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Artificial intelligence (AI) is accelerating the development of unconventional computing paradigms inspired by the abilities and energy efficiency of the brain. The human brain excels especially in computationally intensive cognitive tasks, such as pattern recognition and classification. A long-term goal is de-centralized neuromorphic computing, relying on a network of distributed cores to mimic the massive parallelism of the brain, thus rigorously following a nature-inspired approach for information processing. Through the gradual transformation of interconnected computing blocks into continuous computing tissue, the development of advanced forms of matter exhibiting basic features of intelligence can be envisioned, able to learn and process information in a delocalized manner. Such intelligent matter would interact with the environment by receiving and responding to external stimuli, while internally adapting its structure to enable the distribution and storage (as memory) of information. We review progress towards implementations of intelligent matter using molecular systems, soft materials or solid-state materials, with respect to applications in soft robotics, the development of adaptive artificial skins and distributed neuromorphic computing. Inanimate matter is beginning to show some signs of basic intelligence—the ability to sense, actuate and use memory, as controlled by an internal communication network in functional materials.

In principle, porous physisorbents are attractive candidates for the removal of volatile organic compounds such as benzene by virtue of their low energy for the capture and release of this pollutant. Unfortunately, many physisorbents exhibit weak sorbate–sorbent interactions, resulting in poor selectivity and low uptake when volatile organic compounds are present at trace concentrations. Herein, we report that a family of double-walled metal–dipyrazolate frameworks, BUT-53 to BUT-58, exhibit benzene uptakes at 298 K of 2.47–3.28 mmol g −1 at <10 Pa. Breakthrough experiments revealed that BUT-55, a supramolecular isomer of the metal–organic framework Co(BDP) (H 2 BDP = 1,4-di(1 H -pyrazol-4-yl)benzene), captures trace levels of benzene, producing an air stream with benzene content below acceptable limits. Furthermore, BUT-55 can be regenerated with mild heating. Insight into the performance of BUT-55 comes from the crystal structure of the benzene-loaded phase (C 6 H 6 @BUT-55) and density functional theory calculations, which reveal that C–H···X interactions drive the tight binding of benzene. Our results demonstrate that BUT-55 is a recyclable physisorbent that exhibits high affinity and adsorption capacity towards benzene, making it a candidate for environmental remediation of benzene-contaminated gas mixtures. Volatile organic compounds such as benzene are toxic pollutants that cause health issues even at trace concentrations. Here, a double-walled metal–organic framework is presented that demonstrates high uptake at very low pressures (<10 Pa), allowing the removal of benzene to below acceptable indoor limits.

Artificial muscles are indispensable components for next-generation robotics capable of mimicking sophisticated movements of living systems. However, an optimal combination of actuation parameters, including strain, stress, energy density and high mechanical strength, is required for their practical applications. Here we report mammalian-skeletal-muscle-inspired single fibres and bundles with large and strong contractive actuation. The use of exfoliated graphene fillers within a uniaxial liquid crystalline matrix enables photothermal actuation with large work capacity and rapid response. Moreover, the reversible percolation of graphene fillers induced by the thermodynamic conformational transition of mesoscale structures can be in situ monitored by electrical switching. Such a dynamic percolation behaviour effectively strengthens the mechanical properties of the actuator fibres, particularly in the contracted actuation state, enabling mammalian-muscle-like reliable reversible actuation. Taking advantage of a mechanically compliant fibre structure, smart actuators are readily integrated into strong bundles as well as high-power soft robotics with light-driven remote control.The reversible percolation of a graphene filler network in a liquid crystalline elastomer matrix enables the realization of mammalian-muscle-like actuation.

