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Site-selective installation of fluorine (19F) and its radioisotope (18F) in aromatic molecules can lead to high-value products, but methods for this purpose are not without limitations. Now, using photochemistry, a 19F- and 18F- labelling strategy is reported that complements traditional approaches.
Axial chirality is found in many important compounds, such as bioactive molecules and catalytic components. Now palladium and chiral norbornene cooperative catalysis is reported for the construction of atropisomeric biaryls and chiral fluorenols.
The reductive deuteration of unsaturated hydrocarbons is a promising deuterium-labelling strategy, although it requires expensive gaseous D2 or other stoichiometric reagents. Here, an electrocatalytic palladium membrane reactor is employed to selectively generate C(sp3)–D bonds via reduction of unsaturated compounds using D2O.
The Mackay crystal is a proposed—but synthetically unachieved—nanocarbon molecule that is anticipated to have many desirable properties. Now, a strategy based on annulative coupling of chlorophenanthrene derivatives is reported, allowing streamlined access to an important substructure.
Isolating the role of water in aqueous reactions where it is directly involved as a reactant is equally important and challenging. Now, by confining water inside an organic liquid matrix, the authors observe the formation of aqueous-rich nanodomains and find that the reactivity of the system varies with their nanostructure.
Computational chemistry has remained largely inaccessible to the experimental chemistry community. Here we report the VIRTUAL CHEMIST, a software suite free for academic use, that enables organic chemists without expertise in computational chemistry to perform virtual screening experiments for asymmetric catalyst discovery and design.
The Sonogashira cross-coupling is a key strategy in modern synthesis for C–C bond formation and introduction of the versatile alkyne functionality into organic molecules. Now, a complementary method is reported based on the palladium-catalysed cross-coupling of lithium acetylides with aryl bromides.
Alkali metals have been traditionally used to promote heterogeneous catalysts, albeit their mode of action remains controversial. Now, the authors demonstrate the multifaceted role of sodium ions in promoting atomically dispersed Ru(iii) on Al2O3, resulting in a superior hydrogenation catalyst.
Dual nickel/photoredox catalysis is a promising alternative for palladium-catalysed cross-couplings, but suffers from limitations. Now, the substrate scope and reproducibility of this method are improved by avoiding catalyst deactivation and strategies to achieve the latter are reported.
The stability of polymer electrolyte membrane fuel cells is limited by the degradation of the cathode catalyst during repetitive start-up/shut-down events — a parasitic oxygen reduction reaction on the anode causes an instantaneous potential jump at the cathode. The issue is now addressed by selectively suppressing the oxygen reduction reaction on the anode by exploiting the metal–insulator transition behaviour of Pt/HxWO3 catalysts.
Unlike with inorganic photocatalysts, the facet-dependent reactivity of conjugated polymers remains elusive. Now, the authors provide molecular-level insights on the reactive facets of crystalline poly(triazine imide) intercalated with LiCl and achieve a remarkable improvement in its overall photocatalytic water splitting activity.
In the development of chemical complexity—and the transition into biology—developing catalytic functionality is essential. Here the authors report the emergence of catalytic activity for two separate reactions (including one demonstrating a positive feedback on replication) in a self-replicating system.
Achieving high enantioselective control in the hydrogenation of aliphatic ketones is a long-standing challenge. Now, the design of a spiro iridium catalyst with a narrow, crowded chiral pocket allows highly enantioselective hydrogenation of these compounds.
Tuning the structures of subnanometric metal clusters is challenging but can unlock unexpected catalytic properties. Here, the authors show that changing the composition of MFI zeolite-encapsulated PtSn subnanometric clusters by adding just a few tin atoms can lead to a remarkable stability enhancement in propane dehydrogenation.
Polyketide biosynthesis has remained exclusively based on polyketide synthases. Now, it is shown that certain thiolases can be employed instead, providing a method that offers distinct advantages for the synthesis of valuable products.
Spinel oxides have attracted interest as water oxidation catalysts due to their efficiency and cost-effectiveness. Now, the covalency competition between tetrahedral and octahedral sites is shown to dominate the OER activity on spinel oxides, and the design principle is used to predict and confirm the superior activity of [Mn]T[Al0.5Mn1.5]OO4.
The cleavage of C–F bonds through hydrodefluorination is challenging and has been traditionally limited to unsaturated fluorocarbons. Now, a simple plasmonic approach based on the use of aluminium nanocrystal-supported palladium nanoparticles is introduced to effectively upgrade fluoromethane under visible light.
Site-selective functionalization at chemically inert positions within hydrocarbon molecules is a major challenge in organic chemistry. Iron-catalysed borylation at less-reactive positions vicinal to common functional units by sequential isomerization/protoboration of alkenes is reported.
The asymmetric O-alkylation of alcohols is a useful route to chiral ethers, but aliphatic secondary alcohols have proven to be difficult substrates. Here the authors report a method to achieve this by developing conditions to avoid the decomposition of the alkylating agent.
Methods for the enantioconvergent tertiary C–H functionalization are scarce, but desired for the construction of valuable compounds. Now, a highly enantioconvergent tertiary β-C(sp3)–H amination of racemic ketones with copper/chiral phosphoric acid dual catalysis is reported.