Stress controllability in thermal and electrical conductivity is important for flexible piezoresistive devices. Due to the strength‐elasticity trade‐off, comprehensive investigation of stress‐controllable conduction in elastic high‐modulus polymers is challenging. Here presented is a 3D elastic graphene‐crosslinked carbon nanotube sponge/polyimide (Gw‐CNT/PI) nanocomposite. Graphene welding at the junction enables both phonon and electron transfer as well as avoids interfacial slippage during cyclic compression. The uniform Gw‐CNT/PI comprising a high‐modulus PI deposited on a porous templated network combines stress‐controllable thermal/electrical conductivity and cyclic elastic deformation. The uniform composites show different variation trends controlled by the porosity due to different phonon and electron conduction mechanisms. A relatively high k (3.24 W m−1 K−1, 1620% higher than PI) and suitable compressibility (16.5% under 1 MPa compression) enables the application of the composite in flexible elastic thermal interface conductors, which is further analyzed by finite element simulations. The interconnected network favors a high stress‐sensitive electrical conductivity (sensitivity, 973% at 9.6% strain). Thus, the Gw‐CNT/PI composite can be an important candidate material for piezoresistive sensors upon porosity optimization based on stress‐controllable thermal or electrical conductivity. The results provide insights toward controlling the stress‐induced thermal/electrical conductivities of 3D interconnected templated composite networks for piezoresistive conductors or sensors.

Defects are deliberately introduced into covalent organic frameworks (COFs) via a three‐component condensation strategy. The defective COFs (dCOF‐NH2‐Xs, X = 20, 40, and 60) possess favorable crystallinity and porosity, as well as have active amine functional groups as anchoring sites for further postfunctionalization. By introducing imidazolium functional groups onto the pore walls of COFs via the Schiff‐base reaction, dCOF‐ImBr‐Xs‐ and dCOF‐ImTFSI‐Xs‐based materials are employed as all‐solid‐state electrolytes for lithium‐ion conduction with a wide range of working temperatures (from 303 to 423 K), and the ion conductivity of dCOF‐ImTFSI‐60‐based electrolyte reaches 7.05 × 10−3 S cm−1 at 423 K. As far as it is known, it is the highest value for all polymeric crystalline porous material based all‐solid‐state electrolytes. Furthermore, Li/dCOF‐ImTFSI‐60@Li/LiFePO4 all‐solid Li‐ion battery displays satisfactory battery performance under 353 K. This work not only provides a new methodology to construct COFs with precisely controlled defects for postfunctionalization, but also makes them promising candidate materials as all‐solid‐state electrolytes for lithium‐ion batteries operate at high temperatures.

The discovery of graphene and graphene-like two-dimensional materials has brought fresh vitality to the field of photocatalysis. Bandgap engineering has always been an effective way to make semiconductors more suitable for specific applications such as photocatalysis and optoelectronics. Achieving control over the bandgap helps to improve the light absorption capacity of the semiconductor materials, thereby improving the photocatalytic performance. This work reports two-dimensional −H/−OH terminal-substituted siligenes (gersiloxenes) with tunable bandgap. All gersiloxenes are direct-gap semiconductors and have wide range of light absorption and suitable band positions for light driven water reduction into H 2 , and CO 2 reduction to CO under mild conditions. The gersiloxene with the best performance can provide a maximum CO production of 6.91 mmol g −1 h −1 , and a high apparent quantum efficiency (AQE) of 5.95% at 420 nm. This work may open up new insights into the discovery, research and application of new two-dimensional materials in photocatalysis.

Large-area uniform of single-crystal tungsten disulfide (WS) is important for advanced optoelectronics based on two-dimensional (2D) atomic crystals. However, difficulties in controlling the interrelated growth parameters restrict its development in devices. Herein, we present the synthesis of triangular monolayered WS flakes with good uniformity and single crystal by adjusting the introduction time of sulfur precursor and the distances between the sources and substrates to control the nucleation density. Investigation of the morphology and structure by transmission electron microscopy and Raman spectroscopy indicates that a series of triangular (side length of 233 μm) monolayered WS flakes shows high-quality structure and homogenous crystallinity. Field-effect transistors based on the fabricated triangular monolayered WS with single crystal demonstrate environmentally stable charge transport with a field-effect mobility of 50.5 cm/V s and current modulation I/ I of ∼10. The results of this study pave the way for the application of monolayered WS in a multitude of 2D-material-based devices.

Lithium–sulfur (Li–S) batteries have great prospects as next‐generation energy storage devices because of their high energy density, inexpensive raw materials, and low pollution. However, the development of Li–S batteries is currently restricted by the shuttle effect that occurs during the charge–discharge process. Sulfur‐containing polymers are attractive for use as Li–S battery cathode materials to alleviate the shuttle effect through chemical bonds as well as physical confinement. Moreover, polymers have numerous different molecular structures and definable functional groups. A suitable monomer design can result in a final sulfur‐containing polymer possessing favorable properties such as ion and electron conductivity, high sulfur content, appropriate viscosity, processability, and controllable morphology. These characteristics are of great benefit for use in Li–S battery cathodes to achieve high capacity and stable discharge at high rates. This review summarizes recent developments in sulfur‐containing polymer cathode materials. Focusing on polymers prepared by the facile and low‐cost vulcanization/inverse vulcanization methods and the polymer‐based composites, the chemical structures and electrochemical mechanisms are clarified, and the relationship between their structures and performances is discussed comprehensively. It is expected that more polymer electrode materials with high performance will emerge in the coming years.