Excellent Ionic Conductivity Research Articles

High-Strength and High-Temperature-Resistant Structural Battery Integrated Composites via Polymeric Bi-Continuous Electrolyte Engineering.

Structural battery integrated composites (SBICs) combining outstanding strength and heat resistance are highly desirable candidates for next generation high speed aircraft. Here, a novel high-temperature-resistant bi-continuous electrolyte based on phthalonitrile resin is presented, allowing the construction of SBICs capable of stable operation across a wide temperature range. Excellent mechanical strength and high ionic conductivity can coexist in a bi-continuous structure electrolyte (PL50) where the phthalonitrile resin serves as the matrix phase and the ionic liquid electrolyte serves as the conductive phase. Benefiting from the thermal stability of the phthalonitrile resin, SBICs assembled with a PL50 bi-continuous electrolyte deliver excellent mechanical performance even at temperatures exceeding 200°C, with a flexural strength of 299MPa and a flexural modulus of 31.8GPa. Additionally, with an increase in operating temperature, PL50@SBICs demonstrated enhanced rate performance while maintaining good cycling stability. The demonstration of resisting mechanical abuse at high temperatures and flame retardance further suggests the promise of SBICs with PL50 bi-continuous electrolytes operating under extreme conditions.

High Ion-Conductive Hydrogel: Soft, Elastic, with Wide Humidity Tolerance and Long-Term Stability.

Ion-conductive hydrogels have received great attention due to their significant potential in flexible electronics. However, achieving hydrogels that simultaneously possess high ionic conductivity and stability under varying humidity conditions remains a challenge, limiting their practical applications. Herein, we propose a thermally controlled chemical cross-linking strategy to prepare an elastic and conductive hydrogel (ECH) of poly(vinyl alcohol) (PVA) with high content of H2SO4. The covalent cross-links formed effectively tackle the instability issue in high humidity of physically cross-linked PVA/H2SO4 hydrogels with high ionic conductivity, which were previously developed via the polymer-in-salt strategy. We systematically investigated the reaction conditions and clarified the methods to optimize the hydroxyl dehydration of PVA, resulting in excellent mechanical properties and ion conductivity simultaneously. The ECH demonstrates impressive ionic conductivity (up to 392 ± 49 mS cm-1) and elasticity (over 80% resilience upon stretching and compression after being equilibrated at various humidity levels for 24 days). Thanks to the excellent water retention of the high H2SO4 content, the ECH maintains an ionic conductivity exceeding 210 mS cm-1 for over 420 days at 50% relative humidity (RH) and retains over 100 mS cm-1 even after 3 days under extremely dry conditions (7% RH). These remarkable properties make the ECH an ideal candidate for applications requiring reliable ionic conductivity in diverse environmental conditions. Additionally, we demonstrated that the ECH can function as a stretchable Joule heater with high conformability for heating up objects with curved surfaces. The heating rate could reach a fast rate of ∼12 °C s-1 even when a human-safe alternating current voltage is below 36 V, attributed to the high ionic conductivity. We believe that the high performance and ease of fabrication make our hydrogels a promising candidate for use as electrolytes in flexible energy storage devices, electrolyte gates in electrochemical transistors, and artificial skin, which often face long-term stability challenges under varying humidity conditions.

High-Conductivity and Ultrastretchable Self-Healing Hydrogels for Flexible Zinc-Ion Batteries.

Aqueous zinc-ion batteries are promising candidates for flexible energy storage devices due to their safety, economic efficiency, and environmental friendliness. However, the uncontrollable dendrite growth and side reactions at the zinc anode hinder their commercial application. Herein, we designed and synthesized a dual network self-healing hydrogel electrolyte with zwitterionic groups (PAM-PAAS-QCS), which can be used for the large deformations of flexible devices due to its excellent stretchability (ε = 5100%). The incorporation of zwitterionic groups into the PAM-PAAS-QCS hydrogel electrolyte endows it with high ionic conductivity (33.61 mS/cm), a wide electrochemical stability window, and the ability to suppress zinc dendrite formation and side reactions. Besides, the Zn//Zn symmetric cell with PAM-PAAS-QCS can stably plate and strip zinc for 1500 h at 0.5 mA/cm2, and the Zn//Polyaniline full cell retains 82.4% of its capacity after 1500 cycles at 1 A/g. Additionally, flexible batteries based on both the original and self-healed PAM-PAAS-QCS hydrogel electrolytes demonstrate good cycling stability and stable charge-discharge performance under various bending conditions. This self-healing hydrogel electrolyte with excellent stretchability and high ionic conductivity is expected to pave the way for the development of high-performance flexible energy storage and wearable devices.

