Ion Transfer Research Articles

Recent Advancements in Materials for Proton-Conducting Reversible Solid Oxide Cells

The escalating threats posed by climate change and environmental issues underscore the need for urgent exploration of clean energy technologies. In this context, proton-conducting reversible solid oxide cells (P-RSOCs) have emerged as promising contenders for large-scale energy storage and conversion. Their efficacy at intermediate temperatures (400 - 600 °C) is a distinctive advantage, attributed to the remarkable ionic conductivity of proton conductors within this temperature range. This feature positions P-RSOCs favorably for the efficient, cost-effective, and enduring conversion between clean electricity and green hydrogen.However, the successful commercialization of P-RSOCs hinges on the rational design of novel materials and meticulous surface/interface modifications to significantly enhance performance and durability. Achieving prolonged durability during cycling between fuel cell and electrolysis modes while maintaining high Faraday efficiency and roundtrip energy efficiency is of paramount importance. A central challenge involves the development of electrolyte materials exhibiting exceptional stability and a high ionic transference number under operating conditions. Additionally, bifunctional electrodes/catalysts, particularly for the oxygen electrode, must demonstrate elevated activity for efficient dual-mode operation.To effectively tackle these challenges, it is imperative to devise new protocols for controlling the structure, composition, and morphology of materials across multiple length scales. Equally crucial is gaining a fundamental understanding of degradation mechanisms and electrode processes. This presentation will illuminate the critical scientific challenges inherent in developing a new generation of P-RSOCs, providing insights into the latest advancements in electrolyte materials and bifunctional electrodes/catalysts. Furthermore, it will highlight strategies for enhancing durability and electrode activity through surface/interface modification, along with the latest developments in modeling, simulation, and in situ characterization techniques to deepen our understanding of the underlying mechanisms. The presentation will conclude prospects for achieving low-cost, highly efficient, and durable P-RSOCs through innovative material-based solutions.

Unveiling enamel demineralization mechanisms by sensitive dielectric differentiation based on terahertz nanospectroscopy.

The early stage of dental caries, i.e. demineralization, has always been a topic of concern to dentists. Understanding the essential mechanism of its occurrence is of great significance for the prevention and treatment of dental caries. However, owing to limitations in resolution and the detection capabilities of diagnostic tools, the study of enamel demineralization has always been a challenge. Terahertz (THz) technology, especially the combination of scanning near-field optical microscopy (s-SNOM) and THz time-domain spectroscopy (TDS), due to its nanoscale resolution, has shown great advantages in the field of biological imaging. Here, a THz s-SNOM system is used to perform near-field imaging of enamel before and after demineralization at the nanoscale. It can be found that near-field signals decrease significantly after demineralization. This is due to the changes of the crystal lattice and the transfer of mineral ions during demineralization, which leads to a decrease in the permittivity of the enamel. The novel approach in this study reveals the essence of demineralization and lays the groundwork for additional research and potential interventions.

Real Time Tracking of Nanoconfined Water-Assisted Ion Transfer in Functionalized Graphene Derivatives Supercapacitor Electrodes.

Water molecules confined in nanoscale spaces of 2D graphene layers have fascinated researchers worldwide for the past several years, especially in the context of energy storage applications. The water molecules exchanged along with ions during the electrochemical process can aid in wetting and stabilizing the layered materials resulting in an anomalous enhancement in the performance of supercapacitor electrodes. Engineering of 2D carbon electrode materials with various functionalities (oxygen (─O), fluorine (─F), nitrile (─C≡N), carboxylic (─COOH), carbonyl (─C═O), nitrogen (─N)) can alter the ion/water organization in graphene derivatives, and eventually their inherent ion storage ability. Thus, in the current study, a comparative set of functionalized graphene derivatives-fluorine-doped cyanographene (G-F-CN), cyanographene (G-CN), graphene acid (G-COOH), oxidized graphene acid (G-COOH (O)) and nitrogen superdoped graphene (G-N) is systematically evaluated toward charge storage in various aqueous-based electrolyte systems. Differences in functionalization on graphene derivatives influence the electrochemical properties, and the real-time mass exchange during the electrochemical process is monitored by electrochemical quartz crystal microbalance (EQCM). Electrogravimetric assessment revealed that oxidized 2D acid derivatives (G-COOH (O)) are shown to exhibit high ion storage performance along with maximum water transfer during the electrochemical process. The complex understanding of the processes gained during supercapacitor electrode charging in aqueous electrolytes paves the way toward the rational utilization of graphene derivatives in forefront energy storage applications.

