Themed collection Celebrating our 2021 Prizewinners

Metal–organic frameworks host many types of compositional and structural disorder. In this Highlight article we explore cases where this disorder is correlated, rather than random.

An overview of recent progress in the design of gadolinium-functionalised gold nanoparticles for use in MRI, multimodal imaging and theranostics.

This highlight article surveys some of the key recent advances in crystallization techniques, polymorphism, co-crystals, amorphous materials and crystal engineering.

Cost-effective and atom-efficient isotopic enrichment enables ¹⁷O NMR spectroscopy of microporous materials to be used to probe local structure and disorder and to explore chemical reactivity.

State-to-state chemical reaction dynamics, with complete control over the reaction parameters, offers unparalleled insight into fundamental reactivity.

We survey and assess current knowledge regarding the primary photochemistry of hydrocarbon molecules and radicals.

Stimulated Raman histopathology with computer aided diagnosis.

This review summarises the recent advances of covalent organic framework photocatalysts including structures and applications.

This review summarizes the recent advancements in π-conjugated polymers for various photocatalytic applications under visible light.

Carbon capture and storage (CCS) is vital to climate change mitigation, and has application across the economy, in addition to facilitating atmospheric carbon dioxide removal resulting in emissions offsets and net negative emissions. This contribution reviews the state-of-the-art and identifies key challenges which must be overcome in order to pave the way for its large-scale deployment.

While conventional approaches to stabilizing main group radicals have involved the use of Lewis acids or bases, this tutorial review focuses on new avenues to main group radicals derived from combinations of donor and acceptor molecules.

An emissive yet charge-generating organic donor/acceptor blend is demonstrated, which highlights the importance of electronic hybridization between the charge-transfer and local-exciton states to reduce non-radiative recombination loss.

X-ray radiation induced unit-cell contraction and phase transition selection in the negative thermal expansion material cadmium cyanide.

The coordination behavior of the P₄ butterfly complex toward various d⁶-based half-sandwich complexes is investigated, with the P₄ unit being selectively activated.

A high-throughput mass spectrometry based M^pro assay identifies penicillin esters as new SARS-CoV-2 M^pro inhibitors.

The first mixed-ligand self-assembly reactions of the diarsene complex [Cp₂Mo₂(CO)₄(μ,η²-As₂)] and N-donor organic molecules in the presence of AgPF₆ allow for the synthesis of two discrete and four polymeric supramolecular aggregates.

We report a D_4h@Dy single-molecule magnet (SMM) with a U_eff energy barrier of 1565 K, one of the highest energy barriers for any 6-coordinate lanthanide SMM.

Hard-carbon electrolyte interface stabilisation with a nano-zeolite ZSM-5 electrolyte additive. Unwanted degradation products are trapped within the zeolite cage preventing compositional changes at the interface, maximising the life-time of a sodium-ion battery.

Methyl protonation in a deuterated protein background is used to assign DEER-derived multimodal distance distributions by phase-memory relaxation time filtering.

The incorporation of sterically hindered boron centers into MOFs allows the recyclable adsorption of NH₃ vapour from aqueous solution.

In this article we report a procedure for α-C(sp³)–H amination of ethereal compounds through use of azodicarboxylates as the nitrogen source and freely-available atmospheric oxygen to access ethereal radical intermediates via aerobic C–H activation.

In analogy to transition-metal carbene chemistry, [(OC)₅MoBN(SiMe₃)₂] acts as a source of a borylene fragment for selective intermolecular insertion into C–H bonds under very mild conditions.

The practical synthesis of pseudo-enantiomeric carbohydrate-based NHC–Rh complexes bearing C1 or C3 sterically differentiated positions is reported. We show that steric bulk at either C1 or C3 leads to enantiotopic discrimination in the hydrosilylation of acetophenone.

A bacterial metabolic probe with AIE characteristics shows great potential in in vivo light-up imaging of bacteria and antibacterial therapy.

Superior transparent conducting properties of indium oxide realised by molybdenum donors resonant in the conduction band, avoiding detrimental effects of tin doping.

Two novel triphenylamine based conjugated microporous polymers are designed and synthesized for photocatalytic CO₂ reduction using water vapor as electron donor under ambient condition (>420 nm).

A dipole-bound state is found to survive despite its disruption by an alkyl chain.

Theoretical and experimental investigations of diacetylene-linked COFs with remarkable charge-transport properties.

Protein corona sensor array technology identifies diseases through specific proteomics pattern recognition.

Effective enantioselective reduction of ketimines has been demonstrated by ‘frustrated’ Lewis pair catalysis using an IBiox-stabilised borenium cation.

Acids play positive and negative roles in Mn-catalysed C–H funtionalisation reactions, from substrate sensitivity to catalyst longevity.

Herein, we provide a new easy-to-do protocol for preparing luminescent rubber-like materials based on a wide palette of compounds, such as small-molecules, quantum dots, polymers, and coordination complexes.

‘Designer’ p53: semi-synthesis of the tumor suppressor protein p53 via native chemical ligation enables in vitro structure–activity studies to reveal how this master regulator of cell fate is itself regulated by phosphorylation.

Generic in silico methodology – CrystalGrower – for simulating crystal habit and nanoscopic surface topology to determine crystallisation free energies.

A chemo-enzymatic site-specific fluorination strategy is employed to obtain glyco-nanoparticles with tuneable selectivity towards galectins.

An alternative approach to maleimide conjugate stabilisation is presented, by the consecutive addition of a thiol and an amine to dibromomaleimides. The amine serves to simultaneously deactivate the maleimide and enable dual functionalisation.

