Themed collection 2024 Chemical Science HOT Article Collection

The development of transition metal-catalyzed [(2+2)+1] and [(2+2)+2] carbocyclization reactions of 1,6-enynes bearing 1,1-disubstituted olefins is discussed, highlighting both the challenges and opportunities for expanding this powerful transformation.

Catalysts consisting of isolated metal atoms bonded to solid supports have drawn wide attention by researchers, with recent work emphasizing noble metals on metal oxide and zeolite supports.

O₂ is an attractive oxidant but it is also kinetically inert which limits its use in synthetic transformations. Metal–ligand cooperativity is a promising biomimetic strategy to activate O₂ for oxidative reactivity and catalysis.

Over the years, spectroscopic, electrochemical and structural studies of [FeFe] hydrogenases have provided ‘pieces’ of information to complete the ‘puzzle’ of their catalytic cycle. However, there are still missing pieces that we need to fill in.

An overview of the recent advances in the photoinduced construction of axially chiral compounds was presented.

Photoswitching via indirect excitation allows harnessing low-energy photons to control molecular configuration. Herein, the state of the art of the predominant indirect photoswitching methods is presented.

This perspective highlights the challenges and opportunities in achieving sustainable plastic recycling under mild conditions by imitating the active sites and the substrate-binding clefts of enzymes.

An overview of PVC functionalization through the lens of chemical recycling.

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.

Combining organic crystals and polymers results in a new class of all-organic, lightweight, flexible materials with unprecedented mechanical robustness, resilience, and diversity in combination with other functional materials.

Recent synthetic approaches for AIEzymes and their diverse applications in tumor imaging and therapy, anti-biofilm and antibacterial, food safety analysis, and environmental pollutant monitoring.

This review critically discusses recent in situ and operando studies on Fe-based catalysts in CO₂ hydrogenation, in particular focusing on the effect of composition, promoters, support and particle size.

The study discussed how MOFs treat microplastics, how to make plastic-based MOFs, and how MOF@plastic composites can be used. It aids in understanding how to convert plastic/microplastic concerns into opportunities for high-valued products.

The application of hydrogel-based flexible strain sensors in harsh environments, including extreme temperatures, humidity, high mechanical strain, and strong corrosion, is investigated.

Recent progresses in Cu–oxygen adducts towards recalcitrant C–H activation are reviewed with focus on Cu metalloenzymes and bioinspired synthetic models, mono- to polynuclear complexes, working under homogeneous and heterogeneous catalytic conditions.

Adamantane-type clusters exhibit a huge diversity of chemical compositions, structural details, and resulting properties.

Recent progress of preparation approaches for HCs is systematically overviewed, with a special focus on the comparison between traditional fabrication methods and advanced strategies regarding their influence on performance.

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.

In response to societal developments and the growing demand for high-energy-density battery systems, alkali metal batteries (AMBs) have emerged as promising candidates for next-generation energy storage.

This work revealed the dual beneficial roles of potassium, acting as a self-template to create pore channels and balancing the degree of graphitization.

We propose a method of Zn₂(OH)₂CO₃ assisted ball milling combined with subsequent carbonization to generate closed pores in coal derived hard carbon, leading to a high capacity of 325.3 mA h g⁻¹ (plateau capacity accounting for 45.1%).

We present a hybrid quantum-classical approach that combines quantum and classical hardware to simulate the excited state dynamics of molecules.

Deuteration suppresses the weakly temperature dependent internal conversion (IC) and turns dibenzoterrylene molecules into bright single photon emitters, in agreement with the predictions of the well-known energy-gap law.

Engineered metalloproteins that mimic the active sites of natural copper metalloenzymes are used to systematically investigate the influence of aromatic residues within the secondary coordination sphere on reactivity.

SynAsk is a chemistry-specific LLM platform, fine-tuned with domain data and integrated with in-house tools. It supports tasks like reaction prediction, retrosynthesis, and literature retrieval, advancing organic synthesis research.

Protein–protein interactions (PPIs) drive numerous diseases. We present a new way to inhibit PPIs using high-throughput automated selection of sequence-defined polyphosphoesters, taking the oncogenic mutant KRAS/RAF interaction as a model.

