Themed collection Chemical Communications HOT Articles 2022

In this feature article, we focus on recent progress on MOF-based memristors and their switching mechanisms. In addition, challenges as well as future perspectives are discussed.

By carefully controlling the reactants and precisely probing the products, we can gain insights into how radical reactions occur on a fundamental level.

A highlight of recent synthetic methods for selective deuteration of organic molecules using electrochemistry.

Electrocatalytic nitrite reduction is of great significance for wastewater treatment and value-added chemicals synthesis.

The highlight describes the emerging trend in the C–F functionalization area: recent progress in the single-electron-transfer initiated selective defluorinative functionalizations of C_sp³–F bonds in multifluorinated compounds via radical pathways.

NMR spectroscopy is a powerful approach for the analysis of mixtures. This feature article describes a selection of methods that aim to address the complexity, the low concentrations, and the changing nature that mixtures can display.

Improved stability and higher degree of synthetic tunability has allowed N-heterocyclic carbenes to supplant thiols as ligands for gold surface functionalization.  This review article summarizes the basic science and applications of NHCs on gold.

The development and application of the de novo asymmetric synthesis of oligosaccharides from achiral starting materials using the Achmatowicz reaction is reviewed.

Ligand-ligated Ni–Al bimetallic catalysis not only affects electronic and steric property of substrates, but also produces strong directing effect for facile control of reactivity and selectivity in the activation of C–H and C–C bonds.

This feature article presents the electrolyte synthetic approaches, design strategies, and merging materials that may address the critical issues of solid electrolytes for solid-state Li/Na–metal batteries.

In this Feature Article, we analyze how a minimal cell cycle of growth, replication of genetic information and division could be realized in coacervate protocells. This would allow such primitive cells to undergo evolution at the origins of life.

This article reviews the recent progress in the use of metal–organic frameworks as solid absorbents for hydrogen storage, and their current challenges and future prospects.

This work elaborates on a suite of bioinformatics solutions developed in the Huan lab to address big-data challenges in metabolomics.

The designed strategies for producing MOF-derived porous materials with preserved characters (framework skeletons, surface areas, porosity and properties) and improved stability are outlined.

Single molecule force-spectroscopy techniques provide access to unprecedented molecular-scale details about biochemical and biological mechanisms.

Conjugated polymer (CP) microstructure plays a crucial role in determining the characteristics of a target device. Here, we provide an overview of the key aspects of the CP microstructure-property relationship carried out in our group.

Molecular polymer bottlebrushes offer a comprehensive toolbox for nanomaterials design. Their tuneable and multifunctional architecture has accelerated their use in nano-bio research and nanomedicine applications.

Inspired by the design and performance of biological pores, polymer functionalization of nanopores has emerged as an evolving field to advance transport performance within the last few years.

The treatment of electronic resonances in terms of complex-valued energies is discussed with a focus on recent methodological developments.

Understanding biological interactions at a molecular-level grants valuable information relevant to improving medical treatments and outcomes.

This Feature article presents recent representative applications of the combination of the Activation Strain Model of reactivity and the Energy Decomposition Analysis methods to understand the reactivity of Frustrated Lewis Pairs (FLPs).

Self-assembly of oligo-(p-phenyleneethynylenes) (OPEs), a class of π-conjugated systems, into versatile materials has widened the application horizon of this molecular system with properties ranging from opto-electronics and energy to biology.

Ionic liquids and their siblings deep eutectic solvents offer a unique combinatorial toolbox enabling deliberate nanosynthesis like no other solvents.

Metal–organic cages are macrocyclic structures that can possess an intrinsic void for application in encapsulation, sensing and catalysis. In this article, we highlight approaches and limitations to their computational design.

The recent developments of sustainable catalytic reactions catalyzed by fluxional acridine-based PNP pincer complexes are explored, focusing on their unique structural features and reactivities compared to other traditional pincer complexes.

