Themed collection 2022 ChemSci Pick of the Week Collection
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Chemistry must respond to the crisis of transgression of planetary boundaries
Chemistry, the science of transformation of matter, is fundamental to achieving sustainability through ensuring biogeochemical flows do not transgress planetary boundaries. This requires urgent changes in chemistry education, research and industry.
Chem. Sci., 2022,13, 11710-11720
https://doi.org/10.1039/D2SC03603G
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Umpolung strategies for the functionalization of peptides and proteins
This perspective highlights the growing body of literature that leverages polarity reversal (umpolung reactivity) for the selective modification of proteinogenic functionalities and identifies opportunities for further innovation.
Chem. Sci., 2022,13, 2809-2823
https://doi.org/10.1039/D1SC06133J
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Can super-resolution microscopy become a standard characterization technique for materials chemistry?
SRM, an advanced nanoscopy technique demands a transition from being a niche sophisticated technique to standard routine method for material characterization. The roadmap of necessary developments through multidisciplinary collaboration is discussed.
Chem. Sci., 2022,13, 2152-2166
https://doi.org/10.1039/D1SC05506B
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Stability matters, too – the thermodynamics of amyloid fibril formation
The thermodynamics of amyloid formation has largely been neglected compared to kinetic studies. In this review, the current state of the experimental exploration of amyloid thermodynamics is presented and important open questions are highlighted.
Chem. Sci., 2022,13, 10177-10192
https://doi.org/10.1039/D1SC06782F
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A carbapenem antibiotic inhibiting a mammalian serine protease: structure of the acylaminoacyl peptidase–meropenem complex
The structure of porcine AAP (pAAP) in a covalently bound complex with meropenem was determined by cryo-EM to 2.1 Å resolution, showing the mammalian serine-protease inhibited by a carbapenem antibiotic.
Chem. Sci., 2022,13, 14264-14276
https://doi.org/10.1039/D2SC05520A
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Coordination unsaturation of vanadium nitride quantum dots boosts low-temperature aerobic oxidation of thiophenic sulfides
Vanadium nitride quantum dots are immobilized on graphene to controllably create coordination-unsaturated edge/corner V sites for the efficient aerobic oxidation of thiophenic sulfides.
Chem. Sci., 2022,13, 14063-14069
https://doi.org/10.1039/D2SC05088A
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A photo-switchable molecular capsule: sequential photoinduced processes
The metastable trilacunary heteropolyoxomolybdate [PMo9O31(py)3]3−; py = pyridine) and the ditopic pyridyl bearing diarylethene (DAE) (C25H16N2F6S2) self-assemble via a facile ligand replacement methodology to yield the photo-active molecular capsule [(PMo9O31)2(DAE)3]6−.
Chem. Sci., 2022,13, 13732-13740
https://doi.org/10.1039/D2SC04613J
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Reassessment of N2 activation by low-valent Ti-amide complexes: a remarkable side-on bridged bis-N2 adduct is actually an arene adduct
The complex {(TMEDA)2Li}{[Ti(N(TMS)2)2]2(μ-η2:η2-N2)2} (5-Li) was the only transition metal N2 complex ever reported with two side-on N2 adducts. Reanalysis of 5-Li has revealed that it is an inverse-sandwich toluene adduct, not an N2 adduct.
Chem. Sci., 2022,13, 13330-13337
https://doi.org/10.1039/D2SC04368H
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Critical stresses in mechanochemical reactions
The rates of mechanochemical reactions are generally found to increase exponentially with applied stress.
Chem. Sci., 2022,13, 12651-12658
https://doi.org/10.1039/D2SC04000J
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Pattern enrichment analysis for phage selection of stapled peptide ligands
To effectively identify helical peptide binders from a phage library, we developed “pattern enrichment analysis,” which finds the enriched three-residue patterns by comparison with a control sample.
Chem. Sci., 2022,13, 12634-12642
https://doi.org/10.1039/D2SC04058A
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Precisely synthesized LiF-tipped CoF2-nanorod heterostructures improve energy storage capacities
A facile but robust method to precisely synthesize well-defined LiF-tipped CoF2-nanorod heterostructures is established.