Our generative AI model designs copolymers taking their complex hierarchical structure into account. We design the monomer chemistries, stoichiometric ratios, and chain architecture together, and optimise towards a desired property portfolio.

Dithienoarsinines, the first π-extended arsabenzenes, exhibit high stability and planarity. Their structure, optical/electronic properties, reactivity, and coordination behavior are comprehensively studied, highlighting the features of arsenic.

For sodium-ion batteries, solving the issue of short cycle life is key to their large-scale adoption in the industry, and the electrolyte plays an important role on this.

The accuracy of wave function and DFT methods for spin-state energetics benchmarked against curated experimental data of transition metal complexes.

Halting weed growth through herbistasis is not a well-known phenomenon, but it could offer a new avenue for weed control. A bioisosteric cyclooctatetraene for phenyl ring replacement tactic has unearthed a rare herbistatic against rubber vine.

We introduce 3DSMILES-GPT, a token-based large language model for 3D molecular generation that integrates 2D and 3D molecular data.

Sub-m-benziporphyrins, nonaromatic and aromatic B^III complexes were synthesized.

The kinetics of Li₂O₂ dissolution determine electrode discharge capacity and charging current. It dissolves via surface dissolution or bulk fragmentation, the latter being 100 times faster. Intermittent-desorption improved the discharge capacity.

We show that fluorobenzene-bound dicationic lanthanide complexes containing a single anionic ligand can show interesting single-molecule magnet properties, and can be useful starting materials to heteroleptic complexes containing bulky ligands.

A unimolecular three-helix bundle aromatic foldamer in which each helix interacts with the two others was designed by stepwise transformation of a parallel trimolecular three-helix bundle.

We fabricated different glass structures of a one-dimensional coordination polymer with/without the application of mechanical forces during the melt-quenching process. Under the shear, the glass has an oriented, anisotropic structure.

Water microbubbles containing Fe²⁺ ions have been found to efficiently transform nitrogen (N₂) to nitrate (NO₃⁻) by initiating Fenton's reaction at the gas–water interface.

Gem-difluorinated alkoxyphenyl group conformational and DMPK properties modulation experimentally demonstrated in a macrocyclic system.

The reactivity of a [V^V] alkylidyne with unsaturated substrates such as NCR (R = Ad or Ph) and PCAd leads to the formation of rare transition metal complexes featuring an α-aza-vanadacyclobutadiene and a β-phospha-vanadacyclobutadiene moieties.

Enzyme-mediated synthesis using one or a combination of two substrates produced biocombinatorial mixtures of multimeric linear and macrocyclic hydroxamic acid chelators. Screening the pools with Ga(III) or Zr(IV) revealed new coordination chemistry..

Copper accumulated-cuproptosis has been extensively investigated, copper depleted-cuproptosis remains largely unexplored. Based on the solubility product principle, a novel copper depletion-induced tumor cuproptosis strategy was developed.

Maier and Schleyer first identified in silico that certain cage bicyclic olefins (alkenes) as “hyperstable”, and predicted them to be “remarkably unreactive”. However, this only applies to hydrogenation, as they were observed to undergo oxidation.

Understanding the Pt/ionomer/water interface structure and its impact on the oxygen reduction reaction activity is essential for enhancing catalyst utilization and performance of fuel cells.

We propose a strategy for the hydrogenolysis of furan rings using PtFe_x/LDH catalysts. Mechanism studies reveal that the hydride attacks the carbon atom of the Csp²–O bond, initiating an S_N2 reaction that results in ring-opening products formation.

Two nanometer-sized, nitrogen-containing molecular cylinders were synthesized by connecting the cycloparaphenylene and fused aromatic moieties using cyclocondensation reaction.

The first structural evidence of extremely unstable Cl⋯O halogen bonds formed by dichlorine and pyridine N-oxide has been successfully characterized by X-ray diffraction analysis.

Cancer immuno-profiling: The combination of bioorthogonal chemistry and LC-MS/MS-analysis was successfully used for imaging and quantifying overexpressed cancer receptors in cells, tissues and in vivo.

Chiral ionic organic single-crystal (CIOC) were prepared for the first time via ionic self-assembly using organic anions and cations. Interestingly, the CIOC can be ultrasonically exfoliated to 2D nanosheets and exhibit enhanced enantioseparation.

