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Expanded use of earth-abundant chromophores for excited-state chemistry requires the ability to increase the energy content of excited states while simultaneously lengthening their lifetimes. It has now been shown that this goal can be achieved in Co(III)-based chromophores by virtue of their photophysical dynamics occurring in the Marcus inverted region.
Living anionic polymerization generally requires stringent conditions and one metal initiator per polymer chain. Now it has been shown that a weakly acidic compound serves as the initiator or chain-transfer agent in the presence of a potassium base catalyst to produce a polymer chain through a proton transfer anionic polymerization mechanism.
Compounds containing metal–metal bonds can provide fresh insights into electronic structure and bonding, and their synthesis can open up new chemical space. A sandwich complex containing a lithium–aluminium bond has now delivered some food for thought in this arena.
Carbenes are reactive intermediates that undergo many useful transformations yet are typically accessed via functionalized precursors and often require additives. Now, shelf-stable alkynes have been used to generate metal-free carbenes in an additive- and by-product-free method that rapidly affords diverse heterocyclic frameworks.
Unlike homo-dihalogenation, selective hetero-dihalogenation reactions are underdeveloped. Now an oxidative alkene hetero-dihalogenation reaction adds chloride and fluoride ions over unactivated alkenes with high regio-, chemo- and diastereoselectivity. A switch in the mechanism triggers a reversal of the diastereoselectivity to promote either anti- or syn-addition.
The oxidative addition of the H–H bond to a single main-group centre in a metallomimetic fashion and its further use in catalysis is challenging. Now the oxidative addition of the H–H bond to a single phosphorus centre is shown and used for the catalytic hydrogenation of unsaturated compounds.
The characterization of surface ligands around nanoparticles is challenging and often limited to static studies. Now, the structure of the ligand shell around gold nanoparticles, and at the ligand–gold interface, has been investigated by transmission electron microscopy in a liquid environment by using high-quality graphene liquid cells.
De novo syntheses of 1,2-arylheteroaryl ethanes, key scaffolds in drug discovery, are challenging, typically relying on pre-functionalized synthons, harsh conditions and multi-step processes. Now a modular assembly of arenes, ethylene and heteroarenes yields diverse drug-like 1,2-arylheteroaryl ethanes, highlighting the importance of radical polarity matching in selective multi-component couplings.
Thermal generation of free carbenes with 100% atom economy is rare. Now, it has been shown that this can be achieved by the net [3+2] cycloaddition between many classes of 2-alkynyl iminoheterocycles and electrophilic alkynes. Together with a host of carbene trapping reactions, this method provides facile and versatile access to diverse heterocycle scaffolds.
Nitrogen-rich Ruddlesden–Popper nitrides are notoriously difficult to stabilize. Now a high-pressure high-temperature synthesis method has enabled the preparation of Pr2ReN4, Nd2ReN4 and Ce2TaN4. Neutron diffraction analysis reveals fully nitrided materials and intricate magnetic structures.
Hydroxyl radicals are reactive species capable of water purification and disinfection, although their generation, particularly through renewable approaches, is challenging. Now, low-valent Au on potassium-incorporated carbon nitride has been shown to produce hydroxyl radicals upon solar illumination and to provide high water disinfection rates.
Whereas bonds that strengthen under mechanical stress occur frequently in nature, all synthetic bonds weaken under force. Now, an artificial supramolecular catch bond has been shown to strengthen the particle–surface interface under increasing shear flow in a rolling adhesion assay, thereby mimicking biological adhesion processes.
Global antibiotic scarcity looms owing to bacterial resistance. Now the discovery of a class of allosteric inhibitors targeting DNA gyrase—essential for bacteria—yields a compound LEI-800 that exhibits activity against fluoroquinolone-resistant E. coli. The compound’s unique mode of action, revealed through cryo-EM, makes it a promising candidate for countering bacterial resistance.
The mechanistic details of entangled triplet pair formation in organic materials have been debated over the past decade. Now, the concept of coherent triplet pair formation is revived using a library of pentacene derivatives, invoking charge resonance mixing as a material design principle for harnessing the effect.
The Be–Be bond has long represented a ‘missing link’ between the H–H bond of dihydrogen and the B–B bond of diborane(4) species. Now, a complex with a polarized Be–Be bond that acts as a source of the beryllyl anion is reported. This work also reveals similarities between the homo-elemental linkages of boron and beryllium.
Due to their challenging isolation, stannynes are underexplored and poorly understood. Now, a stannyne has been synthesized and isolated at room temperature using a bulky cyclic phosphino ligand, and it has been shown to exhibit the reactivity characteristics of carbenes, stannylenes and carbon–tin multiply bonded compounds.
Constructing artificial structures that can imitate complex topological transformation with sophisticated functions is challenging. Now, using topological operations involving ‘glue–cut’ processes, the global conformational change of topology-programmed DNA origami has been demonstrated. The reconfigurable DNA origami system developed here can encode signal propagation at the nanoscale.
The optimization of chemical reactions can be laborious, particularly in the case of complex, multicomponent catalytic cycles. Now, it is shown that Bayesian optimization methods, underpinned by explainable computational physical models, can guide chemists to discover efficient organic molecular metallophotocatalyst formulations, avoiding the use of precious metals such as iridium.
Organic photoredox catalysts enable diverse chemical transformations, but predicting their activity is challenging due to complex properties. Now, a two-step data-driven approach is introduced for targeted organic photoredox catalysts synthesis and reaction optimization. Using Bayesian optimization, promising catalysts can be efficiently identified, yielding competitive results with iridium catalysts.
Standard DNA is limited by low information density and functional diversity. Now it has been shown that an expanded genetic alphabet—incorporating a synthetic nucleotide, dZ—allows for the creation of stable three-dimensional DNA structures under mild alkaline conditions. Such stable structures enrich our understanding of DNA’s structural diversity and its potential in synthetic biology applications.