Janus-Architectured Lithium Replenishment Separators Boosting Longevity of Anode-Free Lithium Metal Batteries.

Addressing the issue of inactive dead lithium deposition on the anode side remains a significant challenge for anode-free lithium metal batteries. While lithium compensation techniques can mitigate lithium depletion, directly introducing lithium compounds into the cathode material may degrade the electrode structure. Here the design and fabrication of a novel lithium replenishment separator (LRS) using a lithium compensation agent of Li2C4O4 is reported. The electrospun LRS demonstrates excellent ionic conductivity of 1.82 mS cm-1 and a high Li+ transference number of 0.51. Such a functionalized LRS not only provides additional active lithium for anode-free lithium metal batteries but also promotes uniform deposition of lithium metal. Compared with conventional polyolefin-based separators, the LRS effectively boosts LiFePO4||Cu anode-free batteries with enhanced cyclability. These results suggest this LRS strategy can find promising applications in next-generation anode-free batteries with high energy densities.

Bis-cationic crosslinked anion exchange membranes based on carbazole-containing polyaromatics with excellent ionic conductivity for alkaline water electrolysis

As the core component in anion exchange membrane water electrolyser (AEMWE), anion exchange membrane (AEM) directly determines the electrolysis performance and long-term durability of AEMWE. Herein, we synthesized novel poly(carbazole-p-terphenylpiperidine) (PCTP-x) copolymers and then prepared a series of bis-cationic cross-linked AEMs (QPCTP-x-bpip) using the Menshutkin reaction between the cross-linker 4,4′-trimethylenebis(1-methylpiperidine) and the alkyl bromide on the polymer side chains. For comparison, non-crosslinked AEMs containing alkylpiperidinium side chains (QPCTP-x-pip) were prepared via a grafting reaction of alkyl bromide with 1-methylpiperidine. The bis-cationic crosslinked membrane exhibited high hydroxide conductivity of 190.0 mS cm−1, and demonstrated outstanding alkaline stability in a 1 M KOH solution at 80 °C, retaining more than 90 % of the initial hydroxide conductivity and tensile strength after 2200 h alkaline treatment. Meanwhile, the flexural carbazole backbone enhanced polymer solubility, enabling the utilization of QPCTP-20-pip as an anion exchange ionomer (AEI) in AEMWE. For the water electrolysis testing, AEMWE employing QPCTP-20-bpip as the AEM and QPCTP-20-pip as the AEI exhibited excellent performance, achieving a current density of 2910 mA cm−2 at 2.0 V using a 1 M KOH feed at 80℃. Moreover, the voltage increase during the in-situ durability test over 200 h was a mere 0.65 mV/h, demonstrating its promising potential for AEMWE applications.

Long‐lifespan 522 Wh kg‐1 Lithium Metal Pouch Cell Enabled by Compound Additives Engineering

Matching high‐voltage cathodes with lithium metal anodes represents the most viable technological approach for developing secondary batteries with ultra‐high energy density exceeding 500 Wh kg‐1. Nevertheless, the instability of electrolyte/electrode interface film and commercial electrolytes with cut‐off voltage above 4.3 V is still a major concern. Herein, we present that excellent cycling stability with an ultra‐high cut‐off voltage of up to 5.0 V can be obtained by using three‐component additives containing fluoroethylene carbonate (FEC), hexadecyl trimethylammonium chloride (CTAC), and tri(pentafluorophenyl)borane (TPFPB). Excellent ionic conductivity, robust interfacial films on both electrodes, and long‐lasting uniform Li+ regulation ability can be obtained in the modifying electrolyte. Consequently, using a high plating/stripping capacity of 3 mAh cm‐2 under the current density of 1 mA cm‐2, lithium symmetric cells demonstrate stable cycling performance exceeding 800 hours. Meanwhile, the 7.3 Ah‐class Li[NixCoyMn1‐x‐y]O2 (x=0.83, NCM83)| Li pouch cells are assembled, which show a high energy density of 522 Wh kg‐1 and present excellent stability over 178 cycles with a high initial coulombic efficiency (CE) of 98.0%.

