- Fast room temperature lability of aluminosilicate zeolitesNature Communications, Published online: 16 October 2019; doi:10.1038/s41467-019-12752-yWhile aluminosilicate zeolites are of interest for many applications, the affect of water on zeolite stability in mild aqueous conditions has yet to be established. Here, using ab initio calculations and NMR spectroscopy, the authors show that covalent bonds in the zeolite chabazite are labile when in contact with neutral liquid water.
- Super-resolution imaging of fluorescent dipoles via polarized structured illumination microscopyNature Communications, Published online: 16 October 2019; doi:10.1038/s41467-019-12681-wPolarization microscopy has been combined with single-molecule localization, but it’s often limited in either speed or resolution. Here the authors present polarized Structured Illumination Microscopy (pSIM), a method that uses polarized laser excitation to measure dye orientation during fast super-resolution live cell imaging.
- Modular quantum computation in a trapped ion systemNature Communications, Published online: 16 October 2019; doi:10.1038/s41467-019-12643-2Modern computation relies on modular architectures, breaking a complex algorithm into self-contained subroutines, whereas current quantum computers do not have such capability. Here, the authors provide an experimental demonstration of a modular quantum computation protocol using a trapped Yb ion.
- Controlled creation of a singular spinor vortex by circumventing the Dirac belt trickNature Communications, Published online: 16 October 2019; doi:10.1038/s41467-019-12787-1Topological defects and textures are universal phenomena across physics. The authors demonstrate that an initial non-singular spinor texture can be controllably transformed into a pair of singular vortices with cores filled by atoms that continuously connect distinct magnetic phases of matter.
- IL-36 promotes anti-viral immunity by boosting sensitivity to IFN-α/β in IRF1 dependent and independent mannersNature Communications, Published online: 16 October 2019; doi:10.1038/s41467-019-12318-yHerpes simplex virus-1 (HSV-1) suppresses the induction of interferon to evade antiviral immunity. Here, Wang et al. show that during HSV-1 infection, IL-36 increases cellular sensitivity to interferon through induction of IRF1 and the interferon receptor.
- Controlling collective rotational patterns of magnetic rotorsNature Communications, Published online: 16 October 2019; doi:10.1038/s41467-019-12665-wA challenge of magnetically-actuated devices is to obtain different behaviours from each component under the same driving field. Here the authors tune the dipolar interactions between rotors to obtain different rotational behaviours when actuated by a magnetic field leading to complex collective dynamics.
- Epi-illumination gradient light interference microscopy for imaging opaque structuresNature Communications, Published online: 16 October 2019; doi:10.1038/s41467-019-12634-3Quantitative phase imaging techniques have been limited by multiple scattering of light or its use in transmission mode. Here, the authors show a gradient light interference microscopy method in a reflection geometry which allows for label-free phase imaging of bulk and opaque samples.
- Ultrasensitive MoS<sub>2</sub> photodetector by serial nano-bridge multi-heterojunctionNature Communications, Published online: 16 October 2019; doi:10.1038/s41467-019-12592-wFabrication of photodetector devices by selective etching of 2D materials can enable broadband detection. Here, the authors design mono- and multi-layer nano-bridge multi-heterojunction photodetectors based on MoS2 with high responsivities of 2.67 × 106 A/W and 1.65 × 104 A/W in the visible–infrared wavelength range and fast photoresponse.