Development of Eco‐Friendly Chitosan‐Dextran Polyblend Electrolyte for Enhanced Performance in Primary Magnesium Batteries

The potential of next‐generation batteries lies in solid biodegradable polymer electrolytes. This research delves into a solid blend polymer electrolyte (SBPE) for magnesium conduction, utilizing a chitosan‐dextran blend matrix doped with magnesium perchlorate (Mg(ClO4)2) salt. The electrolyte films are prepared using a conventional solution casting technique. Through techniques like X‐ray diffraction and Fourier transform infrared spectroscopy, the successful incorporation of Mg(ClO4)2 into the blend matrix is confirmed. Notably, the SBPE containing 30 wt% of Mg(ClO4)2 demonstrates the highest ionic conductivity of 6.99 × 10−4 S cm−1 and a prominent ionic transference number of 0.84. Thermogravimetric analysis is carried out to study thermal stability. Differential scanning calorimetry analysis of the electrolyte systems gives insight into their thermal properties. Additionally, it showcases favorable electrochemical stability of 2.66 V. The oxidation and reduction peaks are observed in the cyclic voltammetry curve of the highest conducting sample. Furthermore, the discharge performance of Mg/(CS + DN + Mg(ClO4)2)/cathode cells is explored with varied cathode materials, illustrating the SBPE's potential for magnesium‐ion batteries. This study unveils a sustainable, biodegradable, and economical electrolyte solution for advanced energy storage systems.

Ionic Liquid‐Supported Single‐Sodium‐Ion‐Conducting Styrene‐Maleic Anhydride Copolymer for Energy Storage Devices

Wide‐ranging research has been done on ionic liquid (IL)‐incorporated conducting polymers in energy storage devices. Herein, by taking the reaction advantage of styrene maleic anhydride (SMA) copolymer with sodium hydroxide, a sodium ion having polymeric material as an electrolyte is synthesized. 1,8‐Diazabicyclo[5.4.0]undec‐7‐enium acetate (DBU acetate) is prepared as an IL and added to the prepared polymer electrolyte to increase the matrix flexibility, semisolid nature, and ionic mobility inside the matrix. This semisolid sodium ion‐based electrolyte shows conductivity in the order of 10−5 S cm−1 and an electrochemical stability window of 2.52 volts with >97% of ionic transference. It also shows the diffusivity constant in the order of 10−4 m2 s−1 and ionic mobility in the order of 10−3 m2 v−1 s−1 at 30 °C. The hydrogel matrix shows a correlated type of hopping with a power exponent <1 at 30 °C with low‐energy requirement of ionic transport, that is, 0.709 eV. A high amount of capacitance is associated with electrolyte that has an insignificant electrode contribution. On behalf of these findings, SMA‐IL‐based semisolid polymer electrolyte confirms its potential for application in sodium ion‐based energy storage systems.

Ion transfer mechanism of fluorescence-labeled octa-arginine on model biomembrane surfaces

The interfacial behavior of a synthesized fluorescent polycationic cell-penetrating peptide, octa-arginine covalently labeled with carboxyfluorescein (FAM-R8), was investigated through spectroelectrochemical analysis at the bare and phospholipid-modified water|1,2-dichloroethane (DCE) interfaces. The potential modulated fluorescence (PMF) analysis indicated that the adsorption of FAM-R8 from the aqueous side of the bare interface occurred in the wide potential range at lower FAM-R8 concentrations, while the ion transfer across the interface proceeded at the positive edge of the polarizable potential window as the concentration increased. The complicated interfacial reaction behavior of FAM-R8 was further observed at the biomimetic interface in the presence of a phospholipid layer, where the adsorption potential of FAM-R8 was positively shifted as compared with the bare interface. Moreover, the ion transfer process of FAM-R8 became predominant when the surface excess of FAM-R8 was substantially increased at the biomimetic interface. The FAM-R8 concentration and its interaction with the phospholipid layer were found to play an important role for the membrane permeation mechanism.

