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2D polymer materials are often limited in performance by insufficient in-plane conjugation and poor charge transport. Guided by theoretical calculations, the authors present diketopyrrolopyrrole-based crystalline 2D poly(arylene vinylene)s with narrow optical band gaps of 1 eV and high charge carrier mobility.

Two-dimensional poly(arylene vinylene) frameworks are promising polymer semiconductors, yet obtaining highly crystalline materials is a major challenge. Now a series of 11 highly crystalline or single-crystalline 2D poly(arylene vinylene)s have been prepared—from 2D imine-linked covalent organic frameworks through a Mannich-elimination strategy—with diverse lattices, enhanced conjugation and specific surface areas up to 2,000 m² g⁻¹.

A gas–liquid–solid triphasic etching strategy is demonstrated to obtain MXenes with uniform and tunable halogen terminations. The resulting MXenes have highly ordered structures, enhanced charge transport properties and programmable surface chemistry for advanced (opto)electronic applications.

Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) are emerging candidates for organic 2D crystal materials, but the precise implantation of chirality has yet to be demonstrated. Here, the authors report a side chain-induced chirality amplification strategy to achieve tunable chiral expression in 2D c-MOFs.

Single-layer graphene, owing to its impermeability, is a promising candidate to prevent transmembrane ion transport. Here, the authors report a covalent functionalization method that enables centimeter-sized graphene to function as a proton exchange membrane in a direct methanol fuel cell.

Mechanically interlocked monolayer and bilayer two-dimensional polymers (2DPs) are synthesized on the water surface by embedding macrocyclic molecules with one and two cavities into the backbones. The resulting bilayer 2DP displays a high effective Young’s modulus, exceeding other reported multilayer 2DPs.

The authors report long-lived pump-induced conductivity suppression in metallic Ti₃C₂ MXenes using ultrafast terahertz and reflectance spectroscopy. The effect is attributed to strong photothermal heating and slow heat dissipation.

Micro-supercapacitors offer the advantage of high power density over lithium batteries and high energy density over electric capacitors, but integration of these advantages is yet to be achieved. Wu et al. develop a graphene-based in-plane micro-supercapacitor with ultrahigh power and energy densities.

The zigzag edges of graphene host edge-localized electronic states with aligned electron spins, but these states strongly interact with metallic substrates. Here, the authors measure the electronic structure of graphene nanoribbons after transferring them to an insulating support.

Graphene sheets used to build electronic devices have defects that limit performance. As a possible bottom-up route towards better devices, Diez-Perez and co-workers build large polyaromatic molecules with precisely defined structures which show good performance as field-effect transistors.

Chemical functionalization of graphene is a useful method for modulating its properties, although this is limited by a lack of control and resulting in poorly defined structures. Here the authors report the atomically precise chlorination of nanographenes and apply the methods to graphene nanoribbons.

The ability to control magnetic coupling in graphene nanomaterials remains elusive. Here, the authors report an approach of engineering magnetic ground states in open-shell bipartite/nonbipartite nanographenes where the magnetic coupling sign between two spins are controlled via breaking bipartite lattice symmetry.

The synthesis of crystalline 2D polymers typically relies on reversible dynamic covalent reactions, but achieving 2D polymers through irreversible carbon-carbon coupling reactions remains a formidable challenge. Here, the authors present an on-liquid surface synthesis method for constructing diyne-linked 2D polymers.

Graphene nanoribbons show promise for high-performance field-effect transistors, however they often suffer from short lengths and wide band gaps. Here, the authors use a bottom-up synthesis approach to fabricate 9- and 13-atom wide ribbons, enabling short-channel transistors with 10⁵ on-off current ratio.

Discotic liquid crystals are materials with high charge-carrier mobility, which are promising for molecular electronics. They self-organize into stacks, usually with a twist of 30^∘, but the shape and periphery of the molecules can now be altered to produce materials with a twist of 60^∘. Defect-limited mobilities of these materials reach 0.2 cm² V⁻¹ s⁻¹, but the potential defect-free mobility could be up to 10 cm² V⁻¹ s⁻¹.

Forming 2D polymers in a controlled manner on the atomic and molecular level is difficult. Here, Feng and others have used Schiff-base polycondensation reactions at an air-water or liquid-liquid interface to form porphyrin containing monolayer and multilayer 2D polymers.

Graphene-based photodetectors have many advantages for applications. Here, the authors demonstrate a high-speed optical coherent receiver for optical communications based on graphene-on-plasmonic slot waveguide photodetectors.

Based on Bader charge descriptors, a Cu2ZnSnS4 nanosheet with S defects is developed for photocatalytic CO2 reduction. Under visible light irradiation, C2H4 is produced from CO2 with a yield of 25.16 µmol g-1 h-1 with ~50% selectivity.

Achieving cathodes with large areal capacities is crucial for advancing aqueous aluminum-based batteries. Here, authors report a hydrate-melt electrolyte based on AlCl₃ and organic halide salts that enables reversible Br⁻ /Br⁰ /Br⁺ chemistry with a high areal capacity of 5 mAh cm⁻².

Effective electrocatalyst is crucial in promoting CO₂ reduction to address current energy/environmental issue. Here, the authors develop bimetallic layered two-dimensional conjugated metal-organic framework to synergistically and efficiently electro-catalyze CO₂ to CO toward syngas synthesis.

Developing chemistries for positive electrodes with large specific capacities and high operating potentials is highly desirable for aqueous zinc batteries. Here, authors report a reversible Se electrode that undergoes ZnSe↔Se↔SeCl₄ reaction, combined with Br⁻ /Br^{n –} redox couple as Se revitalizer to enhance cycling performance.

