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Microenvironment engineering through electrolyte optimization is a promising approach to mitigate catalyst poisoning effects in electrochemical systems, but the role of electrolyte anions is not fully understood. Here, in a combined experimental-theoretical evaluation, the authors study the effects of different acidic electrolytes (pH 1) on platinum for hydrogen (HER/HOR) and oxygen electrocatalysis (ORR/OER), finding that oxygen reduction performance can be improved 4-fold using nitric rather than sulfuric acid.
Magnetic resonance imaging of hyperpolarized contrast agents has enabled unprecedented imaging capabilities in a biomedical setting, but its widespread application is hindered by the time and costs associated with preparing hyperpolarized carbon-13 samples. Here, the authors demonstrate virtually-continuous production of batches of highly-hyperpolarized carbon-13 contrast agents every 15 s within an MRI system without a stand-alone polarizer.
The atmospheric oxidation of dimethyl sulfide affects the Earth’s climate, but the intricate pathways of this complex reaction are still not fully described. Here, the authors use an optimized flash pyrolysis method for gas-phase generation of the methylthio radical to study its O2-oxidation via matrix-isolation spectroscopy, and unambiguously identify two peroxyl radical intermediates.
Lithium sulfur batteries are an emerging energy storage medium, but their stability in carbonate electrolyte remains hampered by side-reactions. Here, the authors show that as-produced monoclinic gamma-sulfur on activated carbon nanofibers converts to Li2S without the formation of intermediate polysulfides, therefore eliminating irreversible side reactions and improving cycling stability.
The metal-organic framework ZIF-8 has demonstrated promise for a wide range of applications, but its synthesis typically involves methodologies that are difficult or expensive to scale up. Here the authors show how the production of nano-ZIF-8 can be conducted at the 1kg scale in an economical manner through the intermediate phase ZIF-L.
Recent high-pressure studies have uncovered many types of chemical bonds present in noble gas compounds. Here, by extrapolating what has been found so far, the authors discuss which future discoveries can be expected and recommend further avenues of exploration.
In the Martian atmosphere, CO2 clusters are predicted to exist at high altitudes motivating a deeper understanding of their photochemistry. Here the authors use quantum chemistry calculations and multi-coincidence mass spectrometry to show that a size-dependent structural transition enhances the production of \({{{{{{{{\rm{O}}}}}}}}}_{2}^{+}\) from photoionized CO2 clusters.
Transition metal-catalysed hydroacylation of alkynes using aldehydes is an atom-economical route to access α,β-unsaturated ketones, but typically requires aldehydes that bear chelating moieties. Here, the authors report a nickel-catalysed anti-Markovnikov selective coupling process to afford non-tethered E-enones from terminal alkynes and S-2-pyridyl thioesters.
The biosynthetic gene clusters of Actinobacteria are poorly expressed in the laboratory, necessitating a better understanding of the signals that promote their expression in order to exploit their full biosynthetic potential. Here, the authors show that the stress hormone epinephrine elicits the expression of biosynthetic gene clusters and influences the metabolism of Streptomyces, with the catechol moiety proving key to this response.
In-depth understanding of the bonding characteristics of the lanthanide ions in contemporary lanthanide-based materials is mandatory for tailoring their properties for novel applications. Here, the authors elaborate on open questions regarding the bonding situation in mainly molecular lanthanide (4f) compounds, where, as compared to their actinide (5f) analogs in which covalency of the bonds is a common feature, this is still under discussion for the 4f compounds.
P2-Na2/3[Fe1/2Mn1/2]O2 is a promising high energy density cathode material for rechargeable sodium-ion batteries, but its poor long-term stability in the operating voltage window of 1.5–4.25 V vs Na+/Na hinders its commercial application. Here, the authors use a combination of electrochemical impedance spectroscopy, X-ray photoelectron spectroscopy, and DFT calculations to investigate the origin of the capacity fading, which is attributed to an increase in bulk electronic resistance at high voltage that, among other factors, is nested in a structural phase transition.
Most of our knowledge about the chemical composition of the Earth’s interior is primarily retrieved by indirect observations, experiments and calculations that are limited to simple compositions. Here, the authors present the investigation of inclusions trapped in super deep diamonds as an alternative source of a wealth of information on the chemical state of the Earth’s interior through time.
Neocarcerand Octacid4 can assemble with small molecule guests at room temperature to produce irreversible noncovalent bimolecular complexes, but the nature of the self-assembly pathway remains poorly understood. Here, the author uses unrestricted, unbiased molecular dynamics simulations to capture 81 distinct Octacid4•guest self-assembly pathways, revealing that interactions at the exterior of Octacid4’s cavity portal are key.
Angiotensin converting enzyme 2 (ACE2) has been identified as a cardiovascular disease biomarker and the primary receptor utilized by SARS-CoV-2, but developing serum-stable, selective and high-affinity binders for this target is challenging. Here, the authors use affinity selection-mass spectrometry to identify multiple high affinity ACE2-binding peptides from canonical and noncanonical peptidomimetic libraries containing 200 million members.
Two-dimensional colloidal nanoplatelets can assemble into materials with promising optical properties, and the influence of local curvature on these properties is an area of active interest. Here, the relationship between nanoplatelet geometry, self-assembly, and collective properties is reviewed.
The human fibroblast growth factor receptors (FGFRs) are attractive targets for cancer therapy, but the structural basis for kinase targeting and gatekeeper mutations of covalent FGFR inhibitors are not fully understood. Here the authors report and discuss the potency and selectivity of FGFR inhibitors FIIN-2, TAS-120 and PRN1371 based on the co-crystal structures of SRC/FIIN-2, SRC/TAS-120 and FGFR4/PRN1371 complexes.
Bismuth fluoride is a promising cathode material for lithium ion batteries due to its high theoretical capacity and cycling stability, but low-cost production methods are needed for potential commercialization. Here, the authors report a synthetic method to grow pure BiF3 via thermal decomposition of bismuth trifluoroacetate.
Complexes possessing coordination spheres that can accommodate nine ligand atoms typically display spherical distributions of these atoms. Here, the authors predict that M-centered [OB-B7O7-BO] adopts unusual heptagonal bipyramidal nonacoordination.
Stimuli-responsive molecular organic crystals are of interest as actuating materials, but their mechanical responses are often poorly understood. Here, the authors study the photo-triggered phase transition of a chiral salicylideneamine crystal and uncover superelastic behaviour induced by light irradiation.
Copper-based catalysts are widely investigated for the industrially important hydrochlorination of acetylene (PVC production), whereby phosphorus-doped carbon supports have been found to improve the catalyst’s properties. Here the interaction between the P-C bond and atomically dispersed Cu2+ species is clarified and the reaction path of C2H2 and HCl revealed.