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Rhodamine derivatives are useful spirocyclic fluorescent probes, but tuning their properties can involve laborious synthesis and screening. Here quantum chemical modeling of the equilibrium between open and closed forms allows prediction of the pK of cyclisation and rational tailoring of properties of interest.
Liquid-liquid phase separation occurs in cells and can be induced in artificial systems, but the mechanism of the effect of molecular crowders is unclear. Here dehydration entropy-driven phase separation of model charged polymers lacking any chemical complexity or hydrophobicity is shown to be enhanced by polyethylene glycol.
Modern NMR methods such as chemical shift imaging and mobility ordered spectroscopy offer direct insight into the spatial distribution of chemical species within heterogeneous systems. Here, spatial molecular-dynamically ordered spectroscopy (SMOOSY) is developed and used to characterise the spatial distribution and diffusion behavior of small molecules within a heterogeneous biological sample.
Ferrihydrite nanoparticles have many hydroxyl sites which can react with environmental contaminants and nutrients, but the surface structure of this common mineral is still not fully understood. Here, a combination of vibrational spectroscopy and molecular simulations identify hydroxyl groups exposed along rows at the edges of sheets of iron octahedra.
Formaldehyde is known to react with nucleophilic amino acids in solution but its in vivo nonenzymatic reactivity is poorly understood. Here LC/MS and isotopic labeling studies suggest nonenzymatic formaldehyde metabolism may occur in living mice through the direct reactivity of formaldehyde with amino acids, including a possible role of timonacic, a product of formaldehyde and cysteine, as a reservoir.
Inserting membrane proteins into networks of droplet interface bilayers is important for building biomimetic minimal tissues. Here this is achieved using a chemically activatable mutant of the mechanosensitive channel of large conductance (MscL), where translocation of the activator through the channel defines the overall network flux.
Lectin-like oxidised LDL receptor 1, LOX-1, is implicated in cardiovascular diseases and cancer. Here a small molecule inhibitor of LOX-1 is introduced, which in a unique mode of action stabilises dimers of LOX-1 to prevent LOX-1 mediated signalling.
Characterising ensembles and populations of disordered structures is a challenge in structural biology. Here a Bayesian model allows solution data from NMR, fluorescence, and SAXS experiments to be synthesised in order to quantify the conformational distribution of disordered protein states.
Hydrogenated BiOCl shows high performance as a semiconductor photocatalyst, but the mechanism and synergetic effects of hydrogenation are hard to study. Here interactions of oxygen vacancies and hydrogen atoms in BiOCl nanosheets show a modulation of energy dispersion, which leads to both improvements in charge separation and photocatalytic activity.
Ultrafast laser pump-probe methods allow chemical reactions to be followed in real-time, but to directly show the rearrangement of nuclear frameworks is challenging. Here an improved real-time-resolved 3D covariance-map Coulomb explosion imaging technique for ultrafast gas-phase reactions is presented.
C60 is a highly efficient singlet oxygen (1O2) photosensitizer, but its oxidation by self-sensitized 1O2 has not been reported. Here, the authors uncover a single-photon oxidation mechanism via self-sensitized 1O2 in solvents above an excitation energy of 3.7 eV.
Lysine trimethylation is a key post-translational modification, which some epigenetic reader proteins detect through binding to aromatic cages involving cation-π interactions. Here systematic modification of the aromatic cage reveals that weaker cation-π interactions do not correlate with weaker binding owing to a compensating release of bound water molecules.
In microbial fuel cells direct electron transfer offers high energy conversion efficiency, but low concentrations of redox centers on bacterial membranes result in low power density. Here nitrogen-doping is fine tuned to match Flavin reaction sites, converting diffusive mediators to anchored redox centers toward direct electrochemistry.
Bolaamphiphiles can form liquid crystalline phases with unusual honeycomb-like structures. Here a periodic dodecagonal supertiled structure is observed in liquid crystals, emerging at the transition from triangular to square tiling patterns.
Selective functionalisation of the N-terminus of peptides and proteins may offer a useful tool for single-site modification. Here a general method for selective N-terminal labeling of peptides is reported, based on cyclisation of ethynylbenzaldehyde to form stable isoquinolinium salts.
Low-temperature manganese-based denitrification catalysts require a balance between high reduction reactivity and selectivity. Here aluminium in a mesoporous molecular sieve induces the growth of manganese oxide to obtain an iron-manganese catalyst which achieves high efficiency at temperatures of 150–300 °C.
The microscopic evolution of elementary chemical reactions remains challenging to describe, as a plethora of parallel channels often determines reaction dynamics. Here the authors propose a theoretical approach to formulate the optical potential for Ne*(3P2,0) chemi-ionizations as a prototype gas-phase oxidation process.
Sequence-defined macromolecules are a synthetic challenge but offer opportunities for high-density data storage. Here, Passerini three-component reactions yield dual sequence-defined oligomers via an iterative reaction cycle in which both the backbone and side-chains are independently varied, allowing more than 33 bits to be stored in a pentamer.
Radionuclide pairs 44Sc/47Sc and 86Y/90Y possess great promise in the development of theranostic agents, but realizing the full potential of these isotopes necessitates improving rare-earth chelation chemistry. Here the authors show that a hydroxypyridinone-based ligand is a promising candidate for applications in this arena.
Tyrosinases are an industrially significant class of polyphenol oxidase. Here, two tyrosinases are shown to cleave a specific peptide bond in a carboxylesterase, yielding a truncated product with higher catalytic activity than the full-length enzyme.