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While strain engineering via support modification is a powerful strategy to tune catalytic properties, it is complex to control for immobilized molecular complexes. Now the curvature of carbon nanotubes is leveraged to induce strain to metal phthalocyanine complexes and boost their electrocatalytic activity
Spillover phenomena are crucial in heterogeneous catalysis, yet remain elusive to quantitative characterization. Here the authors measure the surface concentration of hydrogen spilling-over onto TiO2 using Au/TiO2 catalysts and explain the underlying factors governing the process.
Metabolic inactivation of pharmaceuticals has not been sufficiently addressed in the field of drug delivery. Now, a hydrogen-bonded organic framework bioorthogonal platform has been designed, which in situ simultaneously activates an anticancer drug and an inhibitor of a catabolic enzyme.
Chemical synthesis of biodegradable stereoregular polyhydroxyalkanoates has the potential to reduce production costs, but achieving high isotacticity and molecular weight is challenging. Now efficient spiro-salen catalysts are developed to synthesize such polymers with high stereoselectivity from rac-β-butyrolactone.
Despite decades of intensive research, the precise mechanism and active sites involved in CO2 electroreduction on copper catalysts remains unclear. Now, a combination of experimental techniques reveals distinct sites for CO2-to-CO and CO conversion and shows that the presence of CO2 promotes CO reduction.
The large size of nucleases of commonly used CRISPR-Cas systems reduces the delivery efficiency of these gene-editing tools for therapeutic applications. Now, the cryo-electron microscopy structure of the miniature Acidibacillus sulfuroxidans Cas12f1 reveals the determinants for its activity despite its small size.
The generation of nitrogen-centred radicals and their subsequent reaction with control of stereoselectivity is a difficult task in synthetic chemistry. Now, the photoenzymatic production of nitrogen-centred radicals and their use in challenging enantioselective intermolecular radical hydroaminations is reported.
Deployment of fuel-cell-based heavy-duty vehicles requires a complete understanding of cathode degradation. Now, identical-location micro-X-ray fluorescence spectroscopy is performed on realistic membrane electrode assemblies to identify the degradation mechanisms of the platinum catalyst.
Reversibly modulating the structure of supported metals in response to dynamic working conditions is a desirable feature for catalysts. Now, the reversible transformation between single atoms and subnanometre clusters of Pd on CeO2 is demonstrated during automotive exhaust aftertreatment, achieving high methane oxidation activity and stability.
The activation of light alkanes under mild conditions is a challenging task. Now the conversion of alkanes into the corresponding olefins and oxygenates is achieved in solution using Cu powder at ambient temperature and pressure.
Controlling the stereoselectivity in free-radical-mediated reactions is challenging. Now, a metalloredox biocatalysis strategy is reported that uses engineered cytochrome P450 enzymes for the unnatural asymmetric radical cyclization of α-haloesters to arenes.
Cyclases that are able to build medium-sized rings are rare and mechanistic insights are sparse. Now, computational and experimental studies reveal how SoBcmB enables the construction of an eight-membered O-heterocycle over the intrinsically more favourable five-membered tetrahydrofuran in bicyclomycin biosynthesis.
The direct regioselective oxidation of internal alkenes to ketones poses an important synthetic challenge. Now, directed evolution of a cytochrome P450 enzyme affords a ketone synthase that can efficiently oxidize internal arylalkenes directly to ketones with high chemo- and regioselectivity.
Kinetic measurements often involve complex processes, and deconvoluting them to derive active-site chemistry becomes challenging. Now experimental kinetic measurements, density functional theory calculations and microkinetic modelling are combined to provide detailed mechanistic understanding of elementary reactions for ethylene hydrogenation on Pd–Zn γ-brass with isolated active sites.
Ethylene glycol is commercially produced from ethylene under energy-intensive thermocatalytic conditions. Now a cascade electrochemical heterogeneous system can produce ethylene glycol from ethylene or from CO2 under ambient conditions using electrocatalytically generated H2O2 and an integrated catalyst/solid-acid composite.
Hydrogen carriers play an important role in the hydrogen economy. Now, methyl formate is proposed as a suitable chemical hydrogen source for a carbon-neutral hydrogen energy cycle, and faster catalytic hydrogen production rates are achieved compared with those from the widely investigated formic acid and methanol.
Organic semiconductors have potential for application as photocatalysts, but their efficiency is limited by recombination of charge carriers before they can reach the surface. Here hydrogen-bonded organic frameworks with designed micropores decrease the exciton transfer path to improve charge utilization in photocatalytic H2 evolution.
CO2 methanation offers a route to synthetic methane production but typically requires high temperatures to achieve sufficient rates. This study presents light-driven CO2 methanation on an Au/Ce0.95Ru0.05O2 solid-solution catalyst with high CH4 production rate and selectivity benefiting from synergistic photochemical and photothermal effects.
While hydrosulfenation via addition of sulfenic acid to alkynes was reported decades ago, an asymmetric version of this reaction remained elusive. Now, Ni-catalysed hydrosulfenation of alkynes with in situ-generated sulfenic acids enables the synthesis of chiral alkenyl sulfoxides.
Molecular insights into the mechanism of amide bond formation in the biosynthesis of lincosamide antibiotics remain scarce. Now, the crystal structure of the condensation enzyme CcbD that catalyses this reaction is solved, its substrate scope investigated and a catalytic mechanism proposed.