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A small-molecule manganese-based catalyst has been developed for the selective oxidation of strong methylene C–H bonds in the presence of more oxidatively labile aromatic functionality. This reaction enables the late-stage oxidative derivatization of medicinally relevant compound scaffolds and may also prove useful for diversifying aromatic drugs and natural products, as well as helping to quickly identify their metabolites.
The concept of ‘interrupted transfer hydrogenation’ is presented, allowing the reductive hydroxymethylation of pyridinium and quinolinium salts at the C3 position. Mechanistic studies show the reaction occurs through an initial reversible iridium hydride reduction, followed by trapping of an enamine generated in situ before a final irreversible iridium-hydride reduction.
One goal of synthetic biologists is to develop artificial systems to help study biological processes. Now, cell communication and differentiation have been demonstrated using spatiotemporal patterns created in artificial multicellular compartments.
Gold nanomaterials are attractive for a variety of applications, including in medicine, but need to be made stable enough to operate in biological systems. Now, gold nanorods have been stabilized for photothermal therapy by sequential surface anchoring, using a bidendate PEG-based ligand that features a thiolate moiety and an Au–NHC moiety.
The periodic table as we know it now seems complete, its current 118 elements nicely fitting in the seven familiar rows. How many more can be synthesized — and how will the table expand to accommodate them? The search for ever-heavier elements is pointing towards new periods, though perhaps not as neatly ordered as the first seven.
The United Nations has declared 2019 to be the International Year of the Periodic Table to coincide with this iconic chemical chart turning 150 years old. We join in with the celebrations by publishing a collection of articles that explore the edges of the periodic system and look at some of the elements that do — and don’t — make up the table.
Scientists and non-scientists alike have long been dreaming of elements with mighty properties. Perhaps the fictional materials they have conjured up are not as far from reality as it may at first seem.
At its inception, the periodic table sorted elements by weight, so it may be surprising that the heaviest natural element on Earth remains controversial, or at best, nebulous. In the strange, perhaps-unfinished search for this weightiest nucleus, the only definitive conclusion is that it lies somewhere beyond uranium.
Intersystem crossing (ISC) is a radiationless process that is important in many photophysical systems. It has now been observed to take place in the exit channel for the reaction of ground-state atomic oxygen with alkylamines.
Preparation of well-defined N-glycans is very demanding, which hampers progress in glycoscience. Now, a biomimetic synthetic approach has been developed in which a readily available bi-antennary glycan can be converted in ten or fewer steps into multi-antennary N-glycans. This approach enables each arm to be uniquely extended by glycosyltransferases to give complex branched N-glycans.
Rapamycin and FK506 are macrocycles that contain an FKBP-binding domain and an effector domain responsible for interacting with their respective targets, mTOR and calcineurin. Now, a 45,000-compound macrocycle library has been synthesized by fusing oligopeptides with synthetic FKBP-binding domains. Screening and subsequent optimization yielded a highly potent FKBP-dependent inhibitor of hENT1.
Widely used palladium-mediated cross-couplings typically operate via a handful of fundamental reaction steps. Now, the reactivity between palladium and C–C σ-bonds has been described. This carbopalladation enables the coupling of organoboronic esters and aryl triflates across a C–C σ-bond of a bicyclo[1.1.0]butane to form disastereomerically pure trisubstituted cyclobutanes.
In native photosystem II (PSII), multi-chromophore antennas surround the reaction centre, capturing light and triggering the quantized (four-flashes) photo-oxidation of water to oxygen. The PSII ‘quantasome’ is the most efficient photo-electrolyser built so far. An artificial quantasome has now been developed; it is specifically designed for oxygen evolution by self-assembling light-harvesting-perylene bisimides with a ruthenium polyoxometalate water-oxidation catalyst.
The creation of a viable technology that enables precise control over the monomer sequence in synthetic polymers remains a significant challenge. High-purity sequence-defined polyethers with readily tailored side-chain functionalities have now been made through liquid-phase iterative synthesis combined with size-exclusion molecular sieving and real-time monitoring.
Some porous coordination polymers (PCPs) are known to be flexible and guest-responsive. Now, the guest-induced sharp, reversible structural transformation of the surface of a single-crystalline PCP has been visualized by in situ liquid-phase atomic force microscopy. This local response occurred at a guest concentration that was too low to trigger changes to the bulk crystal.
The SN2 reaction, a fundamental process associated with ionic chemistry, can be incorporated into a photochemical approach to creating radicals from alkyl electrophiles. This method occurs readily under visible-light irradiation, exhibits broad functional-group tolerance, and enables the formation of open-shell intermediates from substrates that are incompatible with traditional radical-generating strategies.
Synthetic gene circuits encapsulated in lipid membrane compartments are often employed as artificial cell mimics, but these lack the complex behaviour of biological tissues. Now, spatial information based on chemical gradients has been used to engineer non-trivial dynamics such as signal propagation and differentiation in an artificial multicellular system.
