Ionic Conductivity Research Articles

Novel Amorphous Nitride-Halide Solid Electrolytes with Enhanced Performance for All-Solid-State Batteries.

Solid electrolytes (SEs) in all-solid-state batteries (ASSBs) are garnering considerable attention for their potential applications in next-generation energy storage systems. Amorphous SEs with dual-anion hold great promise for achieving favorable performance, such as high ionic conductivity and good compatibility with electrodes within ASSBs. Here, we discover a family of amorphous nitride-halide SEs, Li3xMClyNx (M=Ta or La, 1≤3x≤1.4, y=5 or 3), which can achieve ionic conductivities up to 7.34 mS cm-1 at 30 °C. The amorphous properties and local structures are investigated using powder X-ray diffraction, cryogenic transmission electron microscopy, and atomic pair distribution function analysis. Impressively, ASSBs employing amorphous Li3xTaCl5Nx have demonstrated good performance at high rates and charging voltages, as well as at low temperature.

Interface engineering of electron-ion dual transmission channels for ultra-long lifespan quasi-solid zinc-ion batteries

Hydrogel electrolytes have emerged as effective strategies to prolong the lifespan of aqueous zinc ion batteries (AZIBs). However, dendrites and side reactions are still inescapable due to the residual active water and chaotic migration of Zn2+. Herein, a super stable Zn anode is realized through the synergistic effect of interfacial electron-ion dual transmission channels (EIDC) and an intermediate sodium alginate (SA) gel. Specifically, the SA gel can adjust the solvation structure of Zn2+ and weaken the strong bonding of Zn2+ and H2O molecules. The EIDC polymer layer (PEDOT:PSS) is engineered on the SA hydrogel surfaces, in which PSS chains can offer uniform ion transmission channels via the electrostatic interaction between SO3– groups and Zn2+. While another PEDOT chains can provide electron conducting channels through the conjugated π-π bonds to accelerate charge exchange. Benefiting from the synergistic effect of EIDC polymer layer and SA gel, the as-prepared SA/EIDC gel electrolyte achieves a high ionic conductivity of 41 mS cm–1. The Zn//Zn symmetric batteries exhibit a super-long lifespan of 6750 h at 1 mA cm–2 and 1 mAh cm–2 (>9 months), and cycling life of MnO2-Zn full battery surpasses 4000 cycles. This work presents a new perspective on designing hydrogel electrolytes towards ultra-long lifespan ZIBs.

Electrolyte Design via Cation-Anion Association Regulation for High-Rate and Dendrite-Free Zinc Metal Batteries at Low Temperature.

Low-temperature zinc metal batteries (ZMBs) are highly challenged by Zn dendrite growth, especially at high current density. Here, starting from the intermolecular insights, we report a cation-anion association modulation strategy by matching different dielectric constant solvents and unveil the relationship between cation-anion association strength and Zn plating/stripping performance at low temperatures. The combination of comprehensive characterizations and theoretical calculations indicates that moderate ion association electrolytes with high ionic conductivity (12.09 mS cm-1 at -40 °C) and a stable anion-derived solid electrolyte interphase (SEI) jointly account for highly reversible and dendrite-free Zn plating/stripping behavior, resulting in high-rate and ultrastable cycle performance at low temperature. As a result, at -40 °C, Zn//Zn cells can stably cycle over 400 h at 5 mA cm-2 and 10 mAh cm-2 and Zn//Cu cells exhibit an exceptional average Coulombic efficiency (CE) of 99.91% for 1800 cycles at 1 mA cm-2 and 1 mAh cm-2. Benefiting from enhanced low-temperature Zn plating/stripping performance, Zn//PANI full cells stably operate for 12,000 cycles at 0.5A g-1 and 35,000 cycles at 5 A g-1. Impressively, at -60 °C, Zn//Cu cells still display a high average CE of 99.68% for 2000 cycles. This work underscores the crucial effect of cation-anion association regulation for high-rate and dendrite-free Zn metal anodes, deepening the understanding of intermolecular interaction insights for low-temperature electrolyte design.

Isoleucine gate blocks K+ conduction in C-type inactivation.

