Jonathan Dennis

Abstract Hydrogen gas is naturally produced by microorganisms from renewable feedstocks, yet industrial hydrogenation relies almost entirely on fossil fuel-derived H2. Despite advances in engineering biology and increasing demand for greener manufacturing, microbial H2 has seen limited application in chemical synthesis.

Abstract Small molecule organocatalysts are abundant in all living organisms. However, their use as organocatalysts in cells has been underexplored. Herein, we report that organocatalytic aldol chemistry can be interfaced with living Escherichia coli to enable the α-methylenation of cellular aldehydes using biogenic amines such as L-Pro or phosphate.

Graphical Abstract Introducing new abiotic chemistry into living cells is a grand challenge in the field of chemical biotechnology. Here, we show that phosphate and/or biogenic amines mediate the non-enzymatic α-methylenation of butyraldehyde under biocompatible reaction conditions and can be interfaced with butyraldehyde biosynthesis from D-glucose in the bacterium Escherichia coli. Abstract Small molecule organocatalysts are abundant in all living organisms.