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The discovery of immunosuppressive natural products and synthetic strategies to make these compounds have impacted biology and ultimately human health. This Review highlights synthetic examples of such compounds, which have the potential to discover immunological mechanisms.
Traditionally, enzymes were not commonly used as catalysts by organic and pharmaceutical chemists owing to insufficient stereoselectivity. However, this changed with the onset of directed evolution. This Review introduces mutagenesis methods, describes the enzyme-catalysed production of specific pharmaceuticals and presents further examples.
Tailoring of the short-range microenvironment surrounding the active site in ruthenium-based catalyst systems can lead to enhanced overall water splitting.
Using a fully automated closed-loop system, a robotic chemist synthesizes an oxygen-evolution catalyst from Martian meteorites, with implications for the production of catalysts that may underpin human survival on Mars in the future.
Palladium-catalysed enantioselective α-arylation of azlactones and 5H-oxazol-4-ones with aryl halides using Sadphos ligands enables the synthesis of α-aryl quaternary amino acids and glycolic acid derivatives.
Since the isolation of a Mg–Mg complex, research on low-oxidation-state s-block chemistry has flourished. An approach to forming metal–metal bonds between Mg and the heavier alkaline earth metals (Ca, Sr and Ba) is now demonstrated. The unusual electronic nature of these compounds could stimulate further discussions of metal–metal bonding.
Modular access to nimbolide could provide the opportunity to develop agents that target poly-ADP-ribose polymerase 1 (PARP1) for the treatment of BRCA-deficient cancers. Now, a convergent strategy is reported, in which late-stage coupling of a pharmacophore-containing building block and a diversifiable hydrazone unit enables the preparation of nimbolide and various analogues.
Rapid, long-distance transport of an ultrathin and uniform palladium film on a two-dimensional (2D) crystal of tungsten ditelluride at accessible temperatures is reported. The surprising effect is generalizable and offers possibilities for exploring chemical synthesis in nanoconfined spaces and access to not yet synthesized 2D materials.
An engineered ‘carbene transferase’ is shown to convert both Z and E isomers of silyl enol ethers in a stereoconvergent manner, yielding chiral α-branched ketones with high efficiency and excellent selectivity. This biocatalyst offers an efficient and high-yield method to functionalize these alkene mixtures.
A preactivation-based one-pot glycosylation strategy was used to synthesize RN1 — a polysaccharide comprising 140 monosaccharide units isolated from Panax notoginseng, as well as a glycan fragment library. Evaluation of the biological activity of the glycans in vitro revealed that a decasaccharide fragment shows anti-pancreatic cancer activity.
A nanodroplet sequential fusion strategy is presented that can be used to precisely synthesize branched silica nanotrees, creating complex and functional inorganic superstructures.
By removing water from crystalline molecular complexes, microporous metal–organic framework glasses are formed. The glasses can be obtained in monolithic shapes by melt-quenching.
Triaryloxonium salts are used as aryne precursors under mild and operationally simple conditions, allowing high functional-group tolerance, and cycloaddition reactions are used to trap the arynes generated.
Enantioselective synthesis of medium-sized rings by organocatalytic cycloadditions offers opportunities that are complementary to metal-catalysed cycloadditions. This Review discusses the ability of organocatalytic cycloadditions to synthesize stereodefined medium-sized ring architectures, critically evaluates current synthetic strategies, and highlights avenues for further development.
A β-lactone compound — globilactone A — has been discovered through genome mining and heterologous expression of a biosynthetic gene cluster. Biosynthetic investigations unveiled the mechanism of the formation of the cyclopentane-β-lactone core.
A macroscale scaffolding strategy for building arches and curved surfaces is translated to the molecular level for the face-selective design of zeolitic metal–organic frameworks (ZMOFs).