This feature article gives guidelines to construct molecular crystal-based organic photonic integrated circuits (OPICs) using mechanical micromanipulation with atomic force microscopy tips.

In this feature article, the photolysis and dye-sensitized reactions of diazoalkanes are discussed and applications in organic synthesis are presented.

Combinational photoimmunotherapy (PIT) is considered to be an ideal strategy for the treatment of malignant cancer, because it can ablate the primary tumor and induce the host immune response to control tumor growth and distal metastasis.

Precise surface control of cathode materials for stable Li-ion batteries: materials design, kinetics control and stabilization mechanism.

A perovskite layer functionalized to be an outermost screen can strongly affect the capacity of the underlying device to avoid becoming decomposed under external stimuli, and subsequently affect the photovoltaic performance as well.

Small molecule-based cross-catalytic system that operates using principles of organocatalysis.

Understanding of the energy/charge transfer processes in Mn–CsPbBr₃ NPLs is achieved using temperature-dependent femtosecond TA spectroscopy. Charge transfer process which is efficient at 300 K is seen to be inhibited at 5 K.

A novel ‘AND’-based ratiometric fluorescence probe for the sequential detection of biothiols and hypochlorous acid was developed, which exhibits fast response time and good selectivity in living cells.

The amphiphilic nanostructures of ionic liquids were found to have opposing effects on the rate of dehydration of secondary alcohols in the presence and absence of an added acid catalyst.

Co/N-doped carbon nanospheres act as a superb catalyst for ambient NH₃ synthesis via electrochemical NO₃⁻ reduction, attaining a large NH₃ yield of 758.0 μmol h⁻¹ mg_cat.⁻¹ and a high faradaic efficiency of up to 96.5%.

A binary Ag–Zn alloy interface is designed to efficiently enhance the structural stability in keeping the high Li affinity of the alloy structure, and exhibits a great Li protective ability for a stable and durable Li metal anode.

An intramolecular P/Al-based FLP with a biphenylene scaffold is synthesized by a convenient Al-Sn exchange. Despite the spacer the FLP functions interact leading to a strained compound, capable of CO₂ binding and unprecedented allene activation.

Supramolecular heteromultivalent sensor arrays were constructed by coassembling different amphiphilic calixarenes and cyclodextrin, and applied in cell identification.

A mild silver-catalysed oxidative C–H alkylation of N-heteroarenes is developed, utilizing aliphatic ketone-derived 2,3-dihydroquinazolinones as an alkyl radical reservoir.

The replacement of an ethyl by a benzyl substituent in N-methyl-pseudoephedrine-derived chiral SDAs brings an astonishing inversion of chirality in the resulting -ITV zeolite framework, also leading to an increase of the enantioselective properties.

Pillar[5]arene-functionalized rhodium nanoparticles are prepared for catalytic reduction of toxic nitrophenols and azo dyes and efficient photothermal sterilization.

A systematic exploration of the potential energy surface reveals two global minima with three planar tetra coordinate carbons (ptCs) and two global minima with three quasi-ptCs for E₆C₁₅ (E = Si–Pb) combinations.

The absolute configuration of a clinically important drug candidate, SMTP-7, with only micron-sized powders available, is directly obtained via microcrystal electron diffraction (MicroED) analysis.

The dynamics of alkyne → copper(I) interactions has been determined and used to self-assemble a fast nanorotor, which underwent a self-catalyzed click transformation to a triazole rotor, an interesting process for the production of biohybrid devices.

Here we show using mass photometry how proline substitutions, commonly used for SARS-CoV-2 spike stabilisation in vaccine design, directly affects ACE2 receptor interactions via dynamics of open and closed states.

A rare redox-active Mn(0) dicarbene anion with solvent-dependent electrochemical behaviour has been synthesized and thoroughly characterized.

We developed a hierarchically mesoporous metal–organic framework nanozyme with enhanced alkaline phosphatase-mimicking activity for rapid and sensitive sensing of phosphorylated biomarkers.

