Themed collection 2024 Chemical Science Covers

The comparison of homologous hydrogenases, in which the same inorganic active site is surrounded by a variable protein matrix, has demonstrated that residues that are remote from the active site may have a great influence on catalytic properties.

While chemistry has a role as the central science, other sciences are also central to solving the problems that lie ahead. To be more effective in this endeavor, we need to connect disciplines and break down the silos that artificially separate them.

Advances in bioorthogonal polyoxometalate (POM) chemistry will open exciting opportunities for the controlled use of stimuli-responsive POM-based organic–inorganic nanoassemblies in biomedical applications as well as catalysis and electronics.

This perspective focuses on the latest understanding of the folding-promotion mechanisms by chaperones and oxidoreductases and recent progress in the development of chemical mimics that possess activities comparable to enzymes.

We summarize the challenges to design and synthesize self-assembled molecules, discussing their synthetic routes and structural features in relationship to the efficiency of perovskite-based solar cells where they are applied as selective contacts.

The current amyloid hypothesis does not capture the full complexity of Aβ aggregation. Here we lay out a supersaturation framework to better understand the molecular mechanism of Alzheimer’s disease and to develop more effective treatment strategies.

Recent advances and present status of 3D-printed micro-batteries with respect to the connection between printable materials and printing techniques, as well as the rational design considerations are summarized.

Fluorescent probes for detecting complex environments in vivo play an important role in self-assembly in vitro.

This review highlights the design and synthesis of water-stable MOFs, as well as their applications in carbon capture.

This review covers the syntheses, functionalization strategies of hollow carbon-based materials, as well as their applications in electrocatalytic and thermocatalytic CO₂ conversion.

How a peptoid binds to a protein was revealed by a co-crystal structure and systematic physicochemical studies.

Tailor-made drug release materials based on non-porous therapeutic coordination polymers in which drug-release rates can be primarily tuned by the strength of metal–ligand interactions and finely tuned by altering the length of bis-imidazole linkers.

Ultrafast surface proton hopping conduction was achieved in a gyroid nanostructured polymer films having a 3D continuous interface where sulfonate groups are aligned densely and periodically.

Energy levels of interfacial recombination centres and photocorrosion potential for Zn_0.25Cd_0.75Se particulate photoanodes in nonaqueous electrolytes containing various Ru complexes are elucidated. Redox reaction of Ru complexes can serve as a probe.

A bent azide intermediate is key to form 1-azido-1′-nitrenoferrocene from 1,1′-diazidoferrocene, as shown with UV-pump–mid-IR-probe transient absorption spectroscopy and density functional theoryTD-DFT calculations including spin–orbit coupling.

^63/65Cu solid-state NMR spectroscopy provides a wealth of information regarding the local geometry and bonding at Cu(I) in metal–organic frameworks. This approach is also applicable when systems contain Cu(II) centers or at lower magnetic fields.

A high-throughput single-cell MS platform that can perform both lipid profiling and unsaturated lipid CC location isomer resolution analysis was developed, which can be effectively used for in-depth structural lipid metabolism network analysis.

A protein-based model of carbon monoxide dehydrogenase displays distinct X-ray absorption, EPR, and vibrational signatures upon CO and CN⁻ binding that support ligand-dependent electronic rearrangement throughout the nickel–iron–sulfur core.

Surpassing the tradition, experimental and DFT calculations showed the crucial role of water in the selective synthesis of tetrahydropyridines, aminoketones or enamines via allyl Grignard addition to nitriles, unmatched by dry organic solvents.

DNA compaction is a critical aspect of gene regulation and has significant implications in the field of medicine. This work focuses on an innovative and alternative compaction method for DNA using choline-based magnetic ionic liquids.

Aromatic phosphorus heterocycles react at room temperature highly selectively and reversibly with water by P,N-cooperativity. The aromaticity of such compounds plays an appreciable role in the reversibility of the reaction, supported by NICS calculations.

Molecular Fe azaphthalocyanine catalysts with diverse long-chain “dancing patterns” demonstrate variable oxygen reduction reaction performance for fuel cells, aligning well with our pH-field coupled microkinetic model.

The synthetic receptor cucurbit[8]uril (Q8) binds the N-terminal dipeptide site Lys-Phe with subnanomolar affinity in neutral aqueous buffer.

Cross-coupling of organic fluorides with allenes via radical rearrangement to afford all-carbon quaternary centres mediated by silylboronate/potassium tert-butoxide is disclosed.

Introducing 4-amino-3-thiophenol BODIPY “turn on” probe tunable to NIR wavelengths for monitoring aldehydes in tissues and living organoids by forming dihydrobenzothiazole products with aldehydes, exhibiting a remarkable fluorescence increase.

α-Keto-, β-acetoxy- and β-amidoalkylsilyl peroxides are prepared from various precursors and utilized for Fe-catalyzed and visible-light-promoted radical functionalization with coupling partners under mild conditions with a broad substrate scope.

A genetically encoded aptasensor platform for non-invasive measurement of drug distribution in cells and zebrafish was developed.

STEP: single-cell target profiling, an integrated pipeline for profiling cellular-specific targets of active small molecules in tissues.

Nafion introduced into an aqueous electrolyte activates a thermodynamically ultrastable Zn/electrolyte interface, which guides the directional Zn²⁺ electrodeposition along the (002) crystal surface for a dendrite-free Zn metal anode.

The Accelerated SuFEx Click Chemistry (ASCC) protocol, adapted to a 96-well plate format, has been applied to the late-stage derivatization of bioactive molecules and array synthesis of anticancer agents, showcasing its potential for drug discovery.