Journal of the American Chemical Society: Latest Articles (ACS Publications)
- [ASAP] Pyonitrins A–D: Chimeric Natural Products Produced by <italic toggle="yes">Pseudomonas protegens</italic>Journal of the American Chemical SocietyDOI: 10.1021/jacs.9b09739
- [ASAP] Trans Influence of Ligands on the Oxidation of Gold(I) ComplexesJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b09363
- [ASAP] Architecture-Controlled Ring-Opening Polymerization for Dynamic Covalent Poly(disulfide)sJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b08957
- [ASAP] Copper-Triggered Bioorthogonal Cleavage Reactions for Reversible Protein and Cell Surface ModificationsJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b05833
- [ASAP] Aptamer Displacement Reaction from Live-Cell Surfaces and Its ApplicationsJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b07191
- [ASAP] Catalytically Relevant Intermediates in the Ni-Catalyzed C(sp<sup>2</sup>)–H and C(sp<sup>3</sup>)–H Functionalization of Aminoquinoline SubstratesJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b09109
- [ASAP] Structure and Dynamics of the Rhomboid Protease GlpG in Liposomes Studied by Solid-State NMRJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b08952
- [ASAP] Mechanisms for Hydrogen-Atom Abstraction by Mononuclear Copper(III) Cores: Hydrogen-Atom Transfer or Concerted Proton-Coupled Electron Transfer?Journal of the American Chemical SocietyDOI: 10.1021/jacs.9b08109
- [ASAP] Fe-Catalyzed Reductive Couplings of Terminal (Hetero)Aryl Alkenes and Alkyl Halides under Aqueous Micellar ConditionsJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b04510
- [ASAP] The Role of Proton Shuttles in the Reversible Activation of Hydrogen via Metal–Ligand CooperationJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b09062
- [ASAP] Mechanism and Scope of Nickel-Catalyzed Decarbonylative Borylation of Carboxylic Acid FluoridesJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b08961
- [ASAP] Site-Specific Sequential Protein Labeling Catalyzed by a Single Recombinant LigaseJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b09166
- [ASAP] Engineering the hCRBPII Domain-Swapped Dimer into a New Class of Protein SwitchesJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b04664
- [ASAP] Strong p-Backbonding Enables Record Magnetic Exchange Coupling Through CyanideJournal of the American Chemical SocietyDOI: 10.1021/jacs.9b09445
Angewandte Chemie International Edition
- High‐entropy chemistry stabilizing layered O3‐type structure in Na‐ion cathodeMaterial innovation on high‐performance Na‐ion cathodes and the corresponding understanding of structural chemistry still remain elusive. Herein, we report a new concept of high‐entropy chemistry for Na‐ion cathodes. An example of layered O3‐type NaNi 0.12 Cu 0.12 Mg 0.12 Fe 0.15 Co 0.15 Mn 0.1 Ti 0.1 Sn 0.1 Sb 0.04 O 2 has been designed and prepared successfully, which exhibits the l onger cycling stability ( ~ 83% o
- New Wine in Old Bottle: Prolonging Room‐Temperature Phosphorescence of Crown Ethers by Supramolecular InteractionsSupramolecular macrocyclic hosts have been of great interest in smart materials for years, whereas their triplet emission and regulation at crystal level is still rarely excavated. Herein, ultralong and universal room temperature phosphorescence (RTP) phenomenon is evacuated for traditional crown ethers. Supramolecular strategy involving chain length adjustment and morphological locking through complexation with K+ was explored as general methods
- Biosynthesis of Norsesquiterpene Aculenes Requires Three Cytochrome P450s to Catalyze a Stepwise Demethylation ProcessAculenes are a unique class of norsequiterpenes (C 14 ) produced from Aspergillus aculeatus. The nordaucane skeleton in aculenes A−D may be derived from an ent‐daucane precursor through a demethylation process. Despite their unprecedented structures, the genetic basis and enzymatic mechanisms involved in the biosynthesis of aculenes remained unexplored. Here, we identified the biosynthetic gene cluster of aculenes and characterized the biosynth
- Drawing with Iron on a Gel Containing a Supramolecular SiderophoreGuanosine‐5ʹ‐hydroxamic acid (3) forms hydrogels when mixed with guanosine (1) and KCl. The 5ʹ‐hydroxamic acid (HA) unit is pH‐responsive and also chelates Fe3+. When gels are prepared under basic conditions the 5ʹ‐HA groups are deprotonated and the anionic hydrogel binds cationic thiazole orange (TO), signaled by enhanced fluorescence. The HA nucleoside 3, when immobilized in the G‐quartet gel, acts as a supramolecular siderophore to form red co