An ultrathin polymer electrolyte with superior ionic conductivity and stable electrolyte/electrode interfaces enables a high-loading Li/NCM811 cell with a capacity retention of up to 71% after 400 cycles at a high cut-off voltage of 4.5 V.

We proposed the ‘Fragment Complementary Activation Strategy’ (FCAS) based on the CRISPR/Cas12a system and designed fragment activators consisting of ssDNA and miRNA targets, enabling the direct detection of miRNAs.

We report the first non-d⁰ Re(V) alkylidyne complex capable of effecting alkyne metathesis at room temperature, featuring air/moisture stability, broad functional group compatibility, and scalable synthesis.

Exciton dynamics modulated by long-range charge transfer and heavy-atom effects are systematically investigated via diversiform donors for multiple resonance compounds, and thus high-efficiency narrowband solution-processed OLEDs can be achieved.

A structural constraint approach at a P–P bond is presented that enables the phosphinophosphination of alkynes, alkenes, and carbonyls with high regio- and diastereoselectivity. The apolar nature of the P–P bond facilitates a concerted mechanism.

Leveraging multimodal large language models (MLLMs) to process multimodal data inputs and complex inter-modality data dependencies for automated (electro)chemical data mining from scientific literature.

Herein, we report boron-centered reductive elimination reactions to afford cyclic(alkyl)(amino) carbene (CAAC)-ligated chloroborylene and bromoborylene.

Frustration and dynamic disorder give rugged free energy surface in spin-crossover materials, driving complex relaxation dynamics of trapped spin-states including; exponential, sigmoidal, stretched exponential, multi-modal, and multistep relaxation.

Pseudomonas from Enigma Lake (Antarctica) has a peculiar lipopolysaccharide with an unusual tendency of decreasing lipid A secondary hydroxylation. This results in increased membrane fluidity that ensures bacterial survival at near-zero temperature.

Porous interlayers in 2D metal-halide perovskites enable new modes of reactivity. These include permanent intercalation of redox-active molecules as well as post-synthetic halide-to-halide and halide-to-pseudohalide exchange.

The direct conversion of esters to imines or enamines is achieved using zirconocene hydride (ZrH) catalysis. This transformation occurs through an amine-interrupted reduction, bypassing traditional pathways leading to alcohol products.

Facile and scale-up fabrication of enzyme-loaded mesoporous hydrogen-bonded organic frameworks as efficient biocatalysts is achieved.

The template complex of a zinc porphyrin nanoring forms several pseudopolymorphs featuring different conformations of the π-system. The metal-free nanoring is even more flexible, and adopts an elliptical geometry when co-crystallized with C₆₀.

Phenylene urea, used as an aglet at the N-terminus, facilitates self-assembly. Simple dipeptides with phenylene urea assembled to form autofluorescent polygonal peptide tubes, while bis-urea pseudopeptides formed autofluorescent spherical vesicles.

Helically chiral MR-TADF compounds tBuPh-BN and DPA-tBuPh-BN show narrowband circularly polarized luminescence that translates into high-performance hyperfluorescent organic light-emitting diodes.

The acidic redox-assisted deposition (ARD) of cobalt manganese oxyhydroxides (CMOH) as a solid-state inorganic binder has been demonstrated. CMOH is stable and highly adhesive under high oxidative currents during OER tests.

This study demonstrates β-diketonate ligands' non-innocence in Mo-complexes, stabilizing Mo(II) and Mo(I) complexes, enabling differentiated reactivities toward CO₂ and CS₂.

After a hundred years of waiting, the use of binary heterogroups has succeeded in making an inverted Keggin ion lacunary, the enclosed Mo–oxo framework has been opened up with enhanced Lewis-acid–base catalytic activity.

In this work, molecular dynamics simulation with metadynamics is performed to understand the relationship between lanthanide ion solvation energetics and separation performance.

Combining dimer pair calculations and coarse-grained modelling to predict the solid-state phase behaviour of porous organic cages and build design principles for introducing chirality into achiral cages.

An antiaromatic buckybowl and two doubly curved nanocarbons by fusion of nonbenzenoid rings onto pyrene have been synthesized and characterized.