Simple structural modifications significantly boost the photochromic performance of imine-based photoswitches. This work lays a foundation for exploring new motifs in light-addressable dynamic combinatorial chemistry.

Laser heating of zeolites in combination with time-resolved IR spectroscopy is introduced as a means of studying chemical processes in heterogeneous catalysts from nanoseconds to seconds.

Interfacial enhancement is evidenced on Mo₂C@MoS₂ heteronanorods for the efficient nitroarenes ECH, which promotes the bindings of H* and nitro substrates on Mo₂C–MoS₂ interfaces toward the fast elementary steps of the Langmuir–Hinshelwood mechanism.

The second coordination sphere, Asp721, participates in a hydrogen bond with an iron-coordinated water molecule, thus compensating for the missing facial triad carboxylate in AspH and enabling stereoselective C–H oxidation.

The air–water interface is not the site for H₂O₂(aq) formation; instead, it takes place at the solid–water interface.

In the dynamic environment of multi-component reactive molten salts, speciation unfolds as a complex process, involving multiple competing reaction pathways that are likely to face free energy barriers before reaching the reaction equilibria.

A versatile Ru-porphyrin catalyst system was developed for the mild and selective aerobic epoxidation of alkenes in which water was shown to play a key role as corroborated by detailed mechanistic studies.

In this work, we study the interplay between hydrophilicity/hydrophobicity in cationic aggregation induced emitters, and their application in light emitting electrochemical cells.

ZIF-8 vaccine enhances the humoral immune response through sustained antigen exposure to the immune system whilst zinc adjuvants the vaccine via inducing T cell activation.

Cryogenic double ion trap IR spectroscopy combined with isotopic labelling reveals that the solvent-mediated intracluster proton transfer mechanism in microhydrated protonated p-aminobenzoic acid changes from vehicle to Grotthuss between n = 5 and 7.

Li intercalation and graphite stacking have been extensively studied because of the importance of graphite in commercial Li-ion batteries.

A Cu^II-responsive allosteric DNAzyme was designed by introducing bifacial 5-carboxyuracil (caU) bases that form both hydrogen-bonded caU–A and metal-mediated caU–Cu^II–caU base pairs, and was synthesized by joining short caU oligomers with a DNA ligase.

Oxime chemistry as a robust building block for dynamic networks.

We use a time-resolved method to control the integration of gold nanoparticles in MUV-10 for hybrid crystals with enhanced catalytic performance.

Uniform particle size of high-nickel cathode materials boosts lithium-ion mobility in a cylindrical lithium ion battery cell.

We report reversible switching of oxazine, cyanine, and rhodamine dyes by a nanoporous antimony-doped tin oxide electrode that enables single-molecule (SM) imaging of electrochemical activity.

Intracellular singlet oxygen (¹O₂) generation and detection help optimize the outcome of photodynamic therapy (PDT).

In situ chemistry of solid silver pyrazolates with ethylene gas, depending on the pyrazolyl ring substituents, stops at a trinuclear complex or leads to complete structure re-organizations producing dinuclear complexes as evident from PXRD data.

Quantum-chemical analyses reveal: Si–Si bonds are longer, weaker, and react oppositely to introducing bulkier substituents than C–C bonds.

CO₂-to-ethanol conversion is achieved using a superhydrophobic Cu₂O hollow structure (O–CHS) by continuous CO₂ transport, which maintains a high CO₂ concentration on the catalyst surface and further lowers the energy barrier for C–C coupling.

A series of heptamethine–oxonol dyes featuring different heterocyclic end groups were designed with the aim to explore structure–property relationships in π-extended coupled polymethines.

Two-color infrared photothermal microscopy (2C-IPM) can be used to study lipid metabolism in lipid droplets (LDs). Using deuterated fatty acids, it distinguishes endogenous and newly synthesized lipids, allowing quantitative analysis and monitoring of neutral lipid synthesis in living cell LDs.

The [4 + 2] cycloaddition has led to diverse polycyclic chiral architectures, serving as novel sources for organic synthesis and biological exploration.

Symmetry breaking charge transfer followed by charge separation with appreciable lifetimes has been demonstrated in a newly synthesized bisstyrylBODIPY dimer in polar solvents using pump-probe and other techniques.

The fusion of nonthermal plasma with charged nanodroplets enables selective esterification of saturated fatty acids, which is utilized to overcome challenges associated with type II isobaric overlap in direct infusion mass spectrometry.

Efficient carrier separation is important for improving photochemical water splitting.

Two supramolecular complexes were prepared using cucurbiturils [CBs] as mediators and a four-armed p-xylene derivative (M1) as a guest molecule.

An interdisciplinary approach to derive the structure of a disordered supramolecular system.

The separated contributions from cations, anions, and water in solvation of small molecules are addressed, and the role of the excluded-volume effect is pointed out through correlation analyses.

The presented penta- and hexahelicenes with two boron–nitrogen groups resemble their all-carbon analogs structurally but show considerably improved (chir)optical properties like absorptivities, quantum yields and luminescence dissymmetries.

Ionic strength and solid state packing effects have been used to remove the coordinated water molecule from the LnDOTA complexes, allowing to understand the magnetic anisotropy and single molecule magnet properties of these complexes.

A TADF-emitter was employed to unveil the lysosomal polarity variations during interorganelle interactions and was demonstrated as an indicator to probe complex biological processes like aging through intracellular lifetime imaging.

The heterogeneous electron transfer reactivity of single layer graphene can be regulated by defect engineering via electrochemically induced bromination which offers new possibilities for leveraging graphene in various electrochemical applications.