Simple Feedstocks Research Articles

NiH‐Catalyzed Reductive Relay Hydroalkylation: A Strategy for the Remote C(sp3)−H Alkylation of Alkenes

AbstractThe terminal‐selective, remote C(sp3)−H alkylation of alkenes was achieved by a relay process combining NiH‐catalyzed hydrometalation, chain walking, and alkylation. This method enables the construction of unfunctionalized C(sp3)−C(sp3) bonds under mild conditions from two simple feedstock chemicals, namely olefins and alkyl halides. The practical value of this transformation is further demonstrated by the large‐scale and regioconvergent alkylation of isomeric mixtures of olefins at low catalyst loadings.

Opinion: Studies on the origin of life — the end of the beginning

Understanding how life on Earth might have originated is the major goal of origins of life chemistry. To proceed from simple feedstock molecules and energy sources to a living system requires extensive synthesis and coordinated assembly to occur over numerous steps, which are governed only by environmental factors and inherent chemical reactivity. Demonstrating such a process in the laboratory would show how life can start from the inanimate. If the starting materials were irrefutably primordial and the end result happened to bear an uncanny resemblance to extant biology — for what turned out to be purely chemical reasons, albeit elegantly subtle ones — then it could be a recapitulation of the way that natural life originated. We are not yet close to achieving this end, but recent results suggest that we may have nearly finished the first phase: the beginning. Recent developments in systems chemistry have shown how the molecular building blocks of life could have arisen from plausible prebiotic feedstocks. This Perspective argues that we remain a long way from a full picture and speculates on what pieces of the puzzle are still missing.

Pd(0)-Catalyzed 1,1-Diarylation of Ethylene and Allylic Carbonates

An efficient protocol for the one-step synthesis of biologically relevant 1,1-diarylalkanes has been described. This reaction introduces two different aryl groups across the terminal end of simple feedstock alkenes such as ethylene and allylic carbonates. The propensity to generate π-benzylpalladium intermediates dictates the exclusive 1,1-regioselectivity observed in the product.

Sugar synthesis in a protocellular model leads to a cell signalling response in bacteria

The design of systems with life-like properties from simple chemical components may offer insights into biological processes, with the ultimate goal of creating an artificial chemical cell that would be considered to be alive. Most efforts to create artificial cells have concentrated on systems based on complex natural molecules such as DNA and RNA. Here we have constructed a lipid-bound protometabolism that synthesizes complex carbohydrates from simple feedstocks, which are capable of engaging the natural quorum sensing mechanism of the marine bacterium Vibrio harveyi and stimulating a proportional bioluminescent response. This encapsulated system may represent the first step towards the realization of a cellular 'mimic' and a starting point for 'bottom-up' designs of other chemical cells, which could perhaps display complex behaviours such as communication with natural cells.