Many voltage-gated potassium (Kv) channels display a time-dependent phenomenon called C-type inactivation, whereby prolonged activation by voltage leads to the inhibition of ionic conduction, a process that involves a conformational change at the selectivity filter toward a non-conductive state. Recently, a high-resolution structure of a strongly inactivated triple-mutant channel kv1.2-kv2.1-3m revealed a novel conformation of the selectivity filter that is dilated at its outer end, distinct from the well-characterized conductive state. While the experimental structure was interpreted as the elusive non-conductive state, our molecular dynamics simulations and electrophysiological measurements show that the dilated filter of kv1.2-kv2.1-3m is conductive and, as such, cannot completely account for the inactivation of the channel observed in the structural experiments. The simulation shows that an additional conformational change, implicating isoleucine residues at position 398 along the pore lining segment S6, is required to effectively block ion conduction. The I398 residues from the four subunits act as a state-dependent hydrophobic gate located immediately beneath the selectivity filter. By mutating I398 to Asparagine, ion permeation can be resumed in the kv1.2-kv2.1-3m channel, which was not a reversion C-type inactivation, since AgTxII fails to block the ionic permeation of kv1.2-kv2.1-3m_I398N. As a critical piece of the C-type inactivation machinery, this structural feature is the potential target of a broad class of QA blockers and negatively charged activators thus opening new research directions towards the development of drugs that specifically modulate gating-states of Kv channels.

Development of Tailored Hydrocarbon‐Based Pentablock Copolymer Membranes for Sodium‐Polysulfide Flow Batteries

AbstractLong‐duration energy storage (LDES) technologies are pivotal for the adoption of renewables like wind and solar. Non‐aqueous redox flow batteries (NARFBs) with a sodium‐polysulfide hybrid system feature high energy density independent of power density, yet face challenges with polysulfide shuttling. This study investigates a hydrocarbon‐based penta‐block copolymer membrane, Nexar, to mitigate crossover effects by balancing TFSI conversion and their crosslink density. The membranes are annealed to induce crosslinking for reducing electrolyte uptake and enhancing mechanical stability while demonstrating excellent ionic conductivity. The hydrocarbon‐based membranes address environmental concerns associated with perfluoroalkyl substances and improve the performance and durability of NARFBs. Our findings suggest that annealed Nexar membranes with tailored TFSI functionality offer a scalable, cost‐effective solution for enhancing the efficiency of high‐capacity energy storage systems, pivotal for grid integration of renewable sources.

Engineering Stable Decomposition Products on Cathode Surfaces to Enable High Voltage All‐Solid‐State Batteries

Sulfide solid electrolytes such as Li6PS5Cl hold high promise for solid state batteries due to their high ionic conductivity; however, their oxidation potential of ~2.5 V is not compatible with high voltage Ni‐rich cathodes such as LiNixCoyMn1−x−yO2 (x≥0.8). Here, we devise an effective, conformal and thin coating on the cathode active material guided by density functional theory, which suppresses the oxidative decomposition of Li6PS5Cl as shown by experiment. The nanometric coating on nickel‐rich NMC85 enabled capacity retention of 82% after 200 cycles (2.8‐4.3 V vs Li+/Li) using Li6PS5Cl as the solid electrolyte. In comparison, cells with an uncoated CAM only displayed 56% capacity retention. The coated‐NCM85 cells also demonstrate much better rate performance and higher capacity. The enhanced performance is due to the formation of a stable amorphous cathode‐electrolyte interphase accruing from the decomposition products of the LiPO2F2 precursor (as predicted by DFT), which protect the sulfide electrolyte from oxidation. The coating fabricated in this cost‐effective process showed superior performance to state‐of‐the‐art coatings such as LiNbO3. This work highlights the importance of rationally designing stable coating materials based on their potential decomposition products and confirms the suitability of a low‐cost and conformal coating to enable sulfide electrolyte‐based all‐solid‐state batteries.

A New Class of Oxyhalide Solid Electrolytes NaNbCl6‐2xOx for Solid‐state Sodium Batteries

AbstractSodium‐based batteries are gaining momentum due to the abundance and lower cost of sodium compared to lithium. Solid‐state sodium batteries can also provide further safety advantages. However, sodium‐based solid‐state electrolytes (SSEs) that meet all the rigorous requirements, such as high ionic conductivity, oxidative stability with the cathode, and ease of processability, are lacking. We present here a new class of sodium‐based oxyhalide electrolytes NaNbCl6‐2xOx with a facile mechanochemical synthesis. The oxyhalide NaNbCl4O exhibits close to two orders of magnitude higher ambient‐temperature sodium‐ion conductivity (1.03×10−4 S cm−1) compared to the halide counterpart NaNbCl6 (3×10−6 S cm−1). Structural motifs unique to the oxygen content in NaNbCl6‐2xOx are identified with 23Na and 93Nb magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy and x‐ray diffraction (XRD). Solid‐state sodium batteries assembled with NaNbCl4O electrolyte and the cobalt‐ and nickel‐free layered Na0.70Fe0.3Mn0.65Al0.05O2 cathode exhibit a maximum discharge capacity of 155 mAh g−1 with good cycle life at ambient temperature.