Potassium reduction of a bulky diamido-calcium complex under an N₂ atmosphere afforded the first well-defined, hetero-bimetallic s-block metal complex of activated dinitrogen.

Redox-assisted Disulfide Direct Conjugation (RDDC) allows for disulfide functionalization under mild aqueous conditions without prior reduction.

A one-pot two-step fashion for the synthesis of 3-trifluoromethyl-1,4-benzoxazines from CF₃-imidoyl sulfoxonium ylides and 2-bromophenols via lithium-bromide-promoted O–H insertion of sulfoxonium ylides and annulation has been demonstrated.

Exclusive formation of an integratively sorted tetrahedral complex enables incorporating a unique vertex.

We exploit halogen effects to tune metal–metal interactions, nucleation pathways and hetero-seeded growth in supramolecular copolymerizations.

Covalent organic frameworks (COFs) have enormous potential in various applications because of their high crystallinity and superior surface area.

An eight-coordinate zirconium complex shows dual emission from ligand-to-metal excited states with long photoluminescence lifetime.

A neutral and mononuclear niobium nitride complex (PNP)NbN(N[^tBu]Ar) (PNP⁻ = N[2-PⁱPr₂-4-methylphenyl]₂) can be isolated using the redox-active properties of the [PNP]⁻ ligand.

Pyrithione exhibits size-selective dimerization across the f-block. Experimental and computational analysis shows the Am complex contains greater covalency compared to the Nd analog.

A Ru/NH₂-MCM-41 catalyst was prepared via a coordination-assisted strategy for highly chemoselective hydrogenation of dimethyl oxalate to methyl glycolate (ca. 100%) and ethylene glycol (>90%) at low reaction temperature (343–433 K).

The supporting material with an optimal structure not only changes the growth behavior but also tunes the electronic structure of the catalyst.

Monodispersed hypermodified polymers based on DNA scaffold displaying four different functional groups were synthesized through DNA polymerase catalyzed reverse transcription from RNA templates followed by RNase digestion.

Reductive silylation of the uranyl dication with 1,4-bis(trimethylsilyl)dihydropyrazine, or “Mashima's reagent”, is detailed.

A host–guest system is constructed using quaternary ammonium salts as the hosts. It is the guest-activated hosts that emit room temperature phosphorescence, rather than the host-assisted guests in traditional doped systems.

FeTe₂@GO as a cathode for aluminum-ion batteries displays long-term cycling stability (10 000 cycles) at 1 A g⁻¹, and a mechanism involving multiple cationic and anionic redox reaction was elucidated.

Aldehyde and ketone hydrosilylation turnover frequencies of up to 330 s⁻¹ have been achieved using a phosphine-substituted aryl diimine cobalt catalyst.

A series of porous, heteroleptic, rhodium-based trigonal antiprismatic metal–organic polyhedral was assembled, from which both possible isomers were identified via screening of complementary linkers.

A free-standing multilayer book-like organic based electrode was prepared, presenting high conductivity and excellent flexibility, thereby achieving outstanding performance for flexible lithium-ion batteries and sodium-ion batteries.

A general method of iron-catalyzed deconstructive alkylation of alcohols with olefins through chlorine radical induced C–C single bond cleavage is developed.

An electron counting rule for borophenes based on graphene and MgB₂ helps to design metallated borophenes and borophanes, and suggests strategies to release 2D-borophenes from metal surfaces.

The process for the direct oxidation of methane to methanol is investigated on single atom alloys using density functional theory.

The cubic SBU Ni₈X₆L₆ (X = OH⁻/H₂O, L = ligand) in MOFs has so far been described as neutral in the literature. We investigated by detailed DRIFTS measurements and exchange reactions whether it shows anionic character, as observed in complexes.

A yolk–shell nanostructure with lithiophilic Sn–Co nano-seeds and a N-doped carbon shell is proposed to stabilize lithium nucleation and deposition.