Thin-film composite electro-nanofiltration membrane for one-step and efficient fractionation of dyes and salts in high-salinity textile wastewater

The key to achieve sustainable treatment of high-salinity dye-containing wastewater is effective fractionation of dyes and salts. In this study, a thin-film composite electro-nanofiltration membrane was successfully fabricated by co-deposition of levodopa and ε-polylysine onto a porous ultrafiltration membrane substrate. With the co-deposition of the polylevodopa/ε-polylysine composite coating on the substrate membrane, the surface properties were significantly regulated, resulting in decreased pore size, reduced surface negative charge density and lower specific electric resistance, thus enhancing their ion transfer and dye/salt fractionation efficacy. Specifically, the fabricated LDP-4 membrane (molecular weight cut-off of 408 Da) with a 4-h co-deposition experienced a 99.12 % reactive orange 16 dye rejection and 10.15 % NaCl rejection, indicating an impressive selectivity between dyes and salts. Additionally, the LDP-4 electro-nanofiltration membrane as anion conducting membrane exhibited a fast and efficient electro-driven transfer of Cl− ions. Notably, under an electric field, the fabricated LDP-4 electro-nanofiltration membrane can efficiently fractionate NaCl from the reactive orange 16/NaCl mixed solution, achieving a 98.89 % desalination efficiency and 99.79 % dye recovery. Furthermore, the LDP-4 membrane demonstrated remarkable anti-fouling property and long-term stability over an 8-cycle electro-nanofiltration operation. Therefore, the electro-nanofiltration membranes fabricated by co-deposition of levodopa and ε-polylysine show a promising potential in sustainable resource recovery from high-salinity dye-containing wastewater.

Rational combination of Inverted-Pyramid structured Nickel-based Prussian blue with porous 3D carbon as high-performance sodium-ion batteries cathode

Metal based Prussian blue composite materials with heterogeneous structures possess substantial potential for enhancing both ionic and charge transfer processes, ultimately expediting electrochemical reaction kinetics for various battery devices. However, the limited bonding between carbon materials and Prussian blue analogues (PBAs) and the uncontrolled nucleation rate of metal component resulted in limited specific capacity and cyclic stability. Herein, we introduced a novel approach for the in-situ synthesis of Ni-PBA with an inverted-pyramid structure on a three-dimensional ultra-thin carbon frames (3DUC) substrate via a hydrothermal method. The inverted pyramid structure fits tightly with the 3DUC during nucleation to form a one-piece stable structure. This integration effectively curbs aggregation and hasty nucleation tendencies of NiPBA. Furthermore, the abundant voids and interconnected networks within the 3DUC structure significantly reduce ion diffusion path lengths, thereby lowering the Na diffusion barrier and enhancing the material’s capacitance contribution rate. Consequently, this cathode material exhibits commendable initial capacity (125.2 mAh/g at 50 mA g−1) and exceptional long-term cycling stability (with a capacity retention of 89.06 % after 900 cycles at 50 mA g−1). These findings hold significant promise for advancing the commercial viability of metal-PBA based electrodes by rational heterogeneous structure design.

Regulating interfacial behavior via reintegration the Helmholtz layer structure towards ultra-stable and wide-temperature-range aqueous zinc ion batteries

Aqueous zinc-ion batteries are recognized as a potential candidate in large-scale energy storage devices. However, parasitic reactions on interfaces have severely limited their further development due to sticky de-solvation process of Zn(H2O)62+. Acetylacetone (Hacac) is proposed as a tri-functional additive by altering the solvation structure to address detrimental interface issues. Specifically, the acetyl groups induced by decomposition of Hacac inhibit dendrite growth, by-product aggregation on anode via guiding ordered deposition of zinc ions and suppressing water decomposition in internal Helmholtz plane (IHP). Meanwhile, the acetyl groups remarkably alleviate by-product aggregation and maintain the cathode structure by accelerating zinc ion transfer and inhibiting disintegration of water in IHP. With the addition of 0.5 wt% Hacac, Zn metal maintains a high coulombic efficiency of 99.9 % after 2000 cycles at 10 mA cm−2 and 1 mAh cm−2, with superior longevity of 5200 h at 1 mA cm−2 with 0.5 mAh cm−2 for Zn|Zn cells. As expected, the assembled Zn|NH4V4O10 batteries exhibit an outstanding capacity retention of 90 % up to 22,000 cycles at 10 A/g. As a highly efficient strategy, the reframing of Helmholtz layer structure via electrolyte additive could be broadened to address general interfacial issues in advanced energy storage systems.

Extraordinary Hydrogen Evolution and Oxygen Evolution Reaction Activity From PPy@FeCo-LDH/NF Bifunctional Electrocatalyst in Alkaline Solution

Alkaline water electrolysis is a promising technique for the production of hydrogen and oxygen. Nevertheless, the development of low-cost, high-activity metal-based electrocatalysts that can effectively catalyze the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) remains a significant challenge. Herein, we polymerized Polypyrrole (PPy) with FeCo layered double metal hydroxide grown in situ on nickel foam (NF) (FeCo-LDH/NF) by electrochemical polymerization to acquire composite material PPy@FeCo-LDH/NF. As a promising electrocatalyst with dual functionality for the HER and OER, the HER overpotential of PPy@FeCo-LDH/NF was 153 mV, and the OER overpotential was 245 mV at a current density of 10 mA·cm−2. It was because that PPy increased the number of active adsorption sites, which in turn regulated the ion transfer rate between the electrolyte and the prepared catalyst. At the same time, after 24 h of stability testing, the HER and OER capacitance retention rates were 96.7% and 97.1%, respectively.

Solid-electrolyte interphase governs zinc ion transfer kinetics in high-rate and stable zinc metal batteries

Solid-electrolyte interphase governs zinc ion transfer kinetics in high-rate and stable zinc metal batteries

Bi2WO6 and TiS2 composite nanostructures displaying synergetic boosted energy storage in supercapacitor

The enhancement in the capacitance of a supercapacitor has been successfully achieved by synthesizing Bi2WO6 (BW), TiS2 (T), and Bi2WO6/TiS2 (BW/T) composites utilizing the hydrothermal process. The possible growth mechanism has also been presented. The morphological and structural characteristics of the cultivated samples were observed using FT-IR, XRD, SEM, EDS, and UV–vis spectroscopy techniques. TiS2 nano platelets uniformly dispersed across the hierarchically opened surface of Bi2WO6 in the synthesized hierarchical composite. This leads to an increase in surface porosity and surface area, which in turn enhances the transport of electrons and ions on the composite BW/T surface. The optimal electrode BW/T@40 % composite electrode shown a substantial enhancement in particular capacitance (1153.3 F/g) compared to the separate BW (523.7 F/g) and T (453.3 F/g) electrodes due to its rapid ion transfer, many active sites on its large surface area, and strong synergistic impact. Furthermore, the BW/T@40 % combination demonstrated exceptional stability, with over 92 % of its capacitance maintained after 4500th cycles and b value (0.71) proved the supercapacitor behavior. Therefore, BW/T@40 % binary metal oxide and sulfide composites exhibit improved specific capacitance and greatly prolonged life-cycle, confirming its potential use in high-performance energy storage devices.

Ion Exchange-Mediated 3D Cross-Linked ZIF-L Superstructure for Flexible Electrochemical Energy Storage.

Metal-organic frameworks (MOFs) are considered as a promising candidate for advancing energy storage owing to their intrinsic multi-channel architecture, high theoretical capacity, and precise adjustability. However, the low conductivity and poor structural stability lead to unsatisfactory rate and cycling performance, greatly hindering their practical application. Herein, we propose a sea urchin-like Co-ZIF-L superstructure using molecular template to induce self-assembly followed by ion exchange method, which shows improved conductivity, successive channels, and high stability. The ion exchange can gradually etch the superstructure, leading to the reconstruction of Co-ZIF-L with three-dimensional (3D) cross-linked ultrathin porous nanosheets. Moreover, the precise control of Co to Ni ratios can construct effective micro-electric field and synergistically enhance the rapid transfer of electrons and electrolyte ions, improving the conductivity and stability of CoNi-ZIF-L. The Co6.53Ni-ZIF-L electrode exhibits a high specific capacity (602 F g-1 at 1 A g-1) and long cycling stability (95.3 % retention after 4,000 cycles at 5 A g-1). The Co6.53Ni-ZIF-L//AC asymmetric flexible supercapacitor employing gel electrolyte also exhibits excellent cycling stability (93.3 % retention after 4000 cycles at 5 A g-1). This discovery provides valuable insights for electrode material selection and energy storage efficiency improvement.

Ion Exchange‐Mediated 3D Cross‐Linked ZIF‐L Superstructure for Flexible Electrochemical Energy Storage

AbstractMetal–organic frameworks (MOFs) are considered as a promising candidate for advancing energy storage owing to their intrinsic multi‐channel architecture, high theoretical capacity, and precise adjustability. However, the low conductivity and poor structural stability lead to unsatisfactory rate and cycling performance, greatly hindering their practical application. Herein, we propose a sea urchin‐like Co‐ZIF‐L superstructure using molecular template to induce self‐assembly followed by ion exchange method, which shows improved conductivity, successive channels, and high stability. The ion exchange can gradually etch the superstructure, leading to the reconstruction of Co‐ZIF‐L with three‐dimensional (3D) cross‐linked ultrathin porous nanosheets. Moreover, the precise control of Co to Ni ratios can construct effective micro‐electric field and synergistically enhance the rapid transfer of electrons and electrolyte ions, improving the conductivity and stability of CoNi‐ZIF‐L. The Co6.53Ni‐ZIF‐L electrode exhibits a high specific capacity (602 F g−1 at 1 A g−1) and long cycling stability (95.3 % retention after 4,000 cycles at 5 A g−1). The Co6.53Ni‐ZIF‐L//AC asymmetric flexible supercapacitor employing gel electrolyte also exhibits excellent cycling stability (93.3 % retention after 4000 cycles at 5 A g−1). This discovery provides valuable insights for electrode material selection and energy storage efficiency improvement.

Highly Ionic Conductive, Self-Healing, Li10GeP2S12-Filled Composite Solid Electrolytes Based on Reversibly Interlocked Macromolecule Networks for Lithium Metal Batteries with Improved Cycling Stability.

Ceramic-polymer composite solid electrolytes (CSEs) have attracted great attention by combining the advantages of polymer electrolytes and inorganic ceramic electrolytes. Herein, Li10GeP2S12 (LGPS) particles are incorporated into poly(ethylene oxide) (PEO)-based reversibly interlocked polymer networks (RILNs) derived from the topological rearrangement of two PEO networks cross-linked by reversible imine bonds and disulfide linkages. A series of highly ionic conductive, self-healing CSEs are obtained accordingly. The interlocking architecture successfully inhibits PEO crystallization, increasing the amorphous phase for Li ion transportation, and stabilizes the conductive pathways of LGPS particles by its unique confinement effect. Meanwhile, the LGPS particles cooperate with the RILN matrix, forming a filler-polymer interfacial phase for additional Li ion transportation and strengthening and toughening the resultant CSEs via the strong intermolecular Li+-O2- interactions. Furthermore, the dynamic characteristics of the included reversible bonds ensure a multiple intrinsic self-healing capability. Consequently, the CSEs containing 15 wt % LGPS deliver a high ionic conductivity (1.06 × 10-3 S cm-1) and high Li ion transference number (∼0.6) at 25 °C, a wide electrochemical stability window (>4.9 V), good mechanical properties (0.63 MPa, 377%), and a stable CSE/Li anode interface. The integrated Li/CSE/LiFePO4 battery exhibits a specific discharge capacity of 110.8 mAh g-1 at 1 C (25 °C) and a capacity retention of 76.9% after 200 cycles. Thanks to the healability, the damaged CSEs can regain the structural integrity, ion conductive capability, and cycling performance of the assembled cells. The present work provides an effective strategy to fabricate CSEs for lithium metal batteries that are workable at ambient temperature.

A Nitrogen/Oxygen Dual-Doped Porous Carbon with High Catalytic Conversion Ability toward Polysulfides for Advanced Lithium–Sulfur Batteries

Lithium–sulfur batteries (LSBs) have attracted widespread attention due to their high theoretical energy density and low cost. However, their development has been constrained by the shuttle effect of lithium polysulfides and their slow reaction kinetics. In this work, a nitrogen/oxygen dual-doped porous carbon (N/O-PC) was synthesized by annealing the precursor of zeolitic imidazolate framework-8 grown in situ on MWCNTs (ZIF-8/MWCNTs). Then, the N/O-PC composite served as an efficient host for LSBs through chemical adsorption and providing catalytic conversion sites of polysulfides. Moreover, the interconnected porous carbon-based structure facilitates electron and ion transfer. Thus, the S/N/O-PC cathode exhibits high cycling stability (a stable capacity of 685.9 mA h g−1 at 0.2 C after 100 cycles). It also demonstrates excellent rate performance with discharge capacities of 1018.2, 890.2, 775.1, 722.7, 640.4, and 579.6 mAh g−1 at 0.2, 0.5, 1.0, 2.0, 3.0, and 5.0 C, respectively. This work provides an effective strategy for designing and developing high energy density, long cycle life LSBs.

Optimizing Graphene Anode Performance in Lithium‐Ion Batteries: Investigating the Effects of Diverse Thermal Conditions

Herein, the graphene nanoplatelets (GNPs) anode is prepared using a facile, chemical‐free, and scalable approach that combines probe sonication and microwave treatment in an argon condition. The resulting GNPs exhibit a significant number of structural defects (ID/IG: 0.262), which provide abundant active sites to store lithium ions and offer sufficient pathways for the quick transfer of lithium ions and electrons. In lithium‐ion batteries (LIBs), the GNPs anode exhibits an outstanding electrochemical performance, achieving a high reversible 414 mAh g−1 capacity at the high current density of 1 A g−1 after 350 cycles. The anode maintains desirable capacities of 167 and 150 mAh g−1 even at elevated current densities of 4 and 5 A g−1, respectively. Importantly, it exhibits remarkable cycling performance with more than 100% of the initial reversible capacity retention after 350 cycles. The outcomes show noticeably enhanced performance characteristics, suggesting the potential for developing microwave‐treated graphene anode for long‐lasting and high‐performance LIBs.

Designed inorganics doped gel electrolyte with enhancing ion transfer and diffusion effects for flexible interdigitated supercapacitors

Electrolyte enhancement strategy becomes a promising route to improve flexible interdigitated miniaturized supercapacitors (IMSCs) performance due to the less mass loading of electrode materials on interdigitated electrodes. Herein, we develop a flexible polyvinyl alcohol/KOH (PVA/KOH) gel electrolyte with homogeneous BN-PDA (polydopamine modified boron nitride nanosheets) doping for enhancing energy storage of IMSCs, in which the conductivity is up to 112.1 mS cm−1 with excellent mechanical strength and heat stability. The ionicity of BN-PDA caused by electronegativity difference between B and N atoms significantly facilitates KOH transfer in PVA gel and diffusion in electrode diffuse layer by rapping-pairing effect. Furthermore, the different phase transition behavior of BN-PDA and PVA in water provides additional ions transmission pathways and effectively disperses external forces. With such excellent electrolytes, ultra-high energy density (14.7 μWh cm−2) at a high power density (420 μW cm−2) has been achieved for IMSCs. Moreover, the capacitance of IMSCs can always be maintained at a very high level during the long-term charge and discharge process. Our work suggests a feasible pathway to design inorganic fillers uniformly modified gel electrolyte with high conductivity and increased energy storage capacity of IMSCs as well as other flexible energy storage devices.

Kinetic Insights into Na Ion Transfer at the Carbon‐Based Negative Electrode/Electrolyte Interfaces for Sodium‐Ion Batteries

AbstractThe relentless quest for sustainable and efficient energy storage solutions has propelled sodium‐ion batteries (SIBs) to the forefront of research and development in the realm of rechargeable batteries. This mini review delves into the intricate interfacial kinetics of Na ion transfer within SIBs, with a special focus on the carbon‐based negative electrode/electrolyte interfaces. By synthesizing insights from a myriad of studies encompassing experimental and theoretical analyses, we illuminate the critical role of electrode material properties and interfacial dynamics in dictating the kinetics of Na ion transfer for SIBs. Strategies for optimizing these parameters are scrutinized, revealing pathways to enhance the kinetic behavior of Na ions. Furthermore, emerging materials such as hard carbon, carbon nanospheres, and graphene‐like graphite are evaluated for their potential to surmount existing limitations.

PVDF/lithiated sulfonated poly (ether ether ketone) blend coated PE separators for high-performance lithium metal batteries

Ionic conductivity and lithium ion transference number (tLi+) of electrolytes are essential parameters governing the performances of high energy density lithium metal batteries. Although the importance of tLi+versus ionic conductivity has been theorized by simulation, the systematically experimental study of their respective effects on lithium dendrite suppression and battery performances is rarely carried out. Here, a series of polyvinylidene fluoride and lithated sulfonated poly (ether ether ketone) blend (PVDF/SPEEK-Li) coated polyethylene (PE) separators with exactly the same composition but different pore morphologies are fabricated by vapor and non-solvent induced phase separation. The effects of sulfonate group–ion interaction and pore morphologies on ionic conductivity and tLi+ of the electrolytes are studied. The performances of lithium metal batteries can be obviously improved by subtle increase of the tLi+, especially at high charge rates and even with a decrease in conductivity. Even at a high current density of 3 C, the PVDF/SPEEK-Li coated PE separator assembled lithium metal battery using a LiFePO4 cathode with a mass loading of 10.5 mg cm−2 can run stably for 200 cycles with a capacity retention of 79 %, which is superior to the PE separator assembled battery with a life of only 55 cycles.