Themed collection 2024 Chemical Science HOT Article Collection

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 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.

The construction of a quadrane scaffold by β-terrecyclene synthase via Coates' route is demonstrated through mutagenesis and isotopically sensitive branching studies. Subsequent enzymatic modifications convert β-terrecyclene into terrecyclic acid.

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

A DNA nanocomplex with cascade DNAzymes, promoter-like ZnO₂–Mn nanozymes and intercalated photosensitizers was designed to synergistically disrupt autophagy and relieve tumor hypoxia for efficient pyroptosis therapy.

The first stable linear 2-stannapropadiene has been synthesized. The inert-pair effect favors Sn²⁺, but silyl substituents can counter it, enabling the isolation of 2-stannapropadiene with a Sn⁴⁺.

We show that weaker acid catalysis has profound effects on the dynamicity of vinylogous urethane based polymer networks. Moreover, the dynamicity could be adjusted by changing electronic and steric parameters in the catalytic environment.

If a critical acetylene surface coverage threshold above one monolayer is attained, acetylene conversion to benzene occurs with 100% selectivity on Ag(111). The presence of multiple monolayers has the unforeseen effect of increasing benzene production while maintaining selectivity.

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.

Triplet excited states play a pivotal role in photosensitizers. Detailed simulations reveal how these states are formed efficiently in heavy-atom free systems.

A novel strategy is herein introduced which utilizes azole additives to activate the weak acyl donor peptidyl N-acyl pyrazole, and thereby enables its direct ligation to an N-terminal cysteine peptide for efficient chemical protein synthesis.

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.

Surface-enhanced Raman scattering was used to resolve the chemical species, including chloride ions, on the surface of Ag nanocrystals in their original reaction solution, avoiding changes to the surface while eliminating possible artifacts.

We synthesized a series of naphthobisthiadiazole-polymers by systematically introducing the alkyl, ester, and fluorine groups in the quaterthiophene co-unit and studied the effect of noncovalent interactions on physical and photovoltaic properties.

Efficiently merging low-cost high-throughput screening and characterisation, automated data analysis, computational modelling, and cagey – a custom database analysis tool, enhances large-scale data curation and accelerates discovery of organic cages.

NIR phosphorescent Cu–Pt bimetallic clusters have been synthesized with solid-state quantum yield (QY) of up to 36.7%. Ligand effects enhances emission intensity and modulates emission wavelength via intra- and inter-molecular interactions.

To understand the solvation environment at the air–water interface, we use an azide vibrational reporter. The probe is sensitive to hydrogen bonding and electrostatics of the interface.

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.

An automated solid-phase synthesis route has been developed to rapidly synthesise recognition-encoded melamine oligomer sequences up to 42 monomer units long in remarkably high yield and excellent crude purity.

Cyclopropyl-substituted sulfonium salts are obtained by Rh-catalysed addition of α-diazo dibenzothiophenium salts to olefins. When indenes are used as substrates, initially formed cyclopropyl rings open with concomitant elimination of dibenzothiophene, enabling access to 2-substituted naphthalenes.

Unnatural α-amino acids bearing carbazole side-chains have been shown to be effective structural mimics of tryptophan in peptides and valuable fluorescent probes for the analysis of protein–protein interactions.

A series of synthetic pseudaminic acid analogues bearing different N5/N7 substitutions were transformed enzymatically into corresponding CMP-Pse species via PseF catalysis, which demonstrated the substrate promiscuity of PseF.

Single-crystalline 2D covalent organic frameworks were synthesized in flow with laboratory scale rates of more than 1 g h⁻¹.

The hydrogenation of CO₂ to formic acid is catalyzed for the first time by a Pd²⁺ catalyst, Pd–V/AC–air. The superiority of Pd²⁺ over Pd⁰ is confirmed by a combination of DFT and experimental results.

The Curtin–Hammett principle is used to understand the diastereoselective synthesis of a heterochiral over a homochiral macrocycle, both of which are configurationally stable chiral macrocycles.

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

Solid supramolecular phosphorescence between glycoluril derivatives and polyvinyl alcohol exhibited a green afterglow with a lifetime of 2.12 s, and a self-crimping configuration endows them with ability to encapsulate guests to achieve TS-FRET.

N–N bond formation in octahedral, terminal d¹ Mo(V) nitridos to give μ-dinitrogen complexes requires one eletron oxidation with 0.5 equivalents of oxidant to open a kinetically feasible ambiphilic nitrido coupling pathway.

A highly enantioselective [4 + 2] cycloaddition of a number of simple olefins with cyclic hetero-diene of dioxopyrrolidines is realized by a chiral iron(III)/N,N′-dioxide complex catalyst.

A deep blue TADF emitter composed of rigid D and A units was developed. BOC-PSi-based OLED exhibited not only an impressive EQE_max approaching 20%, but also a superior color purity approaching the Rec.2020 blue standard.

Simulations reveal that both charge and exciton delocalisation can significantly improve the efficiency of charge generation in organic photovoltaics and explain the failure of classical hopping approaches.

