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Although dry reforming of methane can convert CO2 to valuable chemicals, the reaction requires near-equivalent amounts of CH4. Now it has been demonstrated that an electro-thermocatalytic CH4 reforming process, when combined with the reverse water–gas shift and H2O electrolysis reactions, can efficiently catalyse CO2-rich natural gas into syngas.
Propane dehydrogenation is challenging to perform under mild conditions due to the reaction’s endothermic nature. Now, near-ambient propane dehydrogenation has been shown using copper single-atom catalysts supported on titanium oxide under light illumination and a water vapour environment.
Chemical energy conversion and storage rely on the selective movement of protons and electrons, thus understanding these processes is important for applications. Now experiments at elevated pressures are shown to identify excited-state proton-coupled electron transfer mechanisms and to facilitate merging proton transfer with subsequent electron transfer steps towards a concerted pathway.
Achieving stereochemical control in SN1-type nucleophilic substitution reactions is challenging due to the complexity of the successive carbocation intermediates. Now a strategy using neighbouring group participation to form cyclopropylcarbinyl cations enables the preparation of complex molecular skeletons via stereospecific SN1 at a quaternary stereocentre in acyclic systems.
In reticular chemistry, the formation of strong chemical bonds between molecular components is typically considered a core prerequisite for synthesizing open-framework materials. Now a series of robust frameworks have been assembled through van der Waals interactions; the stacking of polyhedral molecular building blocks results in the formation of three-dimensional open diamond networks.
Although several inorganic analogues of cyclopentadiene have been reported with group-15 elements, examples featuring the heavier elements Sb and Bi remain scarce. Now, a Bi5 ring has been stabilized between two Nb(cyclopentadienyl) units, forming a triple-decker sandwich structure; the bonding analysis indicates that a Nb–Nb bond goes through the centre of the Bi5 plane.
In 1972, Erich Clar envisioned Clar’s goblet, a polycyclic aromatic hydrocarbon featuring two unpaired electrons that are spin-paired. However, synthesizing it in a solution phase remains challenging. Now a derivative of Clar’s goblet has been prepared in solution, and spin entanglement at the molecular scale has been demonstrated experimentally.
Understanding the distance dependence and mechanistic behaviour of light-driven charge separation is crucial to advance artificial photosynthesis and solar energy conversion. It has now been shown that donor–bridge–acceptor null-coupled perylene bisimide arrays are good candidates for generating long-lived excitons and display ‘through-stack’ photoinduced electron transfer through pronounced π-orbital overlap.
Degradation of carbon-backbone polymers, which make up most plastics, remains a formidable challenge owing to their strong and inert main-chain C–C bonds. Now it has been shown that aromatization-driven C–C bond cleavage is a viable strategy to endow full degradability into carbon backbones under mild conditions.
The mechanisms that regulate the electrochemical equilibrium of condensates are not well understood. Now it has been shown that the aging process of biomolecular condensates can dynamically modulate the electrochemical equilibrium between phases, thereby affecting the physicochemical functions of condensates. This process potentially provides an active mechanism modulating intracellular ion flux.
Native proteins use hydration frustration—regulating the dehydration of hydrophilic residues and the hydration of hydrophobic residues—to enhance their activity. Now it has been shown that single-polymer-chain nanoparticles made from random heteropolymers can exhibit similar hydration frustration, following design rules orthogonal to those of proteins.
N-monofluoromethyl amides (N-CH2F) have been challenging to prepare. Now, a general method for the synthesis of N-CH2F amides is developed. The strategy can be applied for the N-CH2F modification of peptides and drug derivatives. Moreover, the N-CH2F amides are relatively stable in various media, which could be beneficial for drug development.
Transfer hydrogenation is challenging to apply to aryl halide reductive cross-couplings because of competing hydrogenolysis. Now aryl halide cross-couplings mediated by sodium formate have been developed. These processes display orthogonality to Suzuki and Buchwald–Hartwig couplings as pinacol boronates and anilines are tolerated and, owing to chelated intermediates, effective for challenging 2-pyridyl systems.
Bifunctional methyltransferase–cyclases both transfer a methyl group to alkenes and induce cyclization—a process called methylcyclization. Now a non-enzymatic silver(I)-mediated electrophilic methylcyclization has been reported. The reaction uses commercial reagents, is applicable to a wide range of substrates and affords structures that are difficult to access by conventional synthetic methods.
Antibiotic resistance can be addressed by reinventing classes of antibiotics through chemical synthesis. Here BT-33—a fully synthetic antibiotic—affords broad-spectrum activity against the bacterial ribosome. X-ray crystallography, theoretical calculations and structure–activity relationship studies reveal the structural features that contribute to the enhanced antibacterial activity and metabolic stability of BT-33.
Enzyme-catalysed 1,2-amino migration represents a viable biochemical process that is currently underutilized within the synthetic organic chemistry community. Building upon this biocatalytic mechanism, a biomimetic photoredox-catalysed 1,2-amino migration method has been developed. By integrating photoredox-catalysed conditions, this approach enables the modular synthesis of a diverse library of γ-substituted β-amino acids.
Elena De Vita and Rebecca Page reflect on the unique properties of phosphate, an essential building block with versatile functions in living systems. Modulating protein phosphorylation is an effective therapeutic strategy, with emerging approaches highlighting the continuous development in this area of drug discovery.
There are many steps to preparing a research article for publication, from generating the figures and writing the draft, to responding to reviewers. Shira Joudan explains how their group approaches this task, specifically during the preparation of the research group’s first paper.