MXene, as a new member of the two‐dimensional (2D) material family, has been widely studied. However, people often pay close attention to the versatility of MXene while ignoring its low exfoliation yield. In this work, a simplified and effective strategy to exfoliate multilayer‐MXene via the gentle water freezing‐and‐thawing (FAT) approach is proposed. The volume expansion of intercalated water can promote the exfoliation of MXene nanosheets. The yield of large FAT‐MXene flakes with special wrinkles can reach 39% after four cycles of the FAT process. Moreover, combining with sonication treatment can boost the yield of small MXene to a record high value of 81.4%. With the help of a commercial interdigital mask, an on‐chip all‐MXene micro‐supercapacitor (MSC) assembled by large FAT‐MXene is fabricated, exhibiting high areal and volumetric capacitance of 23.6 mF cm−2 and 591 F cm−3, respectively. This remarkable electrochemical performance of MXene‐MSC also confirms the high quality of MXene through this FAT strategy. This study may open up a new method to simultaneously boost the yield of MXene with small or large flake sizes, facilitating large‐scale and size‐dependent research on MXene.

MXenes as an emerging two-dimensional (2D) material have attracted tremendous interest in electrochemical energy-storage systems such as supercapacitors. Nevertheless, 2D MXene flakes intrinsically tend to lie flat on the substrate when self-assembling as electrodes, leading to the highly tortuous ion pathways orthogonal to the current collector and hindering ion accessibility. Herein, a facile strategy toward multi-scale structural engineering is proposed to fabricate high-performance MXene hydrogel supercapacitor electrodes. By unidirectional freezing of the MXene slurry followed by a designed thawing process in the sulfuric acid electrolyte, the hydrogel electrode is endowed with a three-dimensional (3D) open macrostructure impregnated with sufficient electrolyte and H + -intercalated microstructure, which provide abundant active sites for ion storage. Meanwhile, the ordered channels bring through-electrode ion and electron transportation pathways that facilitate electrolyte infiltration and mass exchange between electrolyte and electrode. Furthermore, this strategy can also be extended to the fabrication of a 3D-printed all-MXene micro-supercapacitor (MSC), delivering an ultrahigh areal capacitance of 2.0 F cm -2 at 1.2 mA cm -2 and retaining 1.2 F cm -2 at 60 mA cm -2 together with record-high energy density (0.1 mWh cm -2 at 0.38 mW cm -2 ).

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A small amount of MXene to boost the thermal conductivity of boron nitride papers due to the well-designed interface.

Layered MXene films have shown enormous potential for wide applications due to their high electrical conductivity and unique laminated microstructure. However, the intrinsic susceptibility to oxidation and the mechanical fragility of MXene films are the two major bottlenecks that prevent their widespread industrial applications. Here, a facile yet efficient assembly strategy is proposed to address these issues by increasing the alignment and compactness of MXene layers as well as strengthening the interlayer interactions. This method involves the gelation of MXene flakes with a multifunctional inorganic “mortar” polymer (ammonium polyphosphate, APP) followed by quasi‐solid‐state assembly enabled by a mechanical rolling process, by which the 3D gel network is transformed into 2D freestanding MXene films with unprecedented flake alignment and compactness. Besides, due to the multiple molecular‐level interactions (hydrogen bonding, coordination bonding, and electrostatic force) between APP and MXene flakes, the resultant MXene‐APP film (MAF) displays high mechanical strength (286.4 ± 20.3 MPa) and excellent electrical conductivity (8012.4 ± 325.6 S cm−1), along with remarkable environmental stability. As an application demonstration, MAF exhibits outstanding electromagnetic interference shielding effectiveness with long‐term durability, highlighting the great potential of this gelation‐assisted assembly strategy in fabricating large‐area, high‐performance MXene films for diverse real‐world applications.

Booming sophisticated robotics and prosthetics put forward high requirements on soft conductive materials that can bridge electronics and biology, those soft conductive materials should imitate the mechanical properties of biological tissues and build information transmission networks. Until now, it remains a great challenge to handle the trade‐off among ease of preparation, high conductivity, processability, mechanical adaptability, and external stimuli responsiveness. Herein, a kind of readily prepared and processed multifunctional MXene nanocomposite hydrogel is reported, which is prepared via the fast gelation of cationic monomer initiated by delaminated MXene sheets. The gelation time can be adjusted (several seconds to minutes) based on the MXene loadings. By adjusting the MXene ratio, the resulting nanocomposites are ultrastretchable (>5000%), three‐dimensional (3D) printable, and show outstanding mechanical and electrical self‐healing. As expected, the integration of multifunctional systems onto various substrates (e.g., gloves and masks) is further demonstrated via 3D printing and could achieve diverse sensory capabilities toward strain, pressure, and temperature, showing great prospects as smart flexible electronics.

Electromagnetic Interference Shielding In article number 2200829, Dong Yang and co‐workers develop a gelation‐assisted assembly strategy to produce large‐area, environmentally‐stable MXene films with excellent trade‐off between mechanical and electrical performances, which endow resultant MXene films with outstanding electromagnetic interference shielding effectiveness with long‐term durability.

The lifespan of proton‐exchange membrane fuel cells heavily relies on the durability of the carbon support of cathode catalysts. However, commercial carbon supports like ketjenblack (KB) and Vulcan carbon (VC) face the challenge of balancing porosity, surface area, and electrochemical stability. To address this issue, a 3D porous wrinkled graphitic carbon (PWGC) is designed and synthesized using a catalyst‐free, plasma‐enhanced chemical vapor deposition approach. The resulting PWGC possesses a hierarchically porous structure with a high surface area, a high degree of graphitization, and exceptional corrosion resistance. As a result, the Pt/PWGC catalysts with the use of PWGC as the carbon support demonstrate superior high potential stability compared to those made with KB and VC as the carbon support. Additionally, a sacrificial layer strategy is introduced to further reduce PWGC corrosion, resulting in Pt@C/PWGC catalysts that show significantly improved durability in membrane electrode assembly tests. After 5K voltage cycles from 1.0 to 1.5 V, the retention of electrochemically active surface area approaches 56.8%, surpassing the 23.6% retention of commercial Pt/C catalysts tested under the same conditions.