A combined experimental and theoretical study on the mechanism of the C–F bond activation of C₆F₆ with [Ni(NHC)₂] is provided.

Exhaustive deoxygenation of perrhenate by pinacol borane forms a new Re anion of boron and hydride ligands only that undergoes borane ligand exchange, stoichiometric C–H boration, and catalytic pyridine hydroboration.

Oligomer chain length and backbone twisting were found to have a strong effect on optoelectronic properties but a trimer of dibenzo[b,d]thiophene sulfone was found to have high photocatalytic activity approaching that of its polymer analogue.

An organic catalyst uses low-energy photons to generate acyl and carbamoyl radicals upon activation of the corresponding chlorides via a nucleophilic acyl substitution path. The synthetic potential and the mechanism of this strategy are discussed.

Use of sensitive, non-destructive and straightforward 3D SERS for investigating the cellular uptake processes of functionalised nanotags in entire cell volume.

A unified framework that explains the reactivity of [1.1.1]propellane through electron delocalization.

The failure of the Stokes–Einstein relation is assessed in aerosol measurements and molecular dynamics simulations.

Modulation of pore environment is an effective strategy to optimize guest binding in porous materials.

Molecular simulations led to the discovery of a new class of small molecules that inhibit the cyclophilin family of proteins.

We present a comprehensive investigation of a recently introduced method to determine transient structures of molecules in excited electronic states with sub-ångstrom resolution from time-resolved gas-phase scattering signals.

Exposure to micro/nanoplastics (M/NPLs) deteriorates the intestinal barrier by disturbing the bacterial composition in the gut.

The first above-threshold resonance of 2-naphthoxide decays through vibrational mode specific autodetachment with a lifetime of 130 ± 10 fs. This state is not a doorway to stable interstellar anion formation.

Switchable catalysis is a useful one-pot method to prepare block polyesters utilising a single catalyst exposed to a mixture of monomers.

Process simulations allow the evaluation of the emissions and selling price for the production of the key monomer FDCA based on different feedstocks and solvent systems, alongside considerations of safety and current process development.

We report the synthesis of group 6 borylene complexes by the salt elimination method and study their borylene transfer capability to other transition metal fragments, providing new borylene complexes that are inaccessible by other routes.

Efficient polymerization catalyses transform bio-sourced monomers into thermoplastics with high elasticity and strength, which can be degraded to allow for chemical recycling. The plastics utilize carbon dioxide, limonene oxide and ε-decalactone.

Multi-state Pair-Density Functional Theory (MS-PDFT) gives the correct topology of interacting potential energy surfaces where state-specific calculations fail.

Lone pair Sb 5s orbitals are identified at the valence band maximum of Sb₂Se₃ bulk crystals using photoemission and density functional theory. The resulting band alignments are determined and implications for solar cell applications are discussed.

Functionalized plasmonic Ag nano-assemblies moving in a living cell were employed to visualize the spatiotemporal change of intracellular pH by surface-enhanced Raman scattering.

Pyrazole-based polyamines stabilise G-quartet based GMP hydrogels at human skin pH and GMP concentrations one order of magnitude lower than typically employed, allowing in some cases drug encapsulation without disrupting the hydrogel structure.

Characterisation of the external surface of bacteriophage M13 using PVIII protein structural data and measuring ζ-potential of the entire virus.

Structure–property–activity relationships in solution processable polymer photocatalysts for hydrogen production from water were probed by varying the chemical structure of both the polymer side-chains and the polymer backbone.

A ternary heterostructure Ru/RuO₂/g-C₃N₄ was designed for ammonia photosynthesis under visible light irradiation, which exhibited 6 times higher activity with excellent stability than the pristine g-C₃N₄.

Doped-ZnO nanoparticles, capped with dioctylphosphinate ligands, are synthesised by the controlled hydrolysis of a mixture of organometallic precursors.

This paper reports a SAMDI-mass spectrometry assay that can evaluate antagonists of cancer-associated isocitrate dehydrogenase 1 in high throughput.

A facile ambient environment solution approach to prepare γ-CsPbI_3−xBr_x is reported for the first time, leading to samples that exhibit vastly improved stability towards both moisture and heating in air.

This investigation examines the reactivity of phosphinoboronate esters Ph₂PBpin (pin = 1,2-O₂C₂Me₄) and Ph₂PBcat (cat = 1,2-O₂C₆H₄), as well as other phosphinoboron species, with various aryl and aliphatic acyl chlorides.

Understanding the trophic transfer and biomagnification potential of nanomaterials in aquatic food chains is crucial for assessing the environmental risks of such materials.

Calcium complexes of cyclic oligocarboxylic acids have been studied as models to understand how subtle changes in molecular structure lead to significant variation in inhibition ability for calcium carbonate deposition

A hydrogen-bonded organic framework is an effective photocatalyst for producing hydrogen from water. Its crystal structure is key to its activity; a chemically identical, amorphous version is almost inactive, as rationalized by crystal structure prediction.

A novel, rapid and sensitive analytical method has been developed and applied to 105 sputum samples from patients with cystic fibrosis, including 5 samples from post-lung transplant patients.

Photolysis of trypto-CORM results in ultra-fast CO-dissociation and formation of a 16-e triplet followed by solvation.

Polymer-supported metal catalysts are used for the heterogeneous polymerisation of renewable lactones, towards the efficient and environmentally benign production of sustainable polymers.

This proof-of-principle study demonstrates the feasibility of a leaky waveguide (LW) aptasensor, where aptamers were immobilised in a mesoporous chitosan waveguiding film for the detection of thrombin.