Long-lifespan 522 Wh kg-1 Lithium Metal Pouch Cell Enabled by Compound Additives Engineering.

Matching high-voltage cathodes with lithium metal anodes represents the most viable technological approach for developing secondary batteries with ultra-high energy density exceeding 500 Wh kg-1. Nevertheless, the instability of electrolyte/electrode interface film and commercial electrolytes with cut-off voltage above 4.3 V is still a major concern. Herein, we present that excellent cycling stability with an ultra-high cut-off voltage of up to 5.0 V can be obtained by using three-component additives containing fluoroethylene carbonate (FEC), hexadecyl trimethylammonium chloride (CTAC), and tri(pentafluorophenyl)borane (TPFPB). Excellent ionic conductivity, robust interfacial films on both electrodes, and long-lasting uniform Li+ regulation ability can be obtained in the modifying electrolyte. Consequently, using a high plating/stripping capacity of 3 mAh cm-2 under the current density of 1 mA cm-2, lithium symmetric cells demonstrate stable cycling performance exceeding 800 hours. Meanwhile, the 7.3 Ah-class Li[NixCoyMn1-x-y]O2 (x=0.83, NCM83)| Li pouch cells are assembled, which show a high energy density of 522 Wh kg-1 and present excellent stability over 178 cycles with a high initial coulombic efficiency (CE) of 98.0%.

A Multifunctional NaxBi/NaCl Flexible Interface Layer for Solid‐State Na Metal Batteries

AbstractNa3Zr2Si2PO12 (NZSP) electrolyte with excellent air stability and acceptable ionic conductivity demonstrates a significant potential for application in solid‐state Na metal batteries. However, the poor interfacial contact between NZSP and Na anode has severely hindered its practical application. Herein, a BiCl3/polytetrafluoroethylene flexible interface layer is constructed between NZSP and Na metal anode. BiCl3 can react with Na metal to form a multifunctional NaxBi/NaCl‐rich flexible interface layer during the cycling process, which can effectively enhance the interfacial contact, avoid the formation of voids and reduce the interfacial resistance. NaxBi with low energy barrier can provide fast Na+ diffusion path, and NaCl with a wide band gap can inhibit electron injection and suppress Na dendrite growth. Owing to the multifunctional NaxBi/NaCl flexible interface layer, the Na/BiCl3@NZSP/Na symmetric cell exhibits a reduced interfacial resistance from 1252.1 to 67.6 Ω and achieves a high critical current density of 2 mA cm⁻2 at 25 °C. At 0.1 mA cm⁻2/0.1 mAh cm⁻2 and 0.3 mA cm⁻2/0.3 mAh cm⁻2, the symmetric cell can stably cycle for 3000 and 1100 h. Additionally, the Na3V2(PO4)3/BiCl3@NZSP/Na full cell can retain 96.7% of initial capacity (≈111 mAh g−1) after 300 cycles at 0.5 C and excellent rate capability.

Flexible high electrochemical collagen/lignin composite hydrogel for sensing and supercapacitor applications

Synthesis of polymer-based highly conductive hydrogels from natural and renewable sources with robust mechanical performances in flexible electronics remains a great challenge. In this research, a dynamic redox system is designed by using collagen (CL), sulfonate lignin (SL), acrylic acid (AA), and Al3+ to synthesize CL/PAA/SL/Al hydrogels. The formation of effective complexes of Al3+ with the abundant functional groups of CL, SL and PAA, the prepared hydrogel delivers various specific properties, for example, excellent ionic conductivity (4.61 S·m−1), stretchability and antimicrobial performance. The CL/PAA/SL/Al hydrogel demonstrates good mechanical strength, while the maximum tensile strength of the hydrogels is ∼604 kPa at a stretching of 1254 %, and the maximum compressive strength is ∼0.45 MPa, with the maximum stretching of 59.6 %. The CL/PAA/SL/Al hydrogel acts as a flexible strain sensor with high sensitivity. Enough hydroxyl and carboxyl groups in the hydrogels are essential for delivering the maximum 191 mV of open circuit voltage (Voc) rendered during moisture spraying. The supercapacitor assembled from CL/PAA/SL/Al hydrogel manifests specific capacitance (Cs), maximum energy density (Ed) and power density (Pd) of 268.75 F·g−1, 23.89 Wh·kg−1 and 2.4 kW·kg−1, respectively. The supercapacitor can retain its capacitance of 95.8 % after 5000 consecutive charge-discharge cycles.

