¿½) versus temperature for PHLM-CSE electrolytes with varying LLZO contents; (g) Comparative ionic conductivity-temperature profiles of PEO-LiTFSI, PHL-CSE, and PHLM-CSE electrolytes; (h) Bar graph comparing the lithium-ion migration activation energy (E_a) across different electrolytes; (i) Linear sweep voltammetry (LSV) curves evaluating the electrochemical stability window of the investigated membranes.

Figure 3. Electrochemical properties and interfacial stability analysis of the PHLM-CSE composite solid-state electrolyte. (a) Galvanostatic charge-discharge profiles of the PHLM-CSE-based cell, with the inset displaying the corresponding electrochemical impedance spectroscopy (EIS) data; (b) Comparison of lithium-ion transference numbers (t_Li+) for PEO-LiTFSI, PHL-CSE, and PHLM-CSE electrolytes; (c) Electrochemical impedance spectra (EIS) of symmetric Li|PEO-LiTFSI|Li, Li|PHL-CSE|Li, and Li|PHLM-CSE|Li cells, reflecting interfacial resistance; (d) Linear sweep voltammetry (LSV) curves used to evaluate the electrochemical stability windows of different electrolytes; (e) Critical current density (CCD) measurements of Li|Li symmetric cells with PEO-LiTFSI, PHL-CSE, and PHLM-CSE electrolytes; (f) Molecular structures and corresponding HOMO-LUMO energy level diagrams of PVDF-HFP, PEO, LiTFSI, and ZIF-8; (g) Electrostatic potential distribution map of ZIF-8, indicating charge localization characteristics; (h) Binding energies (E_b) and optimized configurations of ZIF-8 interacting with PEO, PVDF-HFP, and their binary complex.

Figure 4. Investigation of lithium-ion transport behavior and interfacial stability in PHLM-CSE composite solid-state electrolytes. (a) Raman spectra of PEO-LiTFSI, PHL-CSE, and PHLM-CSE composite electrolytes, highlighting variations in ion coordination environments; (b) Snapshot from a molecular dynamics (MD) simulation of the PHLM-CSE model system; (c) Mean squared displacement (MSD) curves of Li⁺in PEO-LiTFSI, PHL-CSE, and PHLM-CSE electrolytes, reflecting ion mobility; (d) Radial distribution functions (RDFs) and coordination environments between Li⁺ and TFSI^- in various electrolytes; (e) RDFs and coordination environments between Li⁺ and ether oxygen (ï¿½COï¿½C) atoms in the EO segments; (f) Galvanostatic cycling performance of Li|Li symmetric cells with PHLM-CSE, PHL-CSE, and PEO-LiTFSI electrolytes at 0.1 mA cm^-2. (g) enlarged voltage profiles near the short-circuit or failure points in Li|PEO-LiTFSI|Li, Li|PHLM-CSE|Li, and Li|PHL-CSE|Li cell; (h) F 1s core-level XPS spectra of Li anodes after 100 cycles with different electrolytes; (i) SEM images of Li metal surfaces after cycling; (j) Two-dimensional laser confocal microscopy imagesshowing cycled surface morphology; (k) Three-dimensional laser confocal microscopy reconstructions of Li metal surfaces following long-term cycling.

Figure 5. Electrochemical performance and flexible applications of PHLM-CSE-based solid-state lithium metal batteries. (a) Rate capability and (b) corresponding chargeï¿½Cdischarge profiles of LiFePO₄|PHLM-CSE|Li full cells at various current densities. (c) Long-term cycling performance at 0.2 C and (d) corresponding voltage profiles. (e) Cycling stability of NCM811|PHLM-CSE|Li, NCM811|PHL-CSE|Li, and NCM811|PEO-LiTFSI|Li full cells at 1 C, and (f) their voltage profiles. (g) Optical images showing stable operation of a pouch cell under flat, folded, cut, and punctured conditions. (h,i) Demonstration of the pouch cell powering an electromyography (EMG) sensor and a smartphone, respectively.

Ôï¿½ï¿½æœ½Ó£ï¿½https://doi.org/10.1002/adfm.202514738

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