Ultra‐Tough Dynamic Supramolecular Ion‐Conducting Elastomer Induced Uniform Li+ Transport and Stabilizes Interphase Ensures Dendrite‐Free Lithium Metal Anodes

AbstractArtificial polymer solid electrolyte interphases (SEIs) with microphase‐separated structures provide promising solutions to the inhomogeneity and cracking issues of natural SEIs in lithium metal batteries (LMBs). However, achieving homogeneous ionic conductivity, excellent mechanical properties, and superior interfacial stability remains challenging due to interference from hard‐phase domains in ion transport and solid‐solid interface issues with lithium metal. Herein, we present a dynamic supramolecular ion‐conducting poly (urethane‐urea) interphase (DSIPI) that achieves these three properties through modulating the hard‐phase domains and constructing a composite SEI in situ. The soft‐phase polytetrahydrofuran backbone, featuring loose Li+−O coordinating interactions, ensures uniform Li+ transport. Concurrently, sextuple hydrogen bonds in the hard phase dissipate strain energy through sequential bond cleavage, thereby imparting exceptional mechanical properties. Moreover, enriched bis (trifluoromethanesulfonyl) imide anion (TFSI−) in DSIPI promotes the in situ formation of a stable polymer‐inorganic composite SEI during cycling. Consequently, the DSIPI‐protected lithium anode (DSIPI@Li) enables symmetric cells with exceptional cyclability exceeding 4,000 hours at an ultra‐high current density of 20 mA cm−2, thereby demonstrating excellent cycling stability. Furthermore, DSIPI@Li facilitates stable operation of the pouch cells under the constraints of a high‐loading LiNi0.8Co0.1Mn0.1O2 cathode and low negative/positive capacity (N/P) ratio. This work presents a powerful strategy for designing artificial SEIs and high‐performance LMBs.

Engineering Stable Decomposition Products on Cathode Surfaces to Enable High Voltage All-Solid-State Batteries.

Sulfide solid electrolytes such as Li6PS5Cl hold high promise for solid state batteries due to their high ionic conductivity; however, their oxidation potential of ~2.5 V is not compatible with high voltage Ni-rich cathodes such as LiNixCoyMn1-x-yO2 (x≥0.8). Here, we devise an effective, conformal and thin coating on the cathode active material guided by density functional theory, which suppresses the oxidative decomposition of Li6PS5Cl as shown by experiment. The nanometric coating on nickel-rich NMC85 enabled capacity retention of 82% after 200 cycles (2.8-4.3 V vs Li+/Li) using Li6PS5Cl as the solid electrolyte. In comparison, cells with an uncoated CAM only displayed 56% capacity retention. The coated-NCM85 cells also demonstrate much better rate performance and higher capacity. The enhanced performance is due to the formation of a stable amorphous cathode-electrolyte interphase accruing from the decomposition products of the LiPO2F2 precursor (as predicted by DFT), which protect the sulfide electrolyte from oxidation. The coating fabricated in this cost-effective process showed superior performance to state-of-the-art coatings such as LiNbO3. This work highlights the importance of rationally designing stable coating materials based on their potential decomposition products and confirms the suitability of a low-cost and conformal coating to enable sulfide electrolyte-based all-solid-state batteries.

Thermodynamic modeling of the structure of alkali aluminophosphate glasses and their ionic conductivity

AbstractThis study presents the structural and ionic conductivity thermodynamic modeling for glasses with compositions in the system 50M2O‐xAl2O3‐(50 − x)P2O5, with M = Li or K. The Shakhmatkin and Vedishcheva thermodynamic model (SVTDM), or associated solutions model, has been previously used in successfully predicting the structure of simple binary phosphate glasses and it has now been employed with the aim to discerning the model's capability to predict the structural changes induced in the phosphate network by the addition of alumina. The results have been furthermore validated through their comparison with literature experimental data on the structural characterization of the glasses by 31P NMR measurements as well as on ionic conductivity determined by impedance spectroscopy. Although this methodology demonstrates good agreement with experimental data on the structure of aluminophosphate glasses, some disparities persist, potentially arising from experimental uncertainties. However, SVTDM faces limitations, including the need for comprehensive knowledge of stable phases and their formation energies. Predictions of ionic conductivity, though promising, exhibit deviations from experimental values, attributed to factors such as the influence of the chemical environment on dielectric properties. To enhance accuracy in conductivity prediction, a deeper understanding of additional variables such as dielectric constant and attempt frequency is imperative.

Self-healing electronic skin with high fracture strength and toughness

Human skin is essential for perception, encompassing haptic, thermal, proprioceptive, and pain-sensing functions through ion movement. Additionally, it is mechanically resilient and self-healing for protection. Inspired by these unique properties, researchers have attempted to develop stretchable, self-healing sensors based on ion dynamics. However, most self-healing sensors reported to date suffer from low fracture strength and toughness. In this work, we present an ion-based self-healing electronic skin with exceptionally high fracture strength and toughness. We enhanced self-healing polymers and ionic conductors by introducing two types of orthogonal dynamic crosslinking bonds: dynamic aromatic disulfide bonds and 2-ureido-4-pyrimidone moieties. These dynamic bonds provide autonomous self-healing and high mechanical toughness even in the presence of ionic liquids. As a result, our self-healing polymer and self-healing ionic conductor exhibit remarkable stretchability (700%, 850%), fracture strength (34 MPa, 30 MPa), and toughness (78.5 MJ/m3, 87.3 MJ/m3), the highest values reported among self-healing ionic conductors to date. Using our materials, we developed various fully self-healing sensors and a soft gripper capable of autonomously recovering from mechanical damage. By integrating these components, we created a comprehensive self-healing electronic skin suitable for soft robotics applications.

Antifreezing functionalized-alginate-based electrolytes for zinc-ion batteries

Flexible zinc-ion batteries (ZIBs) assembled with hydrogel electrolyte are considered as promising flexible energy storage devices because of their inherent safety and versatility. However, the ionic conductivity and mechanical properties of most hydrogel electrolytes are not satisfactory, Furthermore, they will freeze at subzero temperature due to existing water. In this work, a freezing resistant polycarboxylic double network gel electrolyte (SIP-CS) with high ionic conductivity (14.36 mS cm⁻1 at −20 °C) and excellent mechanical property (fracture stress of 241.5 kPa and fracture strain of 1011 %) is prepared. Iminodiacetic acid (IDA) is applied to modify the alginate mainchains with many -COOH groups, which could provide channels for ion migration and endow hydrogel with high ionic conductivity. Additionally, sorbitol, containing lots of hydroxyl groups, is applied as a cryoprotectant to enhance the subzero performance of the electrolyte, because sorbitol could break the hydrogen bonds between water molecules, inhibit the formation of ice crystals, and reduce the freezing point of the gel electrolyte. The freezing point of SIP-CS is −37.0 °C, enabling the electrolyte to perform well at low temperatures. The flexible quasi solid Zn-MnO2 battery is assembled to evaluate the low-temperature electrochemical performance of SIP-CS. The assembled Zn-MnO2 battery shows good cycling and stable electrochemical performance, which proves the excellent antifreezing property of SIP-CS. This work provides a new strategy for preparing an electrolyte with good withstand low-temperature capability.

Interdependence of Support Wettability - Electrodeposition Rate- Sodium Metal Anode and SEI Microstructure.

This study examines how current collector support chemistry (sodiophilic intermetallic Na2Te vs. sodiophobic baseline Cu) and electrodeposition rate affect microstructure of sodium metal and its solid electrolyte interphase (SEI). Capacity and current (6 mAh cm-2, 0.5-3 mA cm-2) representative of commercially relevant mass loading in anode-free sodium metal battery (AF-SMBs) are analyzed. Synchrotron X-ray nanotomography and grazing-incidence wide-angle X-ray scattering (GIWAXS) are combined with cryogenic ion beam (cryo-FIB) microscopy. Highlighted are major differences in film morphology, internal porosity, and crystallographic preferred orientation e.g. (110) vs. (100) and (211) with support and deposition rate. Within the SEI, sodium fluoride (NaF) is more prevalent with Te-Cu versus sodium hydride (NaH) and sodium hydroxide (NaOH) with baseline Cu. Due to competitive grain growth the preferred orientation of sodium crystallites depends on film thickness. Mesoscale modeling delineates the role of SEI (ionic conductivity, morphology) on electrodeposit growth and onset of electrochemical instability.

