43,789 results match your criteria Angewandte Chemie-international Edition[Journal]


Coupling Wireless Bipolar Ultramicroelectrode with Nano-electrospray Ionization Mass Spectrometry: Insights into the Ultrafast Initial Step of Electrochemical Reactions.

Angew Chem Int Ed Engl 2020 Jul 11. Epub 2020 Jul 11.

Najing University, Chemistry, Xianlin Ave. 163, , 210023, Nanjing, CHINA.

We report a new mass spectrometric method for detecting electrogenerated intermediates. This approach is based on simultaneous activation of electrospray ionization and redox reaction on a wireless bipolar ultramicroelectrode, which is fabricated in the tip of a quartz nanopipette. The hollow structure of the ultramicroelectrode permits rapid transferring the transient species from electrode-electrolyte interfaces into gas phase for mass spectrometric identification on the time scale of microseconds. Read More

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http://dx.doi.org/10.1002/anie.202008577DOI Listing

Guest-Responsive Reversible Electron Transfer in a Crystalline Porous Framework Supported by Dynamic Building Node.

Angew Chem Int Ed Engl 2020 Jul 11. Epub 2020 Jul 11.

Jawaharlal Nehru Centre for Advanced Scientfic Research, Chemistry and Physics of Materials Unit, Jakkur, 560 064, Bangalore, INDIA.

Spatial organization of electron donor-acceptor (D-A) supramolecular assembly is critical to the photophysical processes involved in solar energy conversion systems. Subtle variation in geometry, i.e. Read More

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http://dx.doi.org/10.1002/anie.202008189DOI Listing

Tuning Electrical- and Photo-Conductivity by Cation Exchange within a Redox-Active Tetrathiafulvalene-Based Metal-Organic Framework.

Angew Chem Int Ed Engl 2020 Jul 11. Epub 2020 Jul 11.

Nanjing University, School of Chemistry and Chemical Engineering, Han Kou Road 22, 210093, Nanjing, CHINA.

To activate electronic and optical functions of the redox-active metal-organic framework, (Me 2 NH 2 )[In III (TTFTB)]·0.7C 2 H 5 OH· DMF (Me 2 NH 2 @ 1, TTFTB = tetrathiafulvalene-tetrabenzoate, DMF = N,N -dimethylformamide), has been exchanged by tetrathiafulvalenium (TTF •+ ) and N,N ' -dimethyl- 4,4 ' -bipyridinium (MV 2+ ). These cations provide electron carriers and photosensitivity. Read More

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http://dx.doi.org/10.1002/anie.202008941DOI Listing

Universal Access to Two-Dimensional Mesoporous Heterostructures via Micelle-Directed Interfacial Assembly.

Angew Chem Int Ed Engl 2020 Jul 11. Epub 2020 Jul 11.

The University of Queensland, School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology (AIBN), Saint Lucia, 4072, Brisbane, AUSTRALIA.

Two-dimensional (2D) mesoporous heterostructures combining ultrathin nanosheet morphology, periodic porous surface structures and diverse hybrid compositions have recently emerged and become increasingly important for renewable energy storage and electronics. However, it remains a great challenge to develop a universal method to prepare 2D mesoporous heterostructures. Here, we report a composite micelle-directed interfacial assembly method to synthesize vertical heterostructures with ultrathin 2D material and two surrounding mesoporous monolayers assembled on both sides. Read More

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http://dx.doi.org/10.1002/anie.202007063DOI Listing

Synergy of Electrostatic and π-π Interactions in the Realization of Nanoscale Artificial Photosynthetic Model Systems.

Angew Chem Int Ed Engl 2020 Jul 11. Epub 2020 Jul 11.

Universidad Autonoma de Madrid, Organic Chemistry, SPAIN.

In the scientific race to build up photoactive electron donor-acceptor systems with increasing efficiencies, little is known about the interplay of their building blocks when integrated into supramolecular nanoscale arrays, particularly in aqueous environments. Here, we describe an aqueous donor-acceptor ensemble whose emergence as a nanoscale material renders it remarkably stable and efficient. We have focused on a tetracationic zinc phthalocyanine (ZnPc) featuring pyrenes, which shows an unprecedented mode of aggregation, driven by subtle cooperation between electrostatic and π-π interactions. Read More

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http://dx.doi.org/10.1002/anie.202006014DOI Listing

Dealkenylative Alkenylation: Formal σ-Bond Metathesis of Olefins.

Angew Chem Int Ed Engl 2020 Jul 11. Epub 2020 Jul 11.

University of California Los Angeles, Chemistry and Biochemistry, UNITED STATES.

Dealkenylative alkenylation of alkene C(sp3)-C(sp2) bonds has been an unexplored area for C-C bond formation. Herein, we report 64 examples of β-alkylated styrene derivatives synthesized through the reactions of readily accessible feedstock olefins with β-nitrostyrenes through ozone/Fe(II)-mediated radical substitution. These reactions proceed with good efficiency and high stereoselectivity under mild conditions and tolerate an array of functional groups. Read More

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http://dx.doi.org/10.1002/anie.202005267DOI Listing

Merging Electrosynthesis and Bifunctional Squaramide Catalysis in the Asymmetric Detrifluoroacetylative Alkylation Reactions.

Angew Chem Int Ed Engl 2020 Jul 11. Epub 2020 Jul 11.

University of Science and Technology of China, Hefei National Laboratory for Physical Sciences at the Microscale, No.96, JinZhai Road Baohe District, 230026, Hefei, CHINA.

An enantioselective bifunctional squaramide-catalyzed detrifluoroacetylative alkylation reaction under electrochemical conditions has been developed. The unified strategy based on this key tandem methodology has been divergently explored for the asymmetric synthesis of fluorine-containing target molecules with good stereocontrol (up to 95% ee ). Furthermore, this catalytic asymmetric detrifluoroacetylative alkylation reaction demonstrated the benefits of combining electrosynthesis and organocatalysis for the preparation of biologