Solid-state Energy Storage Devices Research Articles

A mechanistic study of the dopant-induced breakdown in halide perovskites using solid state energy storage devices.

Doping halide perovskites (HPs) with extrinsic species, such as alkali metal ions, plays a critical, albeit often elusive role in optimising optoelectronic devices. Here, we use solid state lithium ion battery inspired devices with a polyethylene oxide-based polymer electrolyte to dope HPs controllably with lithium ions. We perform a suite of operando material analysis techniques while dynamically varying Li doping concentrations. We determine and quantify three doping regimes; a safe regime, with doping concentrations of <1020 cm-3 (2% Li : Pb mol%) in which the HP may be modified without detrimental effect to its structure; a minor decomposition regime, in which the HP is partially transformed but remains the dominant species; and a major decomposition regime in which the perovskite is superseded by new phases. We provide a mechanistic description of the processes mediating between each stage and find evidence for metallic Pb(0), LiBr and LiPbBr2 as final decomposition products. Combining results from synchrotron X-ray diffraction measurements with in situ photoluminescence and optical reflection microscopy studies, we distinguish the influences of free charge carriers and intercalated lithium independently. We find that the charge density is equally as important as the geometric considerations of the dopant species and thereby provide a quantitative framework upon which the future design of doped-perovskite energy devices should be based.

Ionogels: Squeeze flow rheology and ionic conductivity of quasi-solidified nanostructured hybrid materials containing ionic liquids immobilized on halloysite

Ionogels are hybrid ion-conducting materials consisting of ionic liquids stabilized by inorganic or polymer fillers and having good prospects for application in solid-state and flexible electronics and energy storage devices. The work presents the results of studying the rheological properties and ionic conductivity of a series of ionogels based on halloysite nanoclay and bis(trifluoromethylsulfonyl)imide ionic liquids with EMIm+, BMIm+, BM2Im+, BMPyrr+, BMPip+ and MOc3Am+ cations and content of the dispersion phase of 43–48%. The obtained values are compared with the analogous characteristics of bulk ionic liquids. It has been established that the IL cation structural characteristics affect the viscoplastic properties of ionogels subjected to uniaxial quasistatic compression (20 °C), ionic conductivity and structural resistance coefficient of an inorganic filler (from −20 to +80 °C). Additive models of conductivity in binary systems are applied to obtain correlations linking ionic conductivity of ionogels with that of pure ionic liquids.

3D Printing for Solid-State Energy Storage.

Ever-growing demand to develop satisfactory electrochemical devices has driven cutting-edge research in designing and manufacturing reliable solid-state electrochemical energy storage devices (EESDs). 3D printing, a precise and programmable layer-by-layer manufacturing technology, has drawn substantial attention to build advanced solid-state EESDs and unveil intrinsic charge storage mechanisms. It provides brand-new opportunities as well as some challenges in the field of solid-state energy storage. This review focuses on the topic of 3D printing for solid-state energy storage, which bridges the gap between advanced manufacturing and future EESDs. It starts from a brief introduction followed by an emphasis on 3D printing principles, where basic features of 3D printing and key issues for solid-state energy storage are both reviewed. Recent advances in 3D printed solid-state EESDs including solid-state batteries and solid-state supercapacitors are then summarized. Conclusions and perspectives are also provided regarding the further development of 3D printed solid-state EESDs. It can be expected that advanced 3D printing will significantly promote future evolution of solid-state EESDs.

Synchronous-ultrahigh conductive-reactive N-atoms doping strategy of carbon nanofibers networks for high‐performance flexible energy storage

Flexible carbon nanofibers networks (FCNNs) play a crucial role in flexible and portable energy storage devices. Doping conductive and reactive N-atoms can enhance charge transport and transfer properties vital for high energy storage and high power. However, synchronous-ultrahigh conductive-reactive N-atoms doped FCNNs (SH-FCNNs) are still challenged by the N-atoms instability at high temperatures. To resolve this problem, an in-situ synergistic-carbonization-nitridation strategy is reported using polyaniline (PANI) implanted highly porous polyacrylonitrile nanofibers as a precursor. The obtained SH-FCNNs were doped with 5.9 at% conductive and 4.73 at% reactive N-atoms. They exhibit a superhigh specific capacitance (580.9 F g−1@0.5 A g−1) and high-rate capability (307.2 F g−1@128 A g−1). The flexible solid-state supercapacitors can output specific energy and power density of 18.3 Wh kg−1 and 16.9 kW kg−1. As for flexible solid-state Zn-ion batteries, the constructed SH-FCNNs@PANI cathodes have specific energy (290 Wh kg−1@0.159 kW kg−1) and supercapacitor-like power performance (128.1 Wh kg−1@23.3 kW kg−1). The synergistic effects of ultrahigh conductive and reactive N-atoms promote these performances to reach the mountaintop of flexible solid-state energy storage devices. The novel strategy also presents new insights on designing high-performance FCNNs for electrochemical energy storage, catalysts, and sensors.

Defect-enriched hydroxyapatite induced by carboxylated chitosan as novel filler for pseudo solid-state supercapacitors

BackgroundThe severe crystalline region in pseudo solid-state polymer electrolyte needs to be addressed to improve the poor ionic conductivity performance. MethodsHydroxyapatite (HA) with rich defect, induced by carboxylated chitosan (CCS) via hydrothermal process is applied to serve as active filler for pseudo solid-state supercapacitor. Significant findingsCCS2 with high degree of carboxylation (DC) of 42.38% is introduced as defect inducing agents to generate CCS2-HA. CCS2-HA possesses small crystallinity index evaluated by FTIR and XRD. Moreover, the obvious structural defect of CCS2-HA in [301] orientation was observed from HRTEM. With CCS2-HA as defect-enriched filler, the crystallization temperature decreases from 75 to 65 °C. Meanwhile, the activation energy for the ionic conductivity decreases from 2.3 to 1.3 kJ/mol. Meanwhile, the loss tangent peak shifts to higher frequency with smaller intensity in the addition of CCS2-HA as active filler, showing the smaller relaxation time and less heat resistance than the pristine. CCS2-HA possessed rich defects to reduce crystalline region, increase amorphous region, enhance segmental motion, and assist short range ion migration for less internal resistance and heat dissipation as novel filler for superior solid-state energy storage devices.

Time-intended effect on electrochemical performance of hydrothermally reduced graphene oxide nanosheets: Design and study of solid-state symmetric supercapacitor

Self-organized porous sheet-like assemblies have attracted extensive attention for the development of flexible high-performance electrodes. This work demonstrates the facile synthesis and effects of reduction time on the electrochemical performance of porous sheet-like assemblies of reduced graphene oxide (rGO) on carbon cloth. An rGO porous assembly with a reduction time of 4 h exhibited a superior specific capacitance of 456 F/g at a scan rate of 5 mV/s and 223 F/g at a current density of 1 mA/cm2, with ~ 93.9% initial capacity retention over 2000 cycles. A solid-state symmetric supercapacitor device constructed of a rGO4//rGO4 porous assembly achieved a specific capacitance of 45.86 F/g at a scan rate of 5 mV/s and yielded an energy density of 1.27 Wh/kg and specific power of 833.3 W/kg in a PVA-H2SO4 gel polymer electrolyte. Furthermore, the flexible solid-state symmetric device provides outstanding cyclic stability with a 95.3% retention of its initial capacity over 2000 cycles. Thus, electrodes constructed of rGO porous sheets show great potential for flexible and transparent solid-state symmetric energy storage devices.

All-3D-printed solid-state microsupercapacitors

Recently, miniaturized electrochemical energy storage units have gained tremendous attention in the fields of microelectronic electronics systems, with the advent of the era of “internet of things”. Shape configurable energy storage devices can be implemented on arbitrarily designable electronics system through 3D printing on the designated surfaces of device systems. In this study, we have developed a methodology of fabricating an all-3D-printed solid-state energy storage device by sequentially printing 3D-printable highly viscous fluids for metallic current collector, electrode and electrolyte layers. The Ni metallic current collector that can be operated stably at a high voltage condition of 3 V, is formed by a combinatorial approach of using 3D printing and 3D laser sintering processes. An intact physical interaction is interpreted comprehensively for the particles residing inside the printed particulate layer and the photons irradiated from a green laser source, based on an in-depth comparative investigation of experimental data and electromagnetic simulation result. A graphene nanoplatelet-based electrode fluid and an ionic liquid-based UV curable electrolyte fluid are printed successively on top of 3D-structured current collectors. It is demonstrated that the all-3D-printed microsupercapacitor device delivers the energy density and power density of 25.4 to 8.5 μWh•cm−2 and 150 to 6,483 μW•cm−2, respectively, even approaching the state-of-the-art level for flat-type conventional devices.

Binder-free NiCoFe layered double hydroxide nanosheets for flexible energy storage devices with high-rate-retention characteristics

In this study, NiCoFe layered double hydroxide (LDH) nanosheets with various composition ratios are synthesized via a simple electrodeposition method. The NiCoFe LDH prepared with a precursor molar ratio of Ni:Co:Fe = 1:2:0.1 shows the best performance with a specific capacity of 727 C g − 1 at 1 A g − 1, a high rate retention of 77% at 50 A g − 1, and a capacity retention of 87% after 10,000 cycles. The quick in-operando X-ray absorption study shows that the electrochemical activity of the various LDHs mainly originates from the change in the valence state of Ni ions, and the Fe ions improve the rate capability as well as the cycling stability. Furthermore, a solid-state energy storage device is fabricated using the NiCoFe-(1:2:0.1) LDH as the positive electrode, commercial activated carbon as the negative electrode, and PVA-KOH as the electrolyte. The device exhibits an energy density of 8.7 Wh kg−1 at 62.8 W kg−1 and 6.8 Wh kg−1 at 3139.2 W kg−1. The cycling stabilities of the device under folding and unfolding conditions are also evaluated, and the performances are found about the same, revealing great potential for flexible energy storage applications.

An extra-wide temperature all-solid-state lithium-metal battery operating from −73 ℃ to 120 ℃

All-solid-state lithium-metal batteries (ASS LMBs) shows a huge advantage in developing safe, high-energy-density and wide operating temperature energy storage devices. However, most ASS lithium-ion batteries need to work at a relatively high temperature range (~55 ℃ to 70 ℃) due to the low kinetics of lithium-ions transfer in electrolytes/electrodes and their interfaces. Here, we report an extra-wide temperature ASS lithium-air battery operating from −73 ℃ to 120 ℃ via harvesting and converting solar energy where ruthenium oxide nanoparticles (RuO2 NPs) assembled on CNTs as a plasmonic air cathode has been used to harvest a broad solar spectrum (>90% absorption efficiency, 200 nm to 2500 nm) and convert it into heat to improve the charge transmission and storage in electrolyte/electrodes. Such battery demonstrates a high discharge capacity of ~2500 mAh g-1 (corresponding CE >88%) with a 200 mA g-1 current density even operating at -73 ℃. Also, the battery shows a stable cycle performance with a limited discharge/charge capacity of 500 mAh g-1 at an extra-wide operating temperature from −73 ℃ to 120 ℃. This battery technology paves a way for developing extra-wide operating temperature solid-state energy storage devices.

N-doped reduced graphene oxide (rGO) wrapped carbon microfibers as binder-free electrodes for flexible fibre supercapacitors and sodium-ion batteries

In this study, N-doped reduced graphene oxide (rGO) wrapped carbon micro fibres (CFs) were synthesized by one-step high temperature pyrolysis method. Free-standing binder-free electrodes of N-doped rGO on CF were fabricated to apply in extended flexible fibrous supercapacitors and sodium-ion batteries (NIBs). The results showed that the attachment of N-doped graphene onto CF led to high electrochemical capacitance properties. The micro-fibre electrodes showed high performance supercapacitor behaviour of 18.7 F cm−3 at a current density of 1 A cm−3 as a flexible solid-state energy storage device. In parallel with the supercapacitance properties, the micro-fibre electrode shows impressive electrochemical performances when evaluated as anode for NIB, delivering a reversible capacity of 400 mAh/g with capacity retention approaching 100% after 100 cycles. The excellent performances are attributed to defects induced by N-doping along with large surface area of hierarchical porous architecture that can facilitate the storage and diffusion of Na+ and prevent the restacking of rGO during cycling. Thus, these N-doped rGO fibrous materials have substantial promise for fabricating extended flexible cable electronics and NIBs with superior strength and performance.

Highly conductive locust bean gum bio-electrolyte for superior long-life quasi-solid-state zinc-ion batteries.

Rechargeable aqueous zinc-ion batteries (ZIBs) are promising wearable electronic power sources. However, solid-state electrolytes with high ionic conductivities and long-term stabilities are still challenging to fabricate for high-performance ZIBs. Herein, locust bean gum (LBG) was used as a natural bio-polymer to prepare a free-standing quasi-solid-state ZnSO4/MnSO4 electrolyte. The as-obtained LBG electrolyte showed high ionic conductivity reaching 33.57 mS cm−1 at room temperature. This value is so far the highest among the reported quasi-solid-state electrolytes. Besides, the as-obtained LBG electrolyte displayed excellent long-term stability toward a Zn anode. The application of the optimized LBG electrolyte in Zn–MnO2 batteries achieved a high specific capacity reaching up to 339.4 mA h g−1 at 0.15 A g−1, a superior rate performance of 143.3 mA h g−1 at 6 A g−1, an excellent capacity retention of 100% over 3300 cycles and 93% over 4000 cycles combined with a wide working temperature range (0–40 °C) and good mechanical flexibility (capacity retention of 80.74% after 1000 bending cycles at a bending angle of 90°). In sum, the proposed ZIBs-based LBG electrolyte with high electrochemical performance looks promising for the future development of bio-compatible and environmentally friendly solid-state energy storage devices.

Excellent film-forming, ion-conductive, zwitterionic graft copolymer electrolytes for solid-state supercapacitors

Polymer electrolytes with robust mechanical properties and high ionic conductivity are highly desirable for solid-state energy storage devices. Therefore, in this study, a polymer electrolyte based on a zwitterionic graft copolymer, poly(vinyl alcohol)-graft-poly(sulfobetaine methacrylate) (PVA-g-PSBMA), is developed. Herein, we designed a graft copolymer that utilizes the excellent film-forming nature of PVA main chains and ion-conductive properties of polyzwitterionic PSBMA side chains. The PVA-g-PSBMA electrolytes exhibited microphase separated structures, wherein H3PO4 interacted more strongly with the PSBMA domains. Therefore, the transport of proton ions was facilitated through the well-defined PSBMA-based ion channels, leading to a significant increase in the ionic conductivity. The polymer electrolyte was applied to the electric double-layer capacitor (EDLC) with activated carbon-based electrode. In comparison with the neat conventional PVA-based cell, the solid EDLC with PVA-g-PSBMA zwitterionic graft copolymer electrolytes showed improved specific capacitance (46.6 F g−1), energy density (3.67 Wh kg−1), and power density (186 W kg−1). The improved performance can be attributed to the higher ionic conductivity and better interfacial compatibility of electrode/electrolyte for the PVA-g-PSBMA electrolytes.

In Situ Formation of "Dimethyl Sulfoxide/Water-in-Salt"-Based Chitosan Hydrogel Electrolyte for Advanced All-Solid-State Supercapacitors.

Biodegradable hydrogel electrolytes are particularly attractive in the fabrication of all-solid-state supercapacitors due to environmental benignity and avoiding of leakage. The introduction of "water-in-salt" (WIS) electrolytes into hydrogels will further broaden the electrochemical stability window of aqueous supercapacitors significantly. Meanwhile, the addition of an organic co-solvent can effectively overcome the inevitable salt precipitation and extend the temperature adaptability. Herein, an in situ cross-linking approach was demonstrated without any extra binder to obtain a "dimethyl sulfoxide/water-in-salt"-based (DWIS) chitosan hydrogel electrolyte. Interestingly, the addition of 4-7 mol L-1 of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salts not only conforms to the criterion of WIS, but also promoted the successful gelation through the supramolecular complexation between Li+ -solvated complexes and chitosan chains. A hydrogel-based all-solid-state supercapacitor was fabricated using the DWIS chitosan hydrogel as the electrolyte and separator while nitrogen-doped graphene hydrogel (NG) was used as the electrode. The optimized supercapacitor with a wide operating voltage of 2.1 V showed a high specific capacitance of 107.6 F g-1 at 1 A g-1 , remarkable capacitance retention of 80.1 % after 5000 cycles, a superior energy density of 62.9 Wh kg-1 at a power density of 1025.5 W kg-1 , and excellent temperature stability in the range of -20 to 70 °C. These findings suggest that the as-prepared hydrogel electrolyte holds great potential in the practical application of high-performance solid-state energy storage devices.

Enhanced Solar-Driven-Heating and Tough Hydrogel Electrolyte by Photothermal Effect and Hofmeister Effect.

Although plenty of progress and achievements are made on hydrogel electrolyte researches, the inherent inferior low-temperature performance of hydrogel electrolyte is still a severe challenge for wider application on the energy storage devices, due to the high content of water within hydrogel. Herein, an enhanced solar-driven-heating composite hydrogel electrolyte and a solar-driven-heating graphene based micro-supercapacitor are developed utilizing the photothermal conversion ability and self-initiation of MoS2 nanosheets and additional Hofmeister effect. The MoS2 composite hydrogel electrolyte not only improves the reliability of micro-supercapacitor owing to its splendid mechanical properties, but also endows the micro-supercapacitor with superior low-temperature electrochemical performance and broadens its operating environment to a much lower temperature (-56 °C), which should be attributed to the excellent ability in converting endless solar energy into required thermal energy. These efforts would construct a new application platform for solar energy conversion and present an efficient method to structure severe-cold resistant solid state energy storage devices for next-generation.

Boosting the safety and energy density of molybdenum disulfide/carbon nanotubes based solid-state sodium-ion supercapacitors with an ionogel electrolyte

Solid-state energy storage devices exhibit superior safety and energy density. However, their practical applications are still limited by the lower conductivity and ion transfer rate. The performances of sodium ion capacitors (SICs) are determined by the combination of device configuration, electrodes, and electrolyte. Therefore, the configuration optimization of solid-state SICs (SS-SICs) is critically important. Here, the fabrication of a safer high-energy-density SS-SIC is demonstrated by using flake-shaped molybdenum disulfide/carbon nanotube nanohybrids and sodium-ion ionogel electrolytes. The microstructures of nanohybrids could support shortened migration paths for sodium ions and can buffer the volume change of electrochemical reactions. Moreover, the optimized sodium-ion ionogel electrolyte was found to exhibit improved flame-retardant ability, accelerated ionic conductivity, and excellent sodium migration rate. Electrochemical analysis and molecular simulation methods of energy storage behaviors were used to uncover the origin of improved performances at higher temperatures. The optimized SS-SIC could deliver a high energy density up to 115.7 W h kg−1 at 70 °C and excellent durability with 81% retention after 8000 cycles. Therefore, a new energy supply device is provided for equipment operating at higher temperatures.

Using Operando Electrochemical TEM as Part of a Correlative Approach to Characterize Failure Modes in Solid-state Energy Storage Devices

Journal Article Using Operando Electrochemical TEM as Part of a Correlative Approach to Characterize Failure Modes in Solid-state Energy Storage Devices Get access Nikhilendra Singh, Nikhilendra Singh Toyota Research Institute of North America, Ann Arbor, Michigan, United States Search for other works by this author on: Oxford Academic Google Scholar James Horwath, James Horwath University of Pennsylvania, Philadelphia, Pennsylvania, United States Search for other works by this author on: Oxford Academic Google Scholar Timothy Arthur, Timothy Arthur Toyota Research Institute of North America, Ann Arbor, Michigan, United States Search for other works by this author on: Oxford Academic Google Scholar Daan Hein Alsem, Daan Hein Alsem Hummingbird Scientific, Lacey, Washington, United States Search for other works by this author on: Oxford Academic Google Scholar Eric Stach Eric Stach University of Pennsylvania, Philadelphia, Pennsylvania, United States Search for other works by this author on: Oxford Academic Google Scholar Microscopy and Microanalysis, Volume 26, Issue S2, 1 August 2020, Pages 1460–1461, https://doi.org/10.1017/S1431927620018206 Published: 01 August 2020

An ultrathin robust polymer membrane for wearable solid-state electrochemical energy storage

Abstract Developing lightweight, flexible, and foldable electrodes with decent mechanical durability and electrochemical activity is a highly desirable goal for solid-state electrochemical energy storage devices yet remains a formidable challenge to overcome. Herein, we invent a freestanding robust PANI membrane via introducing the dynamic boronate bond to bridge rigid PANI chains with complaint polyvinyl alcohol (PVA) chains. The resultant PANI/PVA membrane (PPM) exhibits remarkable elasticity (17.8% strain) along with excellent tensile strength (33.7 MPa), outperforming the majority of existing state-of-the-art flexible electrochemical PANI membranes. Additionally, the PPM can be further assembled into a wearable solid-state supercapacitor with high electrochemical performance as well as decent mechanical durability. The lightweight, flexible, and foldable PANI membrane represents a great advancement in electrode materials for next-generation wearable solid-state electrochemical energy storage devices.