Chem. Sci., 2022,13, 12367-12373
https://doi.org/10.1039/D2SC04008E
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Calculation of exchange couplings in the electronically excited state of molecular three-spin systems
We present a reliable methodology for the calculation of excited state exchange interactions in molecular three-spin systems. Such calculations will help to establish how to optimise inter-spin communication in photogenerated multi-spin systems.
Chem. Sci., 2022,13, 12358-12366
https://doi.org/10.1039/D2SC04701B
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End-to-end differentiable construction of molecular mechanics force fields
Graph neural network-based continuous embedding is used to replace a human expert-derived discrete atom typing scheme to parametrize accurate and extensible molecular mechanics force fields.
Chem. Sci., 2022,13, 12016-12033
https://doi.org/10.1039/D2SC02739A
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A fourteen-component high-entropy alloy@oxide bifunctional electrocatalyst with a record-low ΔE of 0.61 V for highly reversible Zn–air batteries
Nanostructured high-entropy materials such as alloys, oxides, etc., are attracting extensive attention because of their widely tunable surface electronic structure/catalytic activity through mixing different elements in one system.
Chem. Sci., 2022,13, 12056-12064
https://doi.org/10.1039/D2SC04461G
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Dynamic kinetic resolution of γ,γ-disubstituted indole 2-carboxaldehydes via NHC-Lewis acid cooperative catalysis for the synthesis of tetracyclic ε-lactones
NHC-Lewis acid cooperative catalyzed dynamic kinetic resolution (DKR) of transiently generated γ,γ-disubstituted indole 2-carboxaldehydes leading to the enantioselective synthesis of tetracyclic ε-lactones is reported.
Chem. Sci., 2022,13, 11513-11518
https://doi.org/10.1039/D2SC03745A
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Interrogating the thionium hydrogen bond as a noncovalent stereocontrolling interaction in chiral phosphate catalysis
Transferable selectivity profiles allow data from intermolecular reactions using iminium substrates to be applied to predict intramolecular reactions involving thioniums.
Chem. Sci., 2022,13, 11065-11073
https://doi.org/10.1039/D2SC02171D
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Discovery of novel drug-like antitubercular hits targeting the MEP pathway enzyme DXPS by strategic application of ligand-based virtual screening
We identified two drug-like antitubercular hits with submicromolar inhibition constants against the target 1-deoxy-D-xylulose-5-phosphate synthase (DXPS) with a new mode of action and promising activity against drug-resistant tuberculosis.
Chem. Sci., 2022,13, 10686-10698
https://doi.org/10.1039/D2SC02371G
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Accelerating the end-to-end production of cyclic phosphate monomers with modular flow chemistry
A semi-continuous flow platform allows the safer end-to-end production of cyclic phosphate monomers providing an easier access to polyphosphoesters and their applications.
Chem. Sci., 2022,13, 10699-10706
https://doi.org/10.1039/D2SC02891C
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Highly contorted superhelicene hits near-infrared circularly polarized luminescence
This twisted superhelicene employed its twists and loops to shine chiral emission into the NIR region. The proof of its promising applicability in optoelectronic devices is the analogous chiroptical properties obtained in solution and thin films.
Chem. Sci., 2022,13, 10267-10272
https://doi.org/10.1039/D2SC03452B
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Determination of the critical chain length for macromolecular crystallization using structurally flexible polyketones
Critical chain length dividing small-molecule crystallization from macromolecular crystallization was determined for discrete polyketones to be as short as pentamer.
Chem. Sci., 2022,13, 9848-9854
https://doi.org/10.1039/D2SC03083G
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Flexibility is the key to tuning the transport properties of fluorinated imide-based ionic liquids
The interplay of fluorination, flexibility, and mass affects the transport properties of imide ionic liquids. Here we show how the combination of experimental and theoretical techniques can disentangle such confounding variables.
