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Dearomative hydrogenation of benzoic acid and its derivatives is challenging to achieve selectively. Here, a highly active Pt/TiO2 catalyst which works in the presence of common catalyst poisons, including bi- and tri-benzoic acids, is described.
Flow reactors have applications in reaction screening and optimisation, but typically operate in linear or radial configurations. Here a bench-top parallel flow synthesiser which distributes reagents between sixteen microreactors allows for rapid optimisation of chemical libraries, with uniform flow distribution even when clogging occurs.
Superabsorbent materials can absorb many times their weight in water, but are commonly derived from petroleum. Here, acylation of coagulated potato protein concentrate or soluble potato protein fruit juice yields an effective, mould-resistant, and biodegradable superabsorbent polymer.
Mechanistic insight into enantioselective reactions at intrinsically chiral surfaces can be challenging to obtain. Here the catalytic activity of Pd1- and Pd3-terminated PdGa{111} surfaces is shown to differ substantially, with Pd1-terminated surfaces promoting on-surface azide– alkyne cycloadditions enantioand regioselectively.
Ionizing radiation damage to DNA plays a fundamental role in cancer therapy, whereby water radiolysis effects are important to take into account. Here, near-ambient-pressure X-ray photoelectron-spectroscopy is used to directly measure DNA damage during irradiation in water and compared to that in a dry atmosphere.
Halide salts exhibit complex radiation-induced reactions that are relevant in atmospheric chemistry, but detailed characterizations in high-level radiation fields are challenging to obtain. Here, the authors use a custom atomic force microscope to study alkali halide surface transformations in situ under 18 kGy/hr irradiation.
Porphyrins have been incorporated into metal–organic frameworks in a periodic fashion in order to exploit their unique photophysical and electrochemical properties. This article reviews progress in the field, focusing on the fundamental physical properties that arise in porphyrin-based MOFs.
Interpreting ultrafast non-adiabatic vibronic processes of complex systems such as the excited benzene cation remains highly challenging. Here, a computational model is reported, where non-adiabatic events are seen far from a conical intersection and are controlled by electron dynamics involving a superposition of non-adjacent adiabatic states.
Robust and selective C–H functionalisation of alkanes remains a challenge. Here, iodine(III) mediates the radical coupling of N-hydroxyphthalimide and unactivated C(sp3)–H bonds in a range of cyclic and acyclic alkanes.
Chemical warfare agents and simulants are commonly detected with fluorescent sensing materials containing nitrogen-based groups, however these groups’ basicity can cause false positives in the presence of acids. Here, the authors disentangle the response of pyridyl-containing sensing materials to acid-containing and acid-free Sarin and simulants.
Electrocatalytic reactions depend on ion transport phenomena within the electric double layer, but the electrochemical response of single gas bubbles that form on catalyst surfaces remains unclear. Here, the authors use alternating current electrochemical impedance spectroscopy to detect a gateway through which ions can exchange between gas bubble surfaces and solid-state catalyst surfaces.
Criegee intermediates are reactive intermediates formed in Earth’s atmosphere through ozonolysis of alkenes. Here the authors outline the fundamental chemistry that influences their highly conformer- and substituent-dependent unimolecular and bimolecular reactivity, and discuss open questions of fundamental and atmospheric interest.
Existing routes to dibenzofurans have intrinsic regioselectivity, limiting the substitution patterns available in the products. Here a double 1,4-conjugate addition-annulation cascade between propargylamines and imidazolium methylides provides direct access to dibenzofurans with a complementary substitution pattern.
Nidovirus RNA synthesis machineries catalyze nucleotide transfer, but characterization of this activity is limited using existing methods. Here the nucleotidyl transferase activity of SARSCoV-2 replicase proteins is characterized by mass spectrometry of GMP and UMP protein adducts, allowing identification of nucleotidylation sites in vitro.
Thioesters are often suggested to be key intermediates in primordial metabolism, but prebiotic CO2 fixation routes to thioesters remain elusive. Here, the authors show nickel sulfide, partially reduced to Ni(0) with realistic geoelectric potentials, facilitates thioester (S-methyl thioacetate) formation via CO2-to-CO electroreduction, followed by a CO-methanethiol reaction.
The formation of solid solutions can result in changes of relative stabilities of crystal polymorphs. Here, the elusive form III of benzamide is stabilized through solid solution formation with nicotinamide. It is shown, experimentally and computationally, how such thermodynamic switching allows for consistent and facile crystallization of the otherwise elusive benzamide form III.
Benzylic functionalisation of unactivated toluenes remains a challenge in asymmetric catalysis. Here a chiral Brønsted base catalyses the enantioselective C(sp3)-H functionalization of unactivated alkylarenes, enabling carbon-carbon bond formation at benzylic positions of toluene derivatives.
Contact freezing of water is a very fast and common process that is still not well understood due to challenges in probing this microscopic phenomenon. Now, molecular dynamics simulations help to explain experimental data of contact freezing, showing a connection between water’s suspected propensity to undergo surface freezing and the kinetic enhancement during contact nucleation.
Cyclohexane skeletal isomerisation is an important catalytic reaction, but generally involves a trade-off between catalyst activity and selectivity. Here zeolite-based catalysts improve the selectivity of this reaction towards methylcyclopentene while retaining good activity, attributed to the acidic, structural and morphological features of the optimized catalysts.