Design of super stretchability, rapid self-healing, and self-adhesion hydrogel based on starch for wearable strain sensors

Since hydrogels are conductive, easily engineered, and sufficiently flexible to imitate the mechanical properties of human skin, they are seen as potential options for wearable strain sensors. However, it is still a great challenge to prepare a hydrogel through simple and straightforward methods that integrate excellent stretchability, ionic conductivity, toughness, self-adhesion, and self-healing. Herein, an acrylamide/3-acrylamide phenylboronic acid cross-linked network is modified to produce a semi-interpenetrating cross-linked hydrogel in just one easy step by adding starch. The prepared hydrogel contains dynamic boronic ester bonds and hydrogen bonds, which endow the exceptional stretchability (5769–13,976 %, 20–50 wt%), ideal transmittance (>90 %), self-adhesiveness (0.636 ± 0.060 kPa, 30 wt%), and self-healing properties. Notably, the self-healing process is completed instantly, achieving a healing strength of up to 81.21 %. Additionally, the aforementioned hydrogel exhibits a broad working strain range (≈ 500 %) and high sensitivity (gauge factor = 1.99) as a strain sensor, allowing it to record and track human actions precisely. This work provides a novel approach to synthesizing hydrogels with optimal overall mechanical characteristics, with the potential to facilitate the development of wearable strain sensing system based on hydrogels for real-world applications.

Designing a Refined Multi-Structural Polymer Electrolyte Framework for Highly Stable Lithium-Metal Batteries.

Rational structural designs of solid polymer electrolytes featuring rich interface-phase morphologies can improve electrolyte connection and rapid ion transport. However, these rigid interfacial structures commonly result in diminished or entirely inert ionic conductivity within their bulk phase, compromising overall electrolyte performance. Herein, a multi-component ion-conductive electrolyte was successfully designed based on a refined multi-structural polymer electrolyte (RMSPE) framework with uniform Li+ solvation chemistry and rapid Li+ transporting kinetics. The RMSPEis constructed via polymerization-induced phase separation based on a rational combination of lithiophilic components and rigid/flexible chain units with significant hydrophobic/hydrophilic contrasts. Further refined by coating a robust polymer network, this all-organic design endows a homogenous micro-nano porous structure, providing a novel framework favorable for rapid ion transport in both its soft interfacial and bulk phases. The RMSPE exhibited excellent ion conductivity of 1.91 mS cm-1 at room temperature and a high Li+ transference number of 0.7. Assembled symmetrical Li cells realized stable cycling for over 2400 h at 3.0 mA cm-2. LiFePO4 full batteries demonstrated a long lifespan of 3300 cycles with a capacity retention of 93.5% and stable cycling performance at -35 °C. This innovative design concept offers a promising perspective for achieving high-performance polymer-based Li metal batteries.

Microstructural Tuning of High‐Performance Bacterial Cellulose Anion Exchange Membranes via Constrained In Situ Polymerization and Double Chemical Cross‐Linking

