Solid electrolytes are crucial for the development of solid state batteries. Among different types of solid electrolytes, poly(ethylene oxide) (PEO)-based polymer electrolytes have attracted extensive attention owing to their excellent flexibility and easiness for processing. However, their relatively low ionic conductivities and electrochemical instability above 4 V limit their applications in batteries with high energy density. Herein, we prepared poly(vinylidene fluoride) (PVDF) polymer electrolytes with an organic plasticizer, which possesses compatibility with 4 V cathode and high ionic conductivity (1.2 × 10 S/cm) at room temperature. We also revealed the importance of plasticizer content to the ionic conductivity. To address weak mechanical strength of the PVDF electrolyte with plasticizer, we introduced palygorskite ((Mg,Al)SiO(OH)) nanowires as a new ceramic filler to form composite solid electrolytes (CPE), which greatly enhances both stiffness and toughness of PVDF-based polymer electrolyte. With 5 wt % of palygorskite nanowires, not only does the elastic modulus of PVDF CPE increase from 9.0 to 96 MPa but also its yield stress is enhanced by 200%. Moreover, numerical modeling uncovers that the strong nanowire-polymer interaction and cross-linking network of nanowires are responsible for such significant enhancement in mechanically robustness. The addition of 5% palygorskite nanowires also enhances transference number of Li from 0.21 to 0.54 due to interaction between palygorskite and ClO ions. We further demonstrate full cells based on Li(NiMnCo)O (NMC111) cathode, PVDF/palygorskite CPE, and lithium anode, which can be cycled over 200 times at 0.3 C, with 97% capacity retention. Moreover, the PVDF matrix is much less flammable than PEO electrolytes. Our work illustrates that the PVDF/palygorskite CPE is a promising electrolyte for solid state batteries.

Continuously spinnable conductive silk fibers (CSFs) were constructed by a facile dip-coating strategy. The resultant CSFs integrate the mechanical and functional merits of both silk and carbon nanotubes and can be directly woven into smart textiles using automated equipment. These CSF-based e-textiles show promising applications in wearable devices, human augmentation, healthcare monitoring, and human-machine interfaces.

Solid-state lithium metal batteries with solid electrolytes are promising for next-generation energy-storage devices. However, it remains challenging to develop solid electrolytes that are both mechanically robust and strong against external mechanical load, due to the brittleness of ceramic electrolytes and the softness of polymer electrolytes. Herein, we propose a nacre-inspired design of ceramic/polymer solid composite electrolytes with the "brick-and-mortar" microstructure. The nacre-like ceramic/polymer electrolyte (NCPE) simultaneously possesses a much higher fracture strain (1.1%) than pure ceramic electrolytes (0.13%) and a much larger ultimate flexural strength (7.8 GPa) than pure polymer electrolytes (20 MPa). The electrochemical performance of NCPE is also much better than pure ceramic or polymer electrolytes, especially under mechanical load. A 5 × 5 cm 2 pouch cell with LAGP/poly(ether−acrylate) (PEA) NCPE exhibits stable cycling with a capacity retention of 95.6% over 100 cycles at room temperature, even undergoes a large This article is protected by copyright. All rights reserved. point load of 10 N. In contrast, cells based on pure ceramic and pure polymer electrolyte show poor cycle life. The NCPE provides a new design for solid composite electrolyte and opens up new possibilities for future solid-state lithium metal batteries and structural energy storage. The rapid-growing demands for portable electronics and electric vehicles have bolstered needs for next-generation lithium batteries with high energy density [1-4]. However, lithium batteries become more thermally vulnerable as energy density increases. Thermal runaway and explosion are prone to be triggered by failures such as mechanical damage and lithium dendrite growth inside batteries [5, 6]. Nonflammable solid-state ceramic electrolytes (SSEs) provide alternatives to conventional flammable liquid electrolytes [7-9]. Various ceramic electrolytes with attractive ionic conductivities have been developed in the past two decades, including NASICON-type Li 1.5 Al 0.5 Ge 1.5 (PO 4) 3 (LAGP) [10] , Li 1.3 Al 0.3 Ti 1.7 (PO 4) 3 (LATP) [11, 12] , garnet Li 7 La 3 Zr 2 O 12 (LLZO) [13, 14] , and sulfides, such as This article is protected by copyright. All rights reserved. NCPEs, polymer electrolytes and ceramic electrolytes were cut with a thickness of 500 μm and a size of 1.5 cm. A loading rate of 0.5 mm min-1 and a support span of 1.5 cm were used in all tests. The results were averaged from those in five similar specimens. The flexural stress is and The flexural strain is , where F, L, w, h, and D are the applied point force, span length, sample width, thickness, and flexural deflection, respectively. Vickers indentation was carried out on SANS-UTM 6000 using a Vickers indenter. Finite Element Mechanical Simulation: 2D nonlinear finite element simulations were conducted using the software ABAQUS v6.14. In these simulations, the stress/strain distributions and crack propagation in a regular brick-mortar structure and a ceramic film are calculate...