Chem. Sci., 2022,13, 9176-9190
https://doi.org/10.1039/D2SC03074H
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Towards clustered carbonyl cations [M3(CO)14]2+ (M = Ru, Os): the need for innocent deelectronation
Trimeric M3(CO)12 (M = Ru, Os) reacts with typical inorganic oxidants to unwanted side products. Yet, the 9,10-dichlorooctafluoroanthracene radical cation deelectronates these under CO pressure to give the first homotrimetallic [M3(CO)14]2+ salts.
Chem. Sci., 2022,13, 9147-9158
https://doi.org/10.1039/D2SC02358J
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From a Möbius-aromatic interlocked Mn2B10H10 wheel to the metal-doped boranaphthalenes M2@B10H8 and M2B5 2D-sheets (M = Mn and Fe): a molecules to materials continuum using DFT studies
The design of (1) Möbius aromatic interlocked boron wheel Mn2B10H10, (2) Hückel aromatic boron analogs of naphthalene (M2@B10H8; M = Mn and Fe), and (3) metal boride monolayers (FeB5 and Fe2B5), creating a molecules to materials continuum.
Chem. Sci., 2022,13, 8968-8978
https://doi.org/10.1039/D2SC02244C
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Stereoselective peptide catalysis in complex environments – from river water to cell lysates
The reactivity, stereo-, and chemoselectivity of a tripeptide are so high that it catalyzes conjugate addition reactions with high stereoselectivity in complex compound mixtures—even in cell lysates.
Chem. Sci., 2022,13, 8963-8967
https://doi.org/10.1039/D2SC02044K
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Supramolecular encapsulation of redox-active monomers to enable free-radical polymerisation
Extended polymeric structures based on redox-active species are of great interest in emerging technologies related to energy conversion and storage.
Chem. Sci., 2022,13, 8791-8796
https://doi.org/10.1039/D2SC02072F
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Mesoporous sodium four-coordinate aluminosilicate nanoparticles modulate dendritic cell pyroptosis and activate innate and adaptive immunity
Na-IVAl-DMSN acts as both antigen carriers and modulators to “hyperactivate” dendritic cells (DCs) via potassium (K+) efflux dependent pyroptosis, eventually leading to enhanced adaptive and innate immunity.
Chem. Sci., 2022,13, 8507-8517
https://doi.org/10.1039/D1SC05319A
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Chain end-group selectivity using an organometallic Al(III)/K(I) ring-opening copolymerization catalyst delivers high molar mass, monodisperse polyesters
A heterodinuclear Al(III)/K(I) organometallic ring-opening copolymerization catalyst shows exceptional rates, end-group selectivity and good loading tolerance to deliver monodisperse polyesters with molar masses up to 91 kg mol−1.
Chem. Sci., 2022,13, 8543-8549
https://doi.org/10.1039/D2SC02752F
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Expanding the hydride chemistry: antiperovskites A3MO4H (A = Rb, Cs; M = Mo, W) introducing the transition oxometalate hydrides
The synthesis, structures and electronic properties of the first four heteroanionic compounds containing both hydride and transition oxometalate ions are reported.
Chem. Sci., 2022,13, 7773-7779
https://doi.org/10.1039/D2SC01861F
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In situ lattice tuning of quasi-single-crystal surfaces for continuous electrochemical modulation
We reported a new method capable of adjusting the lattice structure of solid surfaces with sub-angstrom precision and achieved in situ and continuous control over electrochemical activity.
Chem. Sci., 2022,13, 7765-7772
https://doi.org/10.1039/D2SC01868C
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CO reductive oligomerization by a divalent thulium complex and CO2-induced functionalization
The divalent thulium complex [Tm(Cpttt)2] activates CO to form reductive CO dimerization or trimerization products. These complexes further react with electrophiles, including CO2, yielding multicarbon oxygenates and original C–H activation products.
Chem. Sci., 2022,13, 7449-7461
https://doi.org/10.1039/D2SC01798A
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Biocatalytic cascades and intercommunicated biocatalytic cascades in microcapsule systems
Dynamic dimerization of GOx-loaded microcapsules with β-gal//hemin/G-quadruplex-bridged T1/T2-loaded microcapsules guides the bi-directional intercommunication of the three catalysts cascade.