AbstractHigh electrochemical and durability anion exchange membranes (AEMs) are a vital material for Flexible zinc‐air batteries (F‐ZAB) and AEM water electrolysis (AEMWE) to achieve green economy and environmental protection. However, the existing AEMs possess the disadvantages of a complicated preparation process, poor homogeneity, and unsatisfactory electrochemical performance. Here, a novel alkaline exchange membrane is synthesized using bacterial cellulose (BC) as the matrix, incorporating constrained in situ Poly (diallyldimethylammonium chloride) (PDDA) polymerization and double chemical cross‐linking techniques. By adjusting the microstructure, a unique long‐range order and dense internal structure to address the issue of loose bonding between PDDA and BC is established and achieve the purpose of rapid OH− conduction. The membranes exhibit excellent application properties, with excellent ionic conductivity (145.12 mS cm−1) and superb mechanical strength (73.26 MPa). Consequently, the membrane is assembled into the F‐ZAB, and the unprecedented power density of 258.7 mW cm−2 can be achieved at room temperature. Moreover, the membrane also can reach 3.0 A cm−2 at 2.3 V, indicating good prospects in the field of water electrolysis in 6 m KOH. The approach paves a new path for manufacturing AEMs for green energy and environmental applications.

Hydrophilic and Insulative Interface Strategy Against Side Reactions for Dendrite‐Free Zinc Metal Anodes

AbstractThe zinc dendrite growth and the parasitic hydrogen evolution reactions (HER) hinder the commercialization of zinc batteries. To address this, a hydroxyl‐rich Boehmite coating (HR‐BC) strategy is developed that combines excellent electrical insulation and high zinc ion conductivity. The hydrophilic hydroxyl groups facilitate hydrogen bond formation with the hydrated zinc ions, accelerating the de‐solvation process and suppressing the HER. Additionally, the electrically insulative nature of Boehmite prevents the reduction of zinc ions within HR‐BC and results in preferential Zn deposition underneath it, leading to a dendrite‐free “sandwich structure” of HR‐BC//Zn deposition//Zn foil. Symmetric cells using HR‐BC‐Zn electrodes obtain an ultralong and stable cycling lifetime of 1700 h at 5 mA cm−2, along with a high cumulative plating capacity of 4250 mAh cm−2. When paired with a V2O5 cathode, the HR‐BC‐Zn anode demonstrates a high capacitance retention of 90% and an average Coulombic efficiency (CE) of 99.8% after 4000 cycles. Furthermore, when combined with a heteroatoms‐doped carbon (HDC) cathode, the HR–BC–Zn//HDC pouch‐type cell exhibits superior lifetime performance with nearly 100% average CE after 15000 cycles at 3.0 A g−1. This work highlights the effectiveness of hydrophilic and insulative coating strategies in fostering the progression of long‐lasting zinc‐based energy storage systems.

Coating Robust Layers on Ni-Rich Cathode Active Materials while Suppressing Cation Mixing for All-Solid-State Lithium-Ion Batteries.

This study focused on addressing the challenges associated with the incompatibility between sulfide solid electrolytes and Ni-rich cathode active materials (CAMs) in all-solid-state lithium-ion batteries. To resolve these issues, protective layers have been explored for Ni-rich materials. Lithium lanthanum titanate (LLTO), a perovskite-type material, is recognized for its excellent chemical stability and ionic conductivity, which render it a potential protective layer in CAMs. However, traditional methods of achieving the perovskite structure involve temperatures exceeding 700 °C, resulting in challenges such as LLTO agglomeration, secondary phase formation between LLTO and CAM, and cation mixing within the CAM. In this study, a rapid technique known as flash-light sintering (FLS) was employed to fabricate a uniform and pure perovskite protective layer without inducing cation mixing within the CAM. The LLTO-coated LiNi0.8Co0.1Mn0.1O2 (NCM811) with FLS treatment demonstrated minimal cation mixing and formed a fully covered dense layer. This resulted in a high initial capacity and effectively addressed the incompatibility issues between the sulfide electrolytes and CAM. The rapid FLS method not only streamlines the fabrication of LLTO-coated NCM811 but also provides opportunities for its broader application to materials that were previously deemed impractical because of high sintering temperatures.