- Excitation‐Dependent Long‐Life Luminescent Polymeric Systems under Ambient ConditionsOrganic room temperature luminescent materials present unique phosphorescence emission with long lifetime. However, a lot of these materials only emit single blue or green color in spite of external stimulation, whereas their color tunability is strictly limited. Herein, we report a rational design to extend the emission color range from blue to red by controlling the doping simple pyrene derivatives into robust polymer matrix. The integration of
- Unique Bora[1]ferrocenophanes with Sterically Protected Boron: A Potential Gateway to Helical PolyferrocenesTilt a whirl: A new class of chiral [1]ferrocenophanes is described which feature a record‐high Cp ring tilt. From one of the monomers a poly(ferrocenylborane) was obtained that, according to DFT calculations, exhibits a left‐handed helical structure. This is the first evidence of a polyferrocene with a chiral secondary structure. Abstract Silicon‐bridged [1]ferrocenophanes are a versatile class of monomers to obtain well‐defined metallopol
- Selectivity of Chemical Conversions: Do Light‐Driven Photoelectrocatalytic Processes Hold Special Promise?The peculiar aspects of interfacial energetics at illuminated semiconductors dictate differences in the kinetics of interfacial reactions compared to electrically biased metallic electrodes. Well‐designed light‐driven photoelectrocatalytic processes are, therefore, highly promising in terms of maximizing the selectivity of catalytic transformations towards specific desired products. Abstract One of the great challenges in chemistry is the d
- Synthesis of Polycyclic Aromatic Hydrocarbons by Phenyl Addition–Dehydrocyclization: The Third WayThe triphenylene and fluoranthene molecules—potential precursors to two‐ and three‐dimensional graphitic nano sheets in the interstellar medium—can be formed through rapid molecular mass growth processes by the reactions of phenyl radical with biphenyl and naphthalene at high temperatures. Abstract Polycyclic aromatic hydrocarbons (PAHs) represent the link between resonance‐stabilized free radicals and carbonaceous nanoparticles generated i
- Inverting External Asymmetric Induction via Selective Energy Transfer Catalysis: A Strategy to β‐Chiral Phosphonate AntipodesEnantiodivergent, catalytic reduction of activated alkenes relays stereochemical information encoded in the antipodal chiral catalysts to the pro‐chiral substrate. Although powerful, the strategy remains vulnerable to costs and availability of sourcing both catalyst enantiomers. Herein, a stereodivergent hydrogenation of α,β‐unsaturated phosphonates is disclosed using a single enantiomer of the catalyst. This enables generation of the R ‐ or S
- Freeing the polarons to facilitate charge transport in BiVO4 from oxygen vacancies with an oxidative 2D precursorThe BiVO 4 photoelectrochemical (PEC) electrode in tandem with a photovoltaic (PV) cell has shown great potential to become a compact and cost‐efficient device for solar hydrogen generation. However, the PEC part is still facing problems such as the poor charge transport efficiency due to the drag of oxygen vacancy bound polarons. In the present work, to effectively suppress oxygen vacancy formation, we have developed a new route to synthesize
- Nucleation and Growth of Amino‐acid and Peptide Supramolecular Polymers through Liquid‐liquid Phase SeparationThe transition of peptides and proteins from solution into fibrillar structures is a general phenomenon encountered in functional and aberrant biology and is increasingly exploited in soft materials science. However, the fundamental molecular events underpinning the early stages of their assembly and subsequent growth have remained challenging to elucidate. Here, we show that liquid‐liquid phase separation into solute‐rich and solute‐poor phases
- Nitrogen Dioxide Catalyzed Aerobic Oxidative Cleavage of C(OH)–C Bonds of Secondary Alcohols to Produce AcidsNO2 in DMSO catalyzes the aerobic oxidative cleavage of C(OH)−C bonds to form a carboxylic group, and NO2 was generated in situ by decomposition of nitrates. A diverse range of secondary alcohols were selectively converted into acids in excellent yields in this transition‐metal‐free system without any additives. Abstract Stable organic nitroxyl radicals are an important class of catalysts for oxidation reactions, but their wide applications