Chem. Sci., 2022,13, 7437-7448
https://doi.org/10.1039/D2SC01542K
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Parallel imaging of coagulation pathway proteases activated protein C, thrombin, and factor Xa in human plasma
Using a collection of natural and unnatural amino acids, we synthesized a set of fluorescent activity-based probes for the fast, direct, and simultaneous detection of coagulation factors in human plasma.
Chem. Sci., 2022,13, 6813-6829
https://doi.org/10.1039/D2SC01108E
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Programmable alignment media from self-assembled oligopeptide amphiphiles for the measurement of independent sets of residual dipolar couplings in organic solvents
We report a programmable strategy to construct multi-alignment media via peptide self-assembly for the measurement of independent sets of residual dipolar couplings (RDCs).
Chem. Sci., 2022,13, 5838-5845
https://doi.org/10.1039/D2SC01057G
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Variable control of the electronic states of a silver nanocluster via protonation/deprotonation of polyoxometalate ligands
The electronic states of Ag nanoclusters were reversibly controlled driven by protonation/deprotonation of polyoxometalate ligands.
Chem. Sci., 2022,13, 5557-5561
https://doi.org/10.1039/D2SC01156E
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Fabrication of a family of atomically precise silver nanoclusters via dual-level kinetic control
A dual-level kinetic control was exploited to fabricate a family of atomically precise silver nanoclusters.
Chem. Sci., 2022,13, 5531-5538
https://doi.org/10.1039/D2SC01016J
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A sequential cyclization/π-extension strategy for modular construction of nanographenes enabled by stannole cycloadditions
Stannoles are introduced as a new, spontaneously aromatizing diene for [4 + 2] cycloadditions that can be easily introduced into diverse conjugated systems, facilitating the efficient synthesis of complex PAHs and their π-extension.
Chem. Sci., 2022,13, 5568-5573
https://doi.org/10.1039/D2SC00397J
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The Janus face of high trans-effect carbenes in olefin metathesis: gateway to both productivity and decomposition
In ruthenium catalysts for olefin metathesis, carbene ligands of high trans influence/effect suppress decomposition via β-H elimination, but increase susceptibility to bimolecular decomposition.
Chem. Sci., 2022,13, 5107-5117
https://doi.org/10.1039/D2SC00855F
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Predicting biomolecule adsorption on MoS2 nanosheets with high structural fidelity
Benchmarked van der Waals density functional theory calculations are used to create a force-field to describe biomolecule interactions at the aqueous MoS2 interface, which can recover interfacial biomolecule adsorption with high structural fidelity.
Chem. Sci., 2022,13, 5186-5195
https://doi.org/10.1039/D1SC06814H
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Stereoregular functionalized polysaccharides via cationic ring-opening polymerization of biomass-derived levoglucosan
We demonstrate the facile synthesis and characterization of stereoregular polysaccharides from the biomass-derived platform molecule levoglucosan via metal-triflate mediated cationic-ring opening polymerization.
Chem. Sci., 2022,13, 4512-4522
https://doi.org/10.1039/D2SC00146B
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Data-driven discovery of cardiolipin-selective small molecules by computational active learning
We present a data-driven approach combining deep learning-enabled active learning with coarse-grained simulations and alchemical free energy calculations to discover small molecules to selectively permeate cardiolipin membranes.
Chem. Sci., 2022,13, 4498-4511
https://doi.org/10.1039/D2SC00116K
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Hydridotetrylene [Ar*EH] (E = Ge, Sn, Pb) coordination at tantalum, tungsten, and zirconium
Low valent cations of tin and lead were used to form hydridotetrylene coordination compounds. The mobility of the hydrogen substituent was investigated in deprotonation equilibria as well as in 1,2-H-shift reactions.
Chem. Sci., 2022,13, 3999-4009
https://doi.org/10.1039/D2SC00297C
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Temperature triggered alternating copolymerization of epoxides and lactones via pre-sequenced spiroorthoester intermediates
We report the alternating copolymerization of caprolactone and epoxide through the in situ formation of pre-sequenced spiroorthoester monomer.
Chem. Sci., 2022,13, 3713-3718
https://doi.org/10.1039/D1SC06634J
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PIGNet: a physics-informed deep learning model toward generalized drug–target interaction predictions
PIGNet, a deep neural network-based drug–target interaction model guided by physics and extensive data augmentation, shows significantly improved generalization ability and model performance.
Chem. Sci., 2022,13, 3661-3673
https://doi.org/10.1039/D1SC06946B
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Primary trifluoroborate-iminiums enable facile access to chiral α-aminoboronic acids via Ru-catalyzed asymmetric hydrogenation and simple hydrolysis of the trifluoroborate moiety
Starting with potassium acyltrifluoroborates (KATs), N-unprotected chiral α-aminoboronic acids are prepared in three simple steps without chromatography. This facile methodology will tap the broad potential of these valuable compounds.
Chem. Sci., 2022,13, 2946-2953
https://doi.org/10.1039/D1SC07065G
![Open Access](https://www.rsc-cdn.org/pubs-core/2022.0.147/content/NewImages/open-access-icon-orange.png)
CO2-responsive Pickering emulsions stabilized by soft protein particles for interfacial biocatalysis
An unprecedented strategy was proposed for recycled interfacial biocatalysis in a CO2-responsive emulsion stabilized by soft protein particles. The recycled enzyme maintained its catalytic activity, with a conversion yield over 90% after 30 cycles.
Chem. Sci., 2022,13, 2884-2890
https://doi.org/10.1039/D1SC06146A
![Open Access](https://www.rsc-cdn.org/pubs-core/2022.0.147/content/NewImages/open-access-icon-orange.png)
Inducing a pH-dependent conformational response by competitive binding to Zn2+ of a series of chiral ligands of disparate basicity
A chemical system comprising a series of chiral acids of differing pKa, a metal, and a conformationally labile chromophore responds to pH with a CD spectrum that reports the absolute stereochemistry of the most basic anion in the mixture.
Chem. Sci., 2022,13, 2258-2269
https://doi.org/10.1039/D1SC06812A
![Open Access](https://www.rsc-cdn.org/pubs-core/2022.0.147/content/NewImages/open-access-icon-orange.png)
Solvent coordination to palladium can invert the selectivity of oxidative addition
In the presence of the bulky monophosphine PtBu3, palladium usually prefers to react with Ar–Cl over Ar–OTf bonds. However, strongly coordinating solvents can bind to palladium, inducing a reversal of selectivity.
Chem. Sci., 2022,13, 1618-1628
https://doi.org/10.1039/D1SC05862B
![Open Access](https://www.rsc-cdn.org/pubs-core/2022.0.147/content/NewImages/open-access-icon-orange.png)
How many more polymorphs of ROY remain undiscovered
Crystal structure prediction suggests that the low-energy polymorphs of ROY have already been found, but a new high-pressure form is predicted.
Chem. Sci., 2022,13, 1288-1297
https://doi.org/10.1039/D1SC06074K
![Open Access](https://www.rsc-cdn.org/pubs-core/2022.0.147/content/NewImages/open-access-icon-orange.png)
Fluorescent supramolecular polymers of barbiturate dyes with thiophene-cored twisted π-systems
Two barbiturate dyes with regioisomeric thiophene-cored twisted π-systems show strongly enhanced emission through supramolecular polymerization. The supramolecular polymers thus formed exhibit distinct emission colors and degree of agglomeration.
Chem. Sci., 2022,13, 1281-1287
https://doi.org/10.1039/D1SC06246H
About this collection
In 2018, the Chemical Science Editorial Team launched ‘ChemSci Pick of the Week’ as a means to select and promote our favourite articles from the week and share them with the wider chemical community. This on-going web collection showcases all ChemSci Picks from 2022.
All ChemSci Picks are promoted via Twitter and have an accompanying news article posted via our website.