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An artificial metalloenzyme based on streptavidin with a biotinylated Rh(III) cofactor provides enantioselective access to various isoindolones with different functional groups. Rational engineering of the streptavidin scaffold reverses the stereoselectivity, offering an enantiodivergent method for the synthesis of isoindolones.
A diazapentadienyl radical featuring a disubstituted carbon centre is discovered allowing the isolation and structural characterization of a stable secondary carbon radical.
The isolation of secondary and primary carbon radical species is challenging, owing to their instability. Now the reduction of an acyclic bis(imino)carbene conjugate acid enables the isolation of a stable pentadienyl-type radical. In silico and in vitro probing of its properties reveal a propensity to act as a secondary carbon radical.
Biocatalytic methods for the synthesis of isoindolones, via C–H activation, have remained elusive. Now, an enantiodivergent artificial-metalloenzyme-catalysed method for the synthesis of chiral isoindolones is reported, using a streptavidin–biotin–Rh(III) catalyst system. Crystallographic analysis reveals the key residues that control stereoselectivity in streptavidin.
Photoinduced C(sp3)–H functionalization reactions, through hydrogen atom transfer (HAT) processes, have become a useful tool in synthesis, but challenges remain. This Perspective showcases the potential of pyridine N-oxides as HAT reagents in photoinduced C(sp3)–H functionalization reactions, highlighting how they can be readily tuned to achieve site-selectivity.
The in situ generation of reactive (di)gallenes from a gallium–fluorobenzene complex and commercial chiral and achiral bisphosphine ligands is presented. The Ga(I) complex cations can undergo reversible cycloadditions to 1-alkenes and bond insertions into H–Si and H–B bonds.
Development of fluorine rebound processes at an enzymatic Fe(III) centre are a challenge. Now, a plant-derived non-haem iron enzyme, 1-aminocyclopropane-1-carboxylic acid oxidase, is repurposed and evolved to catalyse chemo- and enantioselective C(sp3)–H fluorination, forming a range of enantioenriched organofluorine products.
A computationally guided approach was used to predict the hierarchical assembly of four trigonal-shaped organic cage compounds into a more symmetric, higher-order, tetrahedral-shaped ‘cage of cages’ that crystallizes into a porous superstructure.
Using liquid gallium as an atomically smooth substrate enables the deposition of single-crystal layers of conducting two-dimensional metal–organic frameworks.
Enantioselective triple [2 + 2 + 2] cycloadditions are reported that enable the synthesis of 3D π-extended carbo[11] and [13]helicenes, which show excellent circularly polarized luminescence brightness (up to 513 M−1 cm−1), the highest value among helicene derivatives.
Renewable electricity-driven nitrogen oxidation is a green alternative to Haber–Bosch and Ostwald processes, but it is challenging to effectively steer oxygen intermediates towards the nitrogen oxidation reaction pathway. Now, to mitigate competing oxygen evolution and improve nitrogen oxidation efficiency, the use of hydroxyl radicals as the nitrogen oxidant is proposed.
Monolayer gold could exhibit properties of benefit to various applications, but has been challenging to synthesize. Now, the exfoliation of two-dimensional single-atom-thick gold layers — termed goldene — is achieved through wet-chemically etching away Ti3C2 from Ti3AuC2, a nanolaminated MAX-phase. Goldene shows lattice contraction and an increase in the gold 4f binding energy compared with the bulk.
Atomically thin gold nanosheets are predicted to have interesting properties but their synthesis is challenging. Here the exfoliation of two-dimensional single-atom-thick gold, termed goldene, is achieved through wet-chemically etching Ti3C2 from Ti3AuC2. The synthesized goldene has promising properties as a heterocatalyst.