Covalent organic frameworks (COFs) have emerged as a kind of crystalline polymeric materials with high compositional and geometric tunability. Most COFs are currently designed and synthesized as mesoporous (2–50 nm) and microporous (1–2 nm) materials, while the development of ultramicroporous (<1 nm) COFs remains a daunting challenge. Here, we develop a pore partition strategy into COF chemistry, which allows for the segmentation of a mesopore into multiple uniform ultramicroporous domains. The pore partition is implemented by inserting an additional rigid building block with suitable symmetries and dimensions into a prebuilt parent framework, leading to the partitioning of one mesopore into six ultramicropores. The resulting framework features a wedge-shaped pore with a diameter down to 6.5 Å, which constitutes the smallest pore among COFs. The wedgy and ultramicroporous one-dimensional channels enable the COF to be highly efficient for the separation of five hexane isomers based on the sieving effect. The obtained average research octane number (RON) values of those isomer blends reach up to 99, which is among the highest records for zeolites and other porous materials. Therefore, this strategy constitutes an important step in the pore functional exploitation of COFs to implement pre-designed compositions, components, and functions. The development of ultramicroporous covalent organic frameworks (COFs) remains a daunting challenge. Here, the authors report a pore partition strategy, which allows for the segmentation of mesopores of COFs into multiple uniform ultramicroporous domains.

The features of well-conjugated and planar aromatic structures make π-conjugated luminescent materials suffer from aggregation caused quenching (ACQ) effect when used in solid or aggregated states, which greatly impedes their applications in optoelectronic devices and biological applications. Herein, we reduce the ACQ effect by demonstrating a facile and low cost method to co-assemble polycyclic aromatic hydrocarbon (PAH) chromophores and octafluoronaphthalene together. Significantly, the solid photoluminescence quantum yield (PLQYs) for the as-resulted four micro/nanococrystals are enhanced by 254%, 235%, 474 and 582%, respectively. Protection from hydrophilic polymer chains (P123 (PEO 20 -PPO 70 -PEO 20 )) endows the cocrystals with superb dispersibility in water. More importantly, profiting from the above-mentioned highly improved properties, nano-cocrystals present good biocompatibility and considerable cell imaging performance. This research provides a simple method to enhance the emission, biocompatibility and cellular permeability of common chromophores, which may open more avenues for the applications of originally non- or poor fluorescent PAHs. Organic luminescent materials are often used in modern technologies, but aggregation induced quenching caused by planar aromatic structures hampers their applicability. Here, the authors demonstrate a facile co-assembly method for luminescent cocrystals and protection with hydrophilic PEO chains which allow good dispersibility in water.

Bio-inspired self-healing materials hold great promise for applications in wearable electronics, artificial muscles and soft robots, etc. However, self-healing at subzero temperatures remains a great challenge because the reconstruction of interactions will experience resistance of the frozen segments. Here, we present an ultrarobust subzero healable glassy polymer by incorporating polyphenol nano-assemblies with a large number of end groups into polymerizable deep eutectic solvent elastomers. The combination of multiple dynamic bonds and rapid secondary relaxations with low activation energy barrier provides a promising method to overcome the limited self-healing ability of glassy polymers, which can rarely be achieved by conventional dynamic cross-linking. The resulted material exhibits remarkably improved adhesion force at low temperature (promotes 30 times), excellent mechanical properties (30.6 MPa) and desired subzero healing efficiencies (85.7% at −20 °C). We further demonstrated that the material also possesses reliable cryogenic strain-sensing and functional-healing ability. This work provides a viable approach to fabricate ultrarobust subzero healable glassy polymers that are applicable for winter sports wearable devices, subzero temperature-suitable robots and artificial muscles. Self-healing materials hold great promise for applications in wearable electronics, artificial muscles and soft robots but selfhealing at subzero temperatures remains a great challenge. Here, the authors present a robust subzero healable glassy polymer by incorporating polyphenol nano-assemblies with a large number of end groups into polymerizable deep eutectic solvent elastomers.

A dynamic surface pattern with a topography and fluorescence in response to environmental stimulus can enable information recording, hiding, and reading. Such patterns are therefore widely used in information security and anticounterfeiting. Here, we demonstrate a dynamic dual pattern using a supramolecular network comprising a copolymer containing pyridine (P4VP-nBA-S) and hydroxyl distyrylpyridine (DSP-OH) as the skin layer for bilayer wrinkling systems, in which both the wrinkle morphology and fluorescence color can be simultaneously regulated by visible light-triggered isomerization of DSP-OH, or acids. Acid-induced protonation of pyridines can dynamically regulate the cross-linking of the skin layer through hydrogen bonding, and the fluorescence of DSP-OH. On selective irradiation with 450 nm visible light or acid treatment, the resulting hierarchical patterned surface becomes smooth and wrinkled reversibly, and simultaneously its fluorescence changes dynamically from blue to orange-red. The smart surfaces with dynamic hierarchical wrinkles and fluorescence can find potential application in anticounterfeiting. Dynamic surface patterns are widely used in information security and anticounterfeiting technologies. Here, the authors demonstrated a dynamic wrinkled and fluorescent pattern using a supramolecular network in which both the wrinkle morphology and fluorescence color can be regulated by pH or light.