Hot carrier transport in organic systems has remained elusive due to rapid energy relaxation and limited transport properties. Here highly mobile hot carriers and their relaxation dynamics are reported in a crystalline two-dimensional conjugated coordination polymer, revealing two distinct transport regimes.

To mark the occasion of Nature Chemistry turning 10 years old, we asked scientists working in different areas of chemistry to tell us what they thought the most exciting, interesting or challenging aspects related to the development of their main field of research will be — here is what they said.

Open-shell nanographenes are used to fabricate length-controlled antiferromagnetic spin-1/2 Heisenberg chains. It is revealed that the spin excitation spectra evolve from gapped to gapless following a power-law dependence on chain length, along with the visualization of the standing waves of confined single spinons.

The synthesis of crystalline two-dimensional conjugated polymers linked by C = C bonds is highly desirable for applications ranging from membranes to electronics. In this study, the authors present a strategy for producing crystalline two-dimensional conjugated polymers films with tunable thickness and large lateral dimensions, enabling stable and efficient ion-selective transport.

A multilayer-stacked two-dimensional polyaniline crystal shows high electrical conductivity and unique out-of-plane metallic transport behaviour, indicating potential for strong electronic coupling beyond in-plane interactions and three-dimensional metallic conductivity.

A challenge for densely packed micro-supercapacitors (MSCs) is accurate electrolyte placement. Here authors report a surface adhesive-directed electrolyte assembly strategy for precise isolation of densely packed MSCs at micron scale.

On-water surface synthesis, characterized by enhanced reactivity, distinct selectivity, and confined reaction geometry, offers potential for synthesis but is currently limited by the requirement for a stable air-water interface. Here the authors present an approach that mimics on-water surface chemistry using micelles.

Endowing metal–organic frameworks with both high electrical conductivity and magnetic ordering could make such materials useful for spintronics. Here the authors design a layer-stacking coronene-based 2D MOF that exhibits a semiconducting feature with an electrical conductivity of ~10 S cm⁻¹ at 300 K, as well as ferromagnetism below ~20 K.

An antibody–polysialic acid conjugate induces calcification on the surface of methicillin-resistant Staphylococcus aureus and boosts immunogenicity in mice.

Graphene nanostructures with π magnetism offer a chemically tunable platform to explore correlated magnetic interactions. Here, the on-surface synthesis of spin-1/2 antiferromagnetic Heisenberg chains based on N-doped nanographene units is reported. The spin chains are synthesized through ortho sp³ C–H activated polymerization and exhibit parity-dependent magnetic ground states.

Scanning probe microscopy experiments realize the alternating-exchange spin-1/2 Heisenberg model via magnetic nanographene chains. They control odd- to even-Haldane phase transitions and monitor spin–spin correlations and triplon dispersion.

Heterogeneous reactions associated with porous films are vital in nature and industry. A hierarchical-structure-accelerated interfacial dynamic strategy is reported to improve interfacial gas transfer on conductive metal-organic framework films.

Selective activation of C–H bonds is a key challenge in organic reactions. Here, the authors achieve the selective activation of four quasi-equivalent C–H bonds, leading to the formation of N-doped graphene nanoribbons with partial corannulene motifs.

Layered metal-organic frameworks attract interests for optoelectronics and spintronics. Here, the authors report a strategy to tune interlayer charge transport and thermoelectric properties via side-chain induced control of the layer spacing.

MXenes with borate polyanion terminations are synthesized using a flux-assisted eutectic molten etching approach. These triatomic-layer terminations empower MXenes with considerably improved charge transport and charge storage capabilities.

The controlled growth of thin films of conjugated metal–organic frameworks is reported using an on-liquid-gallium surface synthesis strategy under chemical vapour deposition conditions. The surface flatness of the thin films is a tenfold improvement compared with samples synthesized by traditional routes.

The authors report a Cu/Cu₂Se-Cu₂O heterojunction nanosheet array which show cases efficient CO₂ reduction to ethanol using solar energy through a confluence of effects stemming from the catalyst heterostructure and including photothermal and confinement effects.

Traditional methods for tuning the dimensions of organic electronic device structures often rely on cumbersome processes with limited resolution. Here, the authors report ultraviolet irradiation in ambient conditions for tuning structural parameters for organic small molecule hole transport layers.

Controlling site-selectivity and reactivity in chemical reactions continues to be a key challenge in modern synthetic chemistry. Here, the authors demonstrate the assembly of amino-substituted porphyrins on a water surface into J-aggregate structures in the presence of charged surfactants.

Sluggish Zn²⁺-dominated Faradic reactions lead to suboptimal charge-storage capacity and durability of aqueous zinc battery cathodes. Here, the authors present a proton-selective interfacial coating strategy that enables high-performance cathodes with fast-kinetics proton-dominated Faradic reactions.

Linear π-conjugated polymers have attracted great attention as semiconductors for (opto)electronic devices, but charge transfer is only effective along polymer chains. Here poly(benzimidazobenzophenanthroline)-ladder-type two-dimensional conjugated polymers are presented with high charge carrier mobilities.

This study demonstrates the effectiveness and generality of utilizing ultrathin Cu-based hydrotalcite-like hydroxy salts as catalysts for infrared light-driven CO₂ reduction based on their d-d orbital transition mechanism.

Solution-state patterning of functional materials on surfaces is important for a number of emerging technologies. Here, the authors demonstrate a bottom-up method of endowing freestanding surfaces with mesoporous conducting polymer coatings for enhanced electrochemical capacitance properties.

Hydrogen evolution from water promises a future clean energy source, however the cost of noble metal catalysts, which are necessary for high efficiency, are very expensive. Here, the authors fabricate a porous cobalt–nitrogen/carbon catalyst which can deliver high activity and stability but at reduced cost.