Skin-mountable microelectronics are garnering substantial interest for various promising applications including human-machine interfaces, biointegrated devices, and personalized medicine. However, it remains a critical challenge to develop e-skins to mimic the human somatosensory system in full working range. Here, we present a multifunctional e-skin system with a heterostructured configuration that couples vinyl-hybrid-silica nanoparticle (VSNP)–modified polyacrylamide (PAM) hydrogel with two-dimensional (2D) MXene through nano-bridging layers of polypyrrole nanowires (PpyNWs) at the interfaces, featuring high toughness and low hysteresis, in tandem with controlled crack generation and distribution. The multidimensional configurations endow the e-skin with an extraordinary working range (2800%), ultrafast responsiveness (90 ms) and resilience (240 ms), good linearity (800%), tunable sensing mechanisms, and excellent reproducibility. In parallel, this e-skin platform is capable of detecting, quantifying, and remotely monitoring stretching motions in multiple dimensions, tactile pressure, proximity sensing, and variations in temperature and light, establishing a promising platform for next-generation smart flexible electronics.

Polymerization of multifunctional monomers could produce polymers with different functionalities and novel macromolecular architectures. However, the ability to control the homopolymerization of multivinyl monomers (MVMs) has always been a challenge. Here we demonstrate that the homopolymerization of acrylate based MVMs can be kinetically controlled via Cu 0 -mediated controlled/living radical polymerization in the presence of additional Cu II , which enables the efficient promotion of intramolecular cyclization and suppression of intermolecular cross-linking. The gelation is effectively delayed over ca. 40% monomer conversion in the concentrated polymerization system ([M] = 40.9 wt %), which is far higher than the Flory−Stockmayer theory predicts. Moreover, closer inspection of the synthesized polymers reveals that single-chain cyclized/knotted polymeric nanoparticles (SCKNPs) are formed due to the nature of one-pot in situ intramolecular reaction and self-cyclization of the propagating polymer chains. This facile method opens a new avenue to the design and synthesis of a broad range of novel single-chain cyclized/knotted polymeric materials.

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Architected materials that actively respond to external stimuli hold tantalizing prospects for applications in energy storage, wearable electronics, and bioengineering. Molybdenum disulfide, an excellent two-dimensional building block, is a promising candidate for lithium-ion battery anode. However, the stacked and brittle two-dimensional layered structure limits its rate capability and electrochemical stability. Here we report the dewetting-induced manufacturing of two-dimensional molybdenum disulfide nanosheets into a three-dimensional foam with a structural hierarchy across seven orders of magnitude. Our molybdenum disulfide foam provides an interpenetrating network for efficient charge transport, rapid ion diffusion, and mechanically resilient and chemically stable support for electrochemical reactions. These features induce a pseudocapacitive energy storage mechanism involving molybdenum redox reactions, confirmed by in-situ X-ray absorption near edge structure. The extraordinary electrochemical performance of molybdenum disulfide foam outperforms most reported molybdenum disulfide-based Lithium-ion battery anodes and state-of-the-art materials. This work opens promising inroads for various applications where special properties arise from hierarchical architecture.

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