Superionic halide solid electrolyte Li1.7Zr0.7Ta0.3Cl6 for durable all-solid-state lithium batteries

Zirconium-based halide solid electrolyte, Li2ZrCl6, with low raw-material cost and high oxidative stability is a promising candidate for next-generation energy storage devices. However, the low ionic conductivity hinders its practical applicability. Herein, we report a new zirconium-based superionic conductor based on high-valence Ta5+ doping strategy. The optimized Li1.7Zr0.7Ta0.3Cl6 (LZTC) exhibits excellent ionic conductivity of 1.42 mS cm-1 at 25 °C. Moreover, it can be further increased up to 1.68 mS cm-1 with a low activation energy of 0.28 eV by slightly tuning Li+ concentration. In addition, LZTC possesses a big compact density of 2.67 g cm-3 under 250 MPa and is compatible with 4V-class cathodes. Density function theory (DFT) and bond valence site energy (BVSE) calculations reveal Ta5+ substitution significantly reduces the migration energy barrier of lithium ions due to the distortions and defects of local structural environment. The assembled all-solid-state batteries with Li1.7Zr0.7Ta0.3Cl6 as electrolyte and scNCM811 as cathode show excellent cycling performance for 600 cycles at 1C with a high-capacity retention of 85.7%.

In Situ Polymerized Flame‐Retardant Crosslinked Quasi Solid‐State Electrolytes for High‐Voltage Lithium Metal Batteries

AbstractThe construction of poly‐dioxolane (PDOL) solid‐state electrolytes by in situ polymerization is an effective way to achieve high performance lithium‐metal batteries. However, the poor electrochemical stability and safety issues of linear PDOL limit their further application. In this work, a multifunctional crosslinker has been introduced to construct a flame retardant crosslinked quasi solid‐state electrolyte (FCDOL). Due to the synergistic effect of the crosslinked network, the prepared FCDOL achieves excellent room temperature ionic conductivity (0.72 mS cm−1), high Li+ transference number (0.655), wide electrochemical stabilization window (4.8 V vs Li/Li+), and impressive performance when matched with lithium metal anodes (>4000 h plating/stripping) and high‐voltage cathodes, and the corresponding pouch cells can withstand abusive tests such as bending and cutting, encouraging that in situ polymerization of SPEs provides new insights into high‐energy density and high‐safety solid‐state batteries.

Effect of Dispersion Media Composition on the Structure and Rheology of the Short-Sidechain Perfluorosulfonic Acid Ionomer Dispersions

Perflourosulfonic acid (PFSA) ionomers are used in many applications including polymer-electrolyte membrane fuel cells and electrolysers owing to their many attractive properties such as excellent ion-conductivity, chemical resistance, mechanical properties, and thermal stability. In polymer-electrolyte membrane fuel cells and electrolysers, they are used as the membrane and as a component in the catalyst layers, to provide proton conductivity and serve as a binder for the catalyst particles, which are two key components of these devices. Understanding the structure and rheological properties of the ionomer dispersions is important for solution-processed fabrication of the membranes and the catalyst layers, and will enable better control their final structure/morphology, and improve the device performance. A water-alcohol solvent mixture is a common dispersion media for ionomer dispersions as well as the catalyst inks. While significant efforts exist on the structure of ionomer dispersions in water-alcohol solvent mixtures, their rheological properties, particularly the effect of solvent composition at non-dilute concentrations remain less explored. In this talk, the effect of water-alcohol (isopropanol) composition of the dispersion media on the rheological properties of ionomer dispersions will be presented. The results of small-angle x-ray scattering characterization of the ionomer dispersions will be also discussed. As a model ionomer, a short sidechain perfluorinated ionomer (PFSA), produced by 3M, was used. In dispersions with low ionomer concentrations, the zero-shear viscosity scaling with concentration was found to be similar for all alcohol fractions in the solvent mixture, following Fuoss’s law for polyelectrolytes. Whereas at higher concentrations, beyond the semi-dilute unentangled regime, their scaling was strongly dependent on alcohol fraction, where the scaling exponent increasing with increasing the alcohol fraction. Furthermore, the dispersions showed dramatic shear-thickening and strain-stiffening behaviors at higher alcohol fractions. The rheological observations suggest water-alcohol composition significantly alters the interactions between ionomer, and consequently their structure, and has strong implications in processing as well as on the morphology/structure of the membranes and the catalyst layers.

A Stable Polymer-Blended Anion-Exchange Membrane for Enhanced Performance in Redox Flow Batteries

Redox flow batteries (RFBs) operate with a membrane, responsible for the separation of cationic active species and allowing the passage of counter-ions, to preserve electroneutrality on each side of RFBs. Commercial cation-exchange membranes (CEMs), such as Nafion®, possess excellent ionic conductivity and chemical stability. However, they face challenges in blocking cationic active species common in RFBs, leading to significant capacity loss over time. Anion-exchange membranes (AEMs) efficiently block active species with the assistance of the Donnan effect. Nevertheless, commercial AEMs lack acid stability and conductivity compared to their cationic counterparts.Polytetrafluoroethylene (PTFE)-reinforced quaternary ammonium cardo poly(ether)ketone (QPEK-C)-based membranes with Al2O3 additives (PQPAM), a heterogeneous AEM developed in our lab1, possess excellent ionic conductivity with low permeability of active species and good mechanical properties. PQPAM has demonstrated better acid stability than commercial AEMs. However, its acidic and oxidative stability require improvement, as evidenced by degradation after 250 hours of in-situ harsh RFB cycling due to the heterogeneous nature of PQPAM and the exposure of the susceptible QPEK-C-rich side to the electrolytes2. To address this issue, we propose a strategy to enhance the chemical stability of QPEK-C-based membranes by inhibiting the exposure of QPEK-C to oxidation agents through blending with a hydrophobic engineering thermoplastic like polybenzimidazole (PBI)3,4. Furthermore, PBI's known ability to protonate in acidic media will reinforce ionic conductivity and the separation of active species, thus improving the Donnan effect, in addition to enhancing chemical and mechanical stability.Elemental analyses and microscopy images confirm a homogeneous blending of PBI and QPEK-C, promising stability improvement. The results of ex-situ tests on ionic conductivity, cation permeability, and chemical stability align with the mentioned hypotheses, showcasing that blend of PBI/QPEK-C outperforms pure PBI and QPEK-C AEMs. Additionally, the mechanical properties of the PBI/QPEK-C blended AEMs are improved compared to pure QPEK-C AEMs and PBI/QPEK-C blended AEMs outperform pure PBI and QPEK-C AEMs in in-situ cycling tests with our patented titanium-cerium RFBs5. Moreover, this work will explore other strategies to improve the blended AEM properties, such as utilizing inorganic fillers or PTFE reinforcement.

Anti-freezing and conductive hydrogel with water-resistant properties for flexible underwater sensors

Flexible strain sensors based on hydrogels have numerous application prospects. However, the high water content and unsatisfactory water resistance of traditional hydrogel-based sensors limits its application in harsh environment, such as subzero environment and underwater environment. Herein, conductive poly(acrylamide-co-2-hydroxyethyl methacrylate) ionic glycerol-hydrogel was developed through the hydrophobic aggregation interaction and double cross-linking network. The resultant ionic glycerol-hydrogel exhibited excellent anti-freezing properties (-34 °C), water-resistant properties (swelling ratio less than 3 %), ionic conductivity (0.7 S m−1), and strain sensing capabilities (Gauge factor up 1.73). The flexible strain sensors based on ionic glycerol-hydrogel could detect electrical signals at subzero temperatures. Moreover, the hydrogel sensors achieved effective detection and discrimination of Morse codes to transmit underwater information. Demonstrated its potential application in wearable devices.

Highly conductive and stretchable nanostructured ionogels for 3D printing capacitive sensors with superior performance

Ionogels are promising material candidates for ionotronics due to their excellent ionic conductivity, stretchability, and thermal stability. However, it is challenging to develop 3D printable ionogels with both excellent electrical and mechanical properties. Here, we report a highly conductive and stretchable nanostructured (CSN) ionogel for 3D printing ionotronic sensors. We propose the photopolymerization-induced microphase separation strategy to prepare the CSN ionogels comprising continuous conducting nanochannels intertwined with cross-linked polymeric framework. The resultant CSN ionogels simultaneously achieves high ionic conductivity (over 3 S m−1), high stretchability (over 1500%), low degree of hysteresis (0.4% at 50% strain), wide-temperature-range thermostability (−72 to 250 °C). Moreover, its high compatible with DLP 3D printing enables the fabrication of complex ionogel micro-architectures with high resolution (up to 5 μm), which allows us to manufacture capacitive sensors with superior sensing performances. The proposed CSN ionogel paves an efficient way to manufacture the next-generation capacitive sensors with enhanced performance.