We report Layer-by-Layer (LbL) self-assembly of pillared two-dimensional (2D) multilayers, from water, onto a wide range of substrates. This LbL method uses a small molecule, tris(2-aminoethyl) amine (TAEA), and a colloidal dispersion of Ti 3 C 2 T x MXene to LbL self-assemble (MXene/TAEA) n multilayers, where n denotes the number of bilayers. Assembly with TAEA results in highly ordered (MXene/TAEA) n multilayers where the TAEA expands the interlayer spacing of MXene flakes by only ~ 1 Å and reinforces the interconnection between them. The TAEA-pillared MXene multilayers show the highest electronic conductivity of 7.3 × 10 4  S m −1 compared with all reported MXene multilayers fabricated by LbL technique. The (MXene/TAEA) n multilayers could be used as electrodes for flexible all-solid-state supercapacitors delivering a high volumetric capacitance of 583 F cm −3 and high energy and power densities of 3.0 Wh L −1 and 4400 W L −1 , respectively. This strategy enables large-scale fabrication of highly conductive pillared MXene multilayers, and potentially fabrication of other 2D heterostructures. Layer-by-layer self-assembly method using small molecules holds promise to precisely combine atomically thin materials and enable fabrication of pillared structures with superior device performance. Here, the authors report controlled synthesis of supercapacitor electrodes based on 2D Ti 3 C 2 T x MXene multilayers with a volumetric capacitance of 583 F/cm3.

Endosomal escape remains a fundamental barrier hindering the advancement of nucleic acid therapeutics. Taking inspiration from natural phospholipids that comprise biological membranes, we report the combinatorial synthesis of multi-tailed ionizable phospholipids (iPhos) capable of delivering messenger RNA or mRNA/single-guide RNA for gene editing in vivo. Optimized iPhos lipids are composed of one pH-switchable zwitterion and three hydrophobic tails, which adopt a cone shape in endosomal acidic environments to facilitate membrane hexagonal transformation and subsequent cargo release from endosomes. Structure–activity relationships reveal that iPhos chemical structure can control in vivo efficacy and organ selectivity. iPhos lipids synergistically function with various helper lipids to formulate multi-component lipid nanoparticles (called iPLNPs) for selective organ targeting. Zwitterionic, ionizable cationic and permanently cationic helper lipids enable tissue-selective mRNA delivery and CRISPR–Cas9 gene editing in spleen, liver and lungs (respectively) following intravenous administration. This rational design of functional phospholipids demonstrates substantial value for gene editing research and therapeutic applications. Ionizable phospholipid nanoparticles have been designed to efficiently destabilize endosomal membranes and mediate organ-selective mRNA delivery and CRISPR–Cas9 gene editing.

A major challenge in cancer vaccine therapy is the efficient delivery of antigens and adjuvants to stimulate a controlled yet robust tumour-specific T-cell response. Here, we describe a structurally well defined DNA nanodevice vaccine generated by precisely assembling two types of molecular adjuvants and an antigen peptide within the inner cavity of a tubular DNA nanostructure that can be activated in the subcellular environment to trigger T-cell activation and cancer cytotoxicity. The integration of low pH-responsive DNA ‘locking strands’ outside the nanostructures enables the opening of the vaccine in lysosomes in antigen-presenting cells, exposing adjuvants and antigens to activate a strong immune response. The DNA nanodevice vaccine elicited a potent antigen-specific T-cell response, with subsequent tumour regression in mouse cancer models. Nanodevice vaccination generated long-term T-cell responses that potently protected the mice against tumour rechallenge. A DNA nanodevice vaccine has been developed and utilized to stimulate a tumour-specific cytotoxic T lymphocyte response in vivo, leading to the inhibition of tumour growth as well as prevention of metastasis.