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Molecular daisy-chain structures are typically made up of two interlocked components and can exhibit muscle-like contraction and extension in one dimension. Zinc-based multicomponent systems that can operate in two and three dimensions have now been designed and synthesized.
Covalency in actinide–ligand bonding is poorly understood compared to that in other parts of the periodic table due to the lack of experimental data. Here, pulsed electron paramagnetic resonance methods are used to directly measure the electron spin densities at coordinated ligands in molecular thorium and uranium complexes.
Although the synthetic chemistry of carbon dioxide has generally been limited to two-electron pathways, single-electron mechanisms would open avenues to new reactivity. Now, the coupling of carbon dioxide and amines to produce α-amino acids can be achieved by an organic photoredox catalyst in continuous flow.
The design and prediction of network topology is challenging, even when the components' principle interactions are strong. Now, frameworks with relatively weak 'chiral recognition' between organic building blocks have been synthesized and rationalized in silico — an important development in the reticular synthesis of molecular crystals.
Michael Donnay and Michelle Francl want chemists to share the stories behind the work they do, and not be afraid to identify the heroines and heroes — and their epic adventures — that paved the way.
Nature oxidizes biosynthetic intermediates into structurally and functionally diverse peptides. An iron-catalysed C–H oxidation mimics this approach in the lab, enabling chemists to synthesize structural analogues with ease.
Although metal–organic frameworks are often seen as rigid crystalline structures, there is growing evidence that large-scale flexibility, the presence of defects, and long-range disorder are not the exception, but rather the norm. Here we propose that these concepts are inescapably intertwined, and the interfaces between them offer prospects for enhancement of materials' functionalities.
As compared to the drug discovery process, the development of new 18F PET tracers lacks a well-established pipeline that advances compounds from academic research to candidacy for (pre)clinical imaging. In order to bridge the gaps between methodological advances and clinical success, we must rethink the development process from training to implementation.
Imagine a class without lessons, tests and homework, but with missions, quests and teamwork. Video games offer an attractive educational platform because they are designed to be fun and engaging, as opposed to traditional approaches to teaching through lectures and assignments.
Higher-order cycloadditions — cycloadditions involving more than six π electrons — provide easy access to complex molecules containing heterocyclic or carbocyclic scaffolds. Now, it has been shown that aminocatalytic activation of 2-cycloalkenones affords mixtures of dienamines that can undergo [6 + 4] cycloadditions with heptafulvenes through a cross dienamine, or [8 + 2] cycloadditions through a linear dienamine.
Unlike in biomolecular systems, synthetic self-assembly is largely spontaneous, thus limiting the complexity and functionality of the materials one can create. Now, self-assembly under out-of-equilibrium conditions is demonstrated for a metastable supramolecular system. Differentiation of nanoparticles into nanofibres and nanosheets — with electronically distinct states — is achieved through kinetic control, illustrating pathway-dependent material properties.
The operational simplicity of modifying the surfaces of thiol-capped gold nanoparticles has been a hallmark of their success in materials chemistry, despite having limited control over the surface composition. Now, SNAr chemistry on activated perfluoroaromatics has been shown to mimic this simplicity and allow for the synthesis of atomically precise nanomolecules.
Using self-assembly to generate hydrogen-bonded organic networks is an underexplored method when preparing functional framework materials. Now, taking cue from DNA, bio-inspired G-quadruplexes are used as both intrinsic electron donors and hydrogen-bonding linkers to assemble rylene diimide acceptors. The resulting rectangular grids form layered crystalline frameworks, in which photoexcitation produces long-lived mobile charge carriers.
The transmission of chemical information across lipid bilayer membranes is crucial in biological systems. Now, an artificial chemical system able to both transduce and amplify chemical signals across a membrane has been developed. The system works by exploiting the controlled translocation of a synthetic molecule that is embedded within a vesicle membrane.
The use of earth-abundant metals in catalysis is a prerequisite for the development of sustainable synthetic chemical processes for the future. Now, biomass-derived chemicals can be used in an efficient iron-catalysed reaction to make complex spirocycles. The resulting products contain two asymmetric centres that are furnished in high stereoselectivity.
Effective regulation over the motion of self-propelled micro- and nanomotors is a challenging proposition. Now, self-assembled stomatocyte nanomotors with thermoresponsive polymer brushes have been designed that sense changes in local temperature and regulate the accessibility of the hydrogen peroxide fuel — thereby adjusting the speed and behaviour of nanomotor itself.
Parallel kinetic resolution (PKR) of N-heterocycles via asymmetric acylation has been achieved using quasienantiomers of polymer supported hydroxamic acid reagents. Flow techniques provide physical separation of the reagents, establishing a practical implementation of PKR. The enantioenriched amide products can be readily deprotected to reveal the desired amine without detectable epimerization.
Singlet fission — the splitting of a singlet exciton into two triplets — is a process that could be exploited to improve the power conversion efficiency of solar cells. Spectroscopic data now suggest that coherent and incoherent mechanisms for singlet fission in crystalline hexacene coexist and occur on different timescales.