Internet of things (IoT) is expected to significantly improve every aspect of society, especially in soft robotics, structural health monitoring, and human motion detection. Flexible strain sensors with high‐performance characteristics as well as highly efficient and cost‐effective maskless fabrication methods are the key components of IoT for these applications. Herein, a 3D printing technology using digital light processing is developed to fabricate high‐performance flexible strain sensors based on UV‐curable multiwalled carbon nanotubes/elastomer (MWCNT/EA) composite. The MWCNT/EA‐based device with 2 wt% MWCNTs delivers a sensitivity of 8.939 with a linearity up to 45% strain. Additionally, the sensor has a detectable strain range from 0.01% to 60%, a high mechanical durability (10 000 cycles), and linear responses to humidity and temperature. Numerical simulation and impedance study indicate that the sensor works on the deformation‐induced reduction of MWCNT conductive pathway. The developed device can be used to detect various external deformation, when combined with a near‐field communication circuit. Moreover, a 4 × 4 strain sensor array is developed for sensing external stimuli distribution, further demonstrating the high performance of the 3D printed device.

The lithium–sulfur battery is an attractive option for next‐generation energy storage owing to its much higher theoretical energy density than state‐of‐the‐art lithium‐ion batteries. However, the massive volume changes of the sulfur cathode and the uncontrollable deposition of Li2S2/Li2S significantly deteriorate cycling life and increase voltage polarization. To address these challenges, we develop an ϵ‐caprolactam/acetamide based eutectic‐solvent electrolyte, which can dissolve all lithium polysulfides and lithium sulfide (Li2S8–Li2S). With this new electrolyte, high specific capacity (1360 mAh g−1) and reasonable cycling stability are achieved. Moreover, in contrast to conventional ether electrolyte with a low flash point (ca. 2 °C), such low‐cost eutectic‐solvent‐based electrolyte is difficult to ignite, and thus can dramatically enhance battery safety. This research provides a new approach to improving lithium–sulfur batteries in aspects of both safety and performance.

To achieve a high sulfur loading is critical for high-energy lithium-sulfur batteries. However, high sulfur loading, especially at a low electrolyte/sulfur ratio (E/S), usually causes low sulfur utilization, mainly caused by the slow redox kinetics of polysulfides and the passivation of the discharge product, poor electrically/ionically conducting Li 2 S. Herein, by using cobalt-based metal organic frameworks (Co-MOFs) as precursors, a Co, N-doped carbonaceous composite (Co, N-CNTs (carbon nanotubes)-CNS (carbon nanosheet)/CFC (carbon fiber cloth)) is fabricated with hierarchically ordered structure, which consists of a free-standing 3D carbon fiber skeleton decorated with a vertical 2D carbon nanosheets array rooted by interwoven 1D CNTs. As an effective polysulfides host, the hierarchically ordered 3D conductive network with abundant active sites and voids can effectively trap polysulfides and provide fast electron/ions pathways to convert them. In addition, Co and N heteroatoms can strengthen the interaction with polysulfides and accelerate its reaction kinetics. More importantly, the interwoven CNTs with Co, N-doping can induce 3D Li 2 S deposition instead of conventional 2D deposition, which benefits improving sulfur utilization. Therefore, for Co, N-CNTs-CNS/CFC electrodes, even at a high sulfur loading of 10.20 mg cm −2 with a low E/S of 6.94, a high reversible areal capacity of 7.42 mAh cm −2 can be achieved with excellent cycling stability.

Instant interfacial self-assembly of nanoparticle monolayer advances the thin film technology in a “lift-on” and conformal manner.

Despite their high theoretical capacity density (1675 mAh g–1), the application of Li–S batteries has been seriously hindered by the shuttle effect of polysulfides. Here, inspired by the working principle of natural spider webs, we synthesized a spider-web-like nanocomposite in which many hollow mesoporous silica (mSiO2) nanospheres/Co nanoparticles were threaded by interconnected nitrogen-doped carbon nanotubes (NCNTs). Then the nanocomposite (denoted as Co/mSiO2–NCNTs) was coated on the commercial separator by a simple infiltration to mitigate the above issue. The intimate combination of three-dimensional conductive networks (NCNTs) with abundant polysulfide adsorbent sites (SiO2 and N)/polysulfide conversion catalysts (Co and Co–N x species) allows the Co/mSiO2–NCNTs coating layer to not only effectively capture polysulfides via both physical confinement and chemical bonding but also accelerate the redox kinetics of polysulfides significantly. Furthermore, the combination of ex situ experiment and theoretical calculation demonstrates that the reversible adsorption/desorption of polysulfides on mSiO2 nanospheres benefits uniform deposition of Li2S2/Li2S on the conductive networks, which contributes to long-term cycling stability. As a result, Li–S batteries with Co/mSiO2–NCNTs-coated separators exhibited both excellent cycling stability and rate performance.