Ultra-Tough Dynamic Supramolecular Ion-Conducting Elastomer Induced Uniform Li+ Transport and Stabilizes Interphase Ensures Dendrite-Free Lithium Metal Anodes.

Artificial polymer solid electrolyte interphases (SEIs) with microphase-separated structures provide promising solutions to the inhomogeneity and cracking issues of natural SEIs in lithium metal batteries (LMBs). However, achieving homogeneous ionic conductivity, excellent mechanical properties, and superior interfacial stability remains challenging due to interference from hard-phase domains in ion transport and solid-solid interface issues with lithium metal. Herein, we present a dynamic supramolecular ion-conducting poly (urethane-urea) interphase (DSIPI) that achieves these three properties through modulating the hard-phase domains and constructing a composite SEI in situ. The soft-phase polytetrahydrofuran backbone, featuring loose Li+-O coordinating interactions, ensures uniform Li+ transport. Concurrently, sextuple hydrogen bonds in the hard phase dissipate strain energy through sequential bond cleavage, thereby imparting exceptional mechanical properties. Moreover, enriched bis (trifluoromethanesulfonyl) imide anion (TFSI-) in DSIPI promotes the in situ formation of a stable polymer-inorganic composite SEI during cycling. Consequently, the DSIPI-protected lithium anode (DSIPI@Li) enables symmetric cells with exceptional cyclability exceeding 4,000 hours at an ultra-high current density of 20 mA cm-2, thereby demonstrating excellent cycling stability. Furthermore, DSIPI@Li facilitates stable operation of the pouch cells under the constraints of a high-loading LiNi0.8Co0.1Mn0.1O2 cathode and low negative/positive capacity (N/P) ratio. This work presents a powerful strategy for designing artificial SEIs and high-performance LMBs.

A New Class of Oxyhalide Solid Electrolytes NaNbCl6-2xOx for Solid-state Sodium Batteries.

Sodium-based batteries are gaining momentum due to the abundance and lower cost of sodium compared to lithium. Solid-state sodium batteries can also provide further safety advantages. However, sodium-based solid-state electrolytes (SSEs) that meet all the rigorous requirements, such as high ionic conductivity, oxidative stability with the cathode, and ease of processability, are lacking. We present here a new class of sodium-based oxyhalide electrolytes NaNbCl6-2xOx with a facile mechanochemical synthesis. The oxyhalide NaNbCl4O exhibits close to two orders of magnitude higher ambient-temperature sodium-ion conductivity (1.03×10-4 S cm-1) compared to the halide counterpart NaNbCl6 (3×10-6 S cm-1). Structural motifs unique to the oxygen content in NaNbCl6-2xOx are identified with 23Na and 93Nb magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy and x-ray diffraction (XRD). Solid-state sodium batteries assembled with NaNbCl4O electrolyte and the cobalt- and nickel-free layered Na0.70Fe0.3Mn0.65Al0.05O2 cathode exhibit a maximum discharge capacity of 155 mAh g-1 with good cycle life at ambient temperature.

Understanding Electrochemical Reaction Mechanisms of All-Electrochem-Active Mg2Si Electrode in All-Solid-State Batteries.

To better understand the electrochemical reaction mechanism of the Mg2Si electrode in all-solid-state batteries (ASSBs), a rational all-electrochem-active Mg2Si electrode is first designed to minimize the inactive component-related interfacial degradation. This is due to its unique mixed conductivity properties, including a high electronic conductivity of up to 8.9 × 10-2 S cm-1 and an ionic conductivity of 9.7 × 10-5 S cm-1, which allow for fast charges transport. In ASSBs, the Mg2Si electrode exhibits a higher initial Coulombic efficiency of 83.5% at 300 mA g-1 compared with the Si electrode (72.3%). X-ray diffraction and X-ray photoelectron spectroscopy results demonstrate that intermediate products (LixMg2Si, Li-Si alloy, and Li-Mg alloy) can form when the Mg2Si electrode discharges to 0.01 V, and partial Mg2Si still does not react with lithium. This work provides valuable insights into the reaction mechanisms and guides optimization strategies for developing next-generation Si-based ASSBs.

Molecular Control Based on Electrostatically Driven Modification for Solid-State Lithium Metal Batteries.

With the rapid development of energy vehicles, the demand for high-safety and high-energy-density battery systems, such as solid-state lithium metal batteries, is becoming increasingly urgent. Polyethylene oxide (PEO), as a commonly used electrolyte in solid-state batteries, has the advantages of easy processing and good interface compatibility but also faces the issue of poor ionic conductivity. In this study, we have enhanced the mechanical properties and ion conductivity of PEO electrolytes significantly, stabilizing electrochemical cycling, utilizing positively charged MXene as a modifying material for PEO solid electrolytes and leveraging stronger electrostatic forces. With these enhanced properties, the modified solid electrolyte in Li/Li cells demonstrates excellent cycling stability of over 430 h at 0.1 mA cm-2. Furthermore, the Li/LiFePO4 cells show excellent cycling performance, and the capacity retention rate is 92.1%.

3D Printable Polymer Electrolytes for Ionic Conduction based on Protic Ionic Liquids.

A range of protic ionic liquids (PILs) based on tri-n-alkylammonium cations and mesylate/triflate anions were incorporated into a polymer matrix to form ionogels (IGs). These systems were investigated for their thermal and electrochemical behaviour, as well as under the aspect of ion motion via PFG-NMR. The ionic conductivities of the ILs/IGs are in the range of 10‑4-10-3Scm-1 at elevated temperatures and the diffusion coefficients were around 10‑11m2s-1. Successful 3D printing of an IG with 70wt% of IL is possible via stereolithography approaches, opening up applications in, e.g., structured ion-conductive membranes.

Investigation of Charge Transfer Mechanism and Dielectric Relaxation in CsCdCl3 Perovskite

ABSTRACTThe exceptional optoelectronic capabilities of all‐inorganic metal halide perovskite semiconductor components open up a multitude of possible applications. Among all the metal halides, the chloride of cesium cadmium has not been investigated in great detail. Here, we describe a straightforward method for creating CsCdCl3 perovskite single crystals using the slow evaporation solution growth approach. These were investigated by utilizing X‐ray powder diffraction, and optical and impedance spectroscopies. The creation of a single‐phase with a hexagonal‐type structure was verified by the X‐ray powder diffraction (XRPD) data. The compound's semiconductor characteristics were verified by the optical measurement, indicating a direct band‐gap value of about 3.16 eV. The absorption and reflectance spectrum was also used to calculate and explain the optical extinction coefficient, Urbach energy, and skin depth as functions of the input photon's wavelength. Besides, the impedance spectroscopy technique was employed to investigate the characteristics of this component, across a frequency range of 10−1 Hz to 106 Hz and at temperatures ranging from 313 K to 453 K. The frequency behavior of the AC conductivity, σac, was analyzed using the universal Jonscher law. The outcomes of the charge transport investigation on CsCdCl3 imply that the perovskite material possessed a quantum mechanical tunneling (QMT) model for T < 363 K and a large polaron tunneling (OLPT) paradigm for T > 363 K. A correlation between the ionic conductivity and the crystal structure was established and discussed. Ultimately, the low dielectric loss and high dielectric constant of CsCdCl3 make it a promising material for energy harvesting devices.

Highly stretchable, low-hysteresis, and antifreeze hydrogel for low-grade thermal energy harvesting in ionic thermoelectric Supercapacitors

Efficient harvest of low-grade waste heat in the environment through thermoelectric materials represents a promising strategy to address the current energy crisis. In practical applications, the mechanical properties of thermoelectric materials are crucial for their lifespan and operational environment. In this study, we designed a series of ionic thermoelectric hydrogels, PAM/CMC-xLiCl, with high mechanical properties. These hydrogels are formed by a dual network structure composed of polyacrylamide (PAM) and sodium carboxymethyl cellulose (CMC), with LiCl serving as the conductive material. At room temperature, the optimal Seebeck coefficient and ionic conductivity of the hydrogels can reach 2.96 mV K−1 and 36.51 mS cm−1, respectively. Based on the physical entanglement, hydrogen bonding, and chemical crosslinking of the polymer chains within the ionic hydrogels, which demonstrate outstanding mechanical properties (elongation at break >1300 %, fracture toughness >1700 kJ m−3), maintaining 95 % resilience under a large strain of 400 %. Furthermore, due to the hydration properties of LiCl, the ionic hydrogels exhibit excellent freeze resistance and the capability to absorb moisture for self-regeneration upon drying. Lastly, the fabricated ionic thermoelectric supercapacitor can generate a thermoelectric voltage of 0.182 V under a ΔT of 12 K, with a power density of 6.68 mW m−2, showing promising prospects for application in waste heat harvest fields.