Articles in 2011

Nitrogen-containing heterocycles are ubiquitous in natural products, pharmaceuticals and in materials science. Here, the stereoselective synthesis of a wide array of structurally diverse, functionalized lactams by palladium-catalysed enantioselective enolate alkylation is described.

Traditional wisdom suggests that excited electrons will move towards positively charged parts of a molecule. Advanced time-domain calculations show that the conventional picture breaks down in the ultrafast regime, providing key insights into photo-activated, attosecond processes.

Helical coordination compounds that show promising antibiotic activity in aqueous media have been assembled directly in their optically pure form, without the need for a resolution step.

As scientists, are the decisions we make all about weighing up cold hard facts or does the last time we ate come into play? Bruce Gibb offers us some food for thought.

The most complex non-DNA synthetic molecular knot so far has been made in a single step by combining a number of reversible chemical interactions, including metal-directed self-assembly, anion templation and imine bond formation.

Oxygen has contributed to our understanding of the evolution of life on Earth by providing invaluable clues to geological processes — yet it still holds the key to some unsolved mysteries, as Mark H. Thiemens explains.

A new type of protein–polymer conjugate provides improved stability without detrimentally affecting bioactivity, and thus offers great potential for the development of new peptide-based drugs.

The classic organometallic compound ferrocene has been combined with a unique diiron unit in the latest synthetic analogue of an enzyme active site, achieving the three functionalities needed for a working model of diiron hydrogenase, itself of ancient origin.

Poly(ethylene glycol) conjugates have been widely used to improve the stability of proteins for use as therapeutics, but this stability comes at the expense of binding affinity. Here, poly(carboxybetaine) — a zwitterionic polymer — is shown to provide increased stability while also enhancing binding due to its super-hydrophilic nature.

Adsorbed carbon monoxide typically acts to poison the oxidation of alcohols on heterogeneous catalysts and electrocatalysts. Here, it is shown that carbon monoxide that has been adsorbed irreversibly on a Au(111) surface can act as a promoter for this process by enhancing the scission of C–H bonds in the alcohol to yield the corresponding aldehyde.

A general reaction-discovery platform has been used for identification of a new multicomponent transformation. The approach entails rapid analysis of interfacial chemical reactions on arrays of self-assembled monolayers using mass spectrometry. This enabled identification of a simple organic phosphine that catalyses a previously unknown condensation of siloxy alkynes, aldehydes and amines.

A designed metalloprotein containing an Hg(II) trithiolate centre that provides structural stability, and a Zn(II) tris histidine centre serving as a catalytic mimic of carbonic anhydrase, is shown to display rates that are comparable to the natural enzyme for ester hydrolysis and CO₂ hydration.