Single-pot hydrothermal synthesis of manganese phosphate microrods as a cathode material for highly stable flexible solid-state symmetric supercapacitors

Here, we report a binder-free synthesis of microrods-like manganese phosphate thin film over stainless steel substrate by a facile, single-pot hydrothermal method. The XRD analysis reveals that, the formation of manganese phosphate [Mn3(PO4)2] material of a monoclinic crystal structure. From SEM images observed microrods like morphology of manganese phosphate with an average width of ∼25 μm. The manganese phosphate electrode shows a better electrochemical performance with a specific capacitance of 145 F g−1 at 0.2 mA cm-2 current density in 1.0 M Na2SO4 electrolyte. Moreover, the flexible solid-state symmetric electrochemical energy storage device was assembled with PVA-Na2SO4 solid gel-electrolyte consists of manganese phosphate as anode and cathode electrode. The corresponding symmetric supercapacitor achieves a high energy density of 11.7 Wh kg−1 at a high power density of 1.41 kW kg−1 with an excellent specific capacitance of 37 F g−1 at 0.1 mA cm-2 current density. Manganese phosphate shows long-term electrochemical cyclic stability at a current density of 0.8 mA cm-2 for 9000 galvanostatic charge-discharge cycles with excellent capacitance retention (99 %). This excellent capacitive performance confirms that the manganese phosphate is promising material and fabricated flexible solid-state symmetric supercapacitor has high potential in the field of portable and bendable energy storage devices.

Intrinsic Ion Transport Properties of Block Copolymer Electrolytes.

Knowledge of intrinsic properties is of central importance for materials design and assessing suitability for specific applications. Self-assembling block copolymer electrolytes (BCEs) are of great interest for applications in solid-state energy storage devices. A fundamental understanding of ion transport properties, however, is hindered by the difficulty in deconvoluting extrinsic factors, such as defects, from intrinsic factors, such as the presence of interfaces between the domains. Here, we quantify the intrinsic ion transport properties of a model BCE system consisting of poly(styrene-block-ethylene oxide) (SEO) and lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) salt using a generalizable strategy of depositing thin films on interdigitated electrodes and self-assembling fully connected parallel lamellar structures throughout the films. Comparison between conductivity in homopolymer poly(ethylene oxide) (PEO)-LiTFSI electrolytes and the analogous conducting material in SEO over a range of salt concentrations (r, molar ratio of lithium ion to ethylene oxide repeat units) and temperatures reveals that between 20% and 50% of the PEO in SEO is inactive. Using mean-field theory calculations of the domain structure and monomer concentration profiles at domain interfaces-both of which vary substantially with salt concentration-the fraction of inactive PEO in the SEO, as derived from conductivity measurements, can be quantitatively reconciled with the fraction of PEO that is mixed with greater than a few volume percent of polystyrene. Despite the detrimental interfacial effects for ion transport in BCEs, the intrinsic conductivity of the SEO studied here (ca. 10-3 S/cm at 90 °C, r = 0.085) is an order of magnitude higher than reported values from bulk samples of similar molecular weight SEO (ca. 10-4 S/cm at 90 °C, r = 0.085). Overall, this work provides motivation and methods for pursuing improved BCE chemical design, interfacial engineering, and processing.

Interfacial integration and roll forming of quasi-solid-state Li–O2 battery through solidification and gelation of ionic liquid

The development of solid-state lithium-oxygen batteries is currently limited primarily by the high solid-solid interfacial resistance and the lack of efficient assembly of electrolyte and electrode. In this work, noncovalent interactions between the cations of an ammonium ionic liquid and both solid electrolytes and carbon air cathodes are introduced. The ionic liquid-based electrolytes (ILE) are solidified on Li6·40La3Zr1·40Ta0·60O12 (LLZTO) nanoparticles and gelated by multi-wall carbon nanotubes (MWCNTs), respectively, to construct LLZTO@ILE quasi-solid-state electrolyte (QSSE) and MWCNTs-LLZTO/ILE gel cathode (GC). The QSSE exhibits a high ionic conductivity of 1.71 × 10−3 S cm−1 at 60 °C, high Li-ion transference number of 0.56, broad electrochemical window of ~4.8 V and good thermal stability. The GC shows outstanding compatibility with QSSE. Quasi-solid-state Li–O2 batteries are assembled by integrating QSSE and GC films with a facile roll forming method, showing a low total interfacial resistance (~87 Ω cm2), and excellent reversible cycles (70 cycles) with low charge overpotential (<0.44 V) and quite high electrical energy efficiency (>70%) at 60 °C and 200 mA g−1. A 0.12 Ah pouch-type Li–O2 battery was achieved by this method. These results suggest that the noncovalent interactions initiated by IL cations could be an effective approach to solve the solid-solid interface issue and achieve high discharge capacity in solid-state energy storage devices.