The extremely challenging deprotonation of the amine (tBu₃Si)₂NH led to a range of s-block metal complexes with superbulky (tBu₃Si)₂N⁻. Depending on metal and solvent, (tBu₃Si)₂N⁻ can be classified as a halogen-free weakly coordinating anion.

A halide-free route to the synthesis of graphitic BC₃ was discovered via decomposition temperature matching: benzene (C₆H₆) as the carbon precursor and the borohydride anion (BH₄⁻) as the boron precursor.

NMR crystallography exposes preferential site ordering of Al and Ga in new mixed-metal phosphate frameworks.

Novel freestanding M-PtBiMo IMSs were achieved via a simple and effective one-step wet chemical method. The M-PtBiMo IMSs as highly efficient anode electrocatalysts boosted the activity and stability toward the EGOR and actual DEGFCs.

In situ regulation of π–π coupling was realized with the combination of rigid intramolecular dimer models and external stimuli, mainly due to the balance of π–π and solvent–π interactions. The results establish the quantitative relationship between emission properties and π–π distances.

We designed a covalent organic framework (TA-PTO-COF) as a dual-active-center cathode. This work presents a promising organic cathode material for a high-performance aqueous zinc-ion battery.

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.

To accelerate the discovery of novel metalloantibiotics we applied combinatorial synthesis to the preparation of 420 novel manganese tricarbonyl complexes.

The utilization of multi-site modifications brings about the manipulation of excited-state processes and multi-stimuli responses of salicylaldehyde Schiff base isomers, which can be successfully applied in multi-level decryption.

An organocatalyzed asymmetric synthesis of C_sp2–N atropisomers by formal C_sp2–O amination has been established from 3-alkynyl-3-hydroxyisoindolinones and 1-methylnaphthalen-2-ols.

A SERS imaging strategy is developed to quantitatively visualize the protein-specific glycan oxidation mediated pathogen–cell interactions and pathogen-resistance mechanisms.

An unprecedented rare-earth ethyne complex is presented, and the α-H abstraction and C–C σ bond metathesis mechanism is proposed based on DFT calculations. The first example of a well-defined non-Cp rare-earth ethylene complex via the β-H abstraction reaction is also described herein.

Silylation of iron-alkyl-dinitrogen complexes gives high-spin iron(IV) products that also have an iron(II) resonance structure. The stability and reactivity of these compounds depends on the alkyl group, with insertion and homolysis observed.

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

Jahn–Teller (JT) distorted Cu^II-containing compounds often display interesting structural and functional behaviour upon compression.

Despite theoretical difficulties, we herein for the first time demonstrate an effective concept for the synthesis of an orange-red multiple resonance (MR) emitter centered on a pyridine ring via stereo effects.

Pentacoordinated Al³⁺-enriched Al₂O₃ containing abundant frustrated Lewis pairs activates H₂ through a heterolytic mechanism and effectively catalyzes the hydrogenation of unsaturated bonds (CC, CC and CO) through a stepwise process.

PoseBusters assesses molecular poses using steric and energetic criteria. We find that classical protein-ligand docking tools currently still outperform deep learning-based methods.

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.

Lewis-basic oxygen and sulfur heteroatoms are introduced to novel asymmetric self-assembled monolayers, realizing enhanced packing, effectively adjusting ITO work function, and passivating buried interface in inverted perovskite solar cells.

Regulating the electrolyte hydrodynamics substantially reduces the proton diffusion length by 80%, which promotes the recovery of carbonate and leads to enhanced single-pass utilization of CO₂ in mild acidic electrolyte.

Pd_n clusters offer unique selectivity and exploitable reactivity in catalysis. Tethering Pd₃ clusters to a resin unlocks compelling new insight into the speciation of Pd during catalytic turnover for Suzuki–Miyaura cross-couplings.

By using resonance Raman spectroscopy and temperature-dependent pulse EPR spectroscopy, we show that bond stretching vibrational modes > 200 cm⁻¹ drive spin relaxation in planar and ruffled copper porphyrins.

An NHC-stabilized heavier nitrile ylide activates white phosphorus, undergoing inorganic Huisgen-type [3 + 2] cycloaddition to form a unique heterocycle with four heteroatoms from groups 14, 15, and 16.

Improving the efficiency of photocleavable protecting groups is crucial for their application. Here we reveal how the fate of the contact ion pair intermediate plays a key role in defining this efficiency.

From a single N-confused dithiahexaphyrin ligand, five mono- and bis-Pd(II) complexes have been synthesized, and the absorption and aromaticity can be modulated by Pd(II) coordination, macrocycle contraction and ancillary ligands.

The stereoselective synthesis of alkylboronic esters from vinyl iodides and various nucleophiles, alkenes or alkynes is presented. Reactions proceed through hydroborations and 1,2-metallate rearrangements without any transition metal catalyst.

Our self-evolving graph neural networks for predicting solubilities reconciled different magnitudes of errors and uncertainties of experimental and computational databases, maximizing the database size and the model’s prediction accuracy.