- Self‐Assembly of a Phosphate‐Centered Polyoxo‐Titanium Cluster: Discovery of the Heteroatom Keggin FamilyOne of the family: A TiIV‐based heteroatom Keggin and its trivacant lacunary architectures were structurally synthesized as a polyoxo‐titanium cluster. They exhibited a very high selectivity and activity for photocatalytic CO2‐to‐HCOOH conversion. Abstract Over the past 200 years, the most famous and important heteroatom Keggin architecture in polyoxometalates has only been synthesized with Mo, W, V, or Nb. Now, the self‐assembly of two pho
- Lead‐Free Sodium–Indium Double Perovskite Nanocrystals through Doping Silver Cations for Bright Yellow EmissionGlow yellow: Lead‐free double perovskite Cs2NaInCl6 and Ag‐doped Cs2NaInCl6 nanocrystals (NCs) are synthesized. Ag‐doped NCs exhibit bright yellow emission with photoluminescence quantum efficiency of 31.1 %. The self‐trapped exciton dynamics mechanism is also studied. Abstract Lead‐free halide perovskite nanocrystals (NCs) have drawn wide attention for solving the problem of lead perovskites toxicity and instability. Herein, we synthesize
- The Microscopic Structure–Property Relationship of Metal–Organic Polyhedron NanocompositesMaking inorganics elastic: Hairy nanocomposites of metal–organic polyhedra are designed and synthesized, and their structures have been fully studied. Their relationship to the unique thermal and mechanical properties of the nanocomposites have been revealed for the first time. The studies finally led to the concept of the first MOP‐based elastomers, which is of immediate and practical motivation of the design of separation membranes. Abstra
- Blue LED Irradiation of Iodonium Ylides Gives Diradical Intermediates for Efficient Metal‐free Cyclopropanation with AlkenesThe Generation of doubly activated cyclopropanes upon irradiating alkenes and β‐dicarbonyl‐derived iodonium ylides with visible light from blue LEDs is shown by S. Quideau, W. S. Hopkins, G. K. Murphy, and co‐workers in their Research Article (DOI: https://doi.org/10.1002/anie.20190899410.1002/anie.201908994). This metal‐free cyclopropane synthesis works with cyclic and acyclic ylides, and with electronically‐diverse alkenes, in yields up to 96 %
- Efficient BiVO4 photoanodes by postsynthetic treatment: remarkable improvements in photoelectrochemical performance from facile borate modificationWater‐splitting photoanodes based on semiconductor materials typically require a dopant in the structure and co‐catalysts on the surface to overcome the problems of charge recombination and high catalytic barrier. Unlike these conventional strategies, we herein report a simple treatment by soaking a sample of pristine BiVO4 in a borate buffer solution. This modifies the catalytic local environment of BiVO4 by the introduction of a borate moiety a
- Straightforward Synthesis and Properties of Highly Fluorescent [5]‐ and [7]‐Helical Dispiroindeno[2,1‐c]fluorenes[5]‐ and [7]‐Helical compounds possessing the dispiroindeno[2,1‐c]fluorene framework were prepared in 5–6 steps with high overall yields by using catalytic intramolecular [2+2+2]‐cyclotrimerization as the crucial step. They exhibit fluorescence in the region of 351–428 nm with high quantum yields (up to 0.88). Abstract This work presents a general approach for synthesis of substituted [5]‐helical dispiroindeno[2,1‐c]fluorenes based on Rh‐ca
- Conformational Entropy as a Means to Control the Behavior of Poly(diketoenamine) Vitrimers In and Out of EquilibriumPoly(diketoenamine) (PDK) vitrimers are an emerging platform for sustainable plastics, providing additive‐tolerant chemical circularity after depolymerization. Here we show how to control the equilibrium and non‐equilibrium thermomechanical behavior of PDKs by incorporating into the dynamic covalent network linear polymer segments varying in both molecular weight ( MW = 0–12 kg mol –1 ) and conformational degrees of freedom. While increasing
- Ultrafast Intercalation Enabled by Strong Solvent–Host Interactions: Understanding Solvent Effect at the Atomic LevelA solvent effect is seen in the solution‐phase intercalation of ferrocene into layered vanadyl phosphate to form an organic–inorganic superlattice. The drastically different intercalation kinetics in primary alcohols following a volcano shape is understood at the atomic level as a result of solvent pre‐intercalation. Abstract Solvents play an essential role in many areas of chemistry and is the cornerstone of understanding reactivity in sol
- Fabrication of Large Single Crystals for Pt‐Based Linear Polymers with Controlled‐Release and Photoactuator PerformancePreparation of large single crystals for linear polymers that are amenable to X‐ray analysis is very challenging in polymer science. Herein, we employed a coordination driven self‐assembly strategy to secure appropriate head‐to‐tail alignment of anthracene moieties, and for the first time obtained large‐sized Pt‐based linear polymer crystals through a [4+4] cycloaddition of anthracene in a single‐crystal to single‐crystal fashion. Using X‐ray dif
- Cascade One‐Pot Synthesis of Orange‐Red Fluorescent Polycyclic Cinnolino[2,3‐f]phenanthridin‐9‐ium Salts by Palladium(II)‐Catalyzed C‐H Bond Activation of 2‐Azobiaryls and AlkenesThe first palladium‐catalyzed synthesis of quaternary ammonium salts through double oxidative C‐H bond activation on azobenzenes in moderate to good yields is reported. In this study, we disclose a highly regioselective synthesis of orange‐red fluorescent cinnolino[2,3‐ f ]phenanthridin‐9‐ium salts and 15 H ‐cinnolino[2,3‐ f ]phenanthridin‐9‐ium‐10‐ide from 2‐azobiaryls and alkenes catalyzed by palladium(II). The reaction mechanism is propo
- CyClick Chemistry for Synthesis of Cyclic PeptidesCyclic peptides are emerging as important class of therapeutics and small‐to‐medium sized rings have been of particular interest. The laboratory synthesis of cyclic peptides can prove to be a difficult and long‐standing problem. One of the major challenges with conventional macrocyclization techniques is the formation of undesirable dimers and cyclooligomers at high concentrations due to intermolecular reactions between linear peptides. Here, we
- Turning the Tap: Conformational Control of Quantum Interference to Modulate Single Molecule ConductanceTogether with the more intuitive and commonly recognized conductance mechanisms of charge‐hopping and tunneling, quantum interference (QI) phenomena have been identified as important factors affecting charge transport through molecules. Consequently, establishing simple, flexible molecular design strategies to understand, control and exploit QI in molecular junctions poses an exciting challenge. Here we demonstrate that destructive quantum interf
- Electrostatic Complementarity drives Amyloid/Nucleic Acid Co‐assemblyProteinaceous plaques associated with neurodegenerative diseases contain many biopolymers including the polyanions glycosaminoglycans and nucleic acids. Polyanion‐induced amyloid fibrillation has been implicated in disease etiology, but structural models for amyloid/nucleic acid co‐assemblies remain limited. Here we constrain nucleic acid/peptide interactions with model peptides that exploit electrostatic complementarity and define a novel amyloi
- Electrochemistry Broadens the Scope of Flavin Photocatalysis: Photoelectrocatalytic Oxidation of Unactivated AlcoholsRiboflavin‐derived photocatalysts have been extensively studied in the context of alcohol oxidation. However, to date, the scope of this catalytic methodology has been limited to benzyl alcohols. In this work, we gained further mechanistic understanding of flavin‐catalyzed oxidation reactions in the absence or presence of thiourea as a cocatalyst. The mechanistic insights enabled us to develop an electrochemically driven photochemical oxidation o
- Elucidating the Ultrafast Molecular Permeation through Well‐defined 2D Nanochannels of Lamellar MembranesLamellar membranes with well‐defined 2D nanochannels exhibit fast, selective permeation. However, the underlying molecular transport mechanism remains unexplored. Here in , regular and robust MXene Ti 3 C 2 T x lamellar membranes are prepared, and the size and wettability of nanochannels are manipulated by chemically grafted hydrophilic (‒NH 2 ) or hydrophobic (‒C 6 H 5 , ‒C 12 H 25 ) groups. These nanochannels have sharp differenc
- Unusual Through‐Space Interactions between Oxygen Atoms Mediate Inverse Morphochromism of an AIE LuminogenWe have studied the photophysics of tetrafurylethene, an aggregation‐induced emission luminogen that has exceptionally short intramolecular O‐O distances of 2.80 Å and shows a significant redshifted morphochromism (27 nm) when going from the aggregate to the crystal. The short O‐O distances, which are substantially smaller than the sum of the van der Waals radii (3.04 Å), are due to the fact that the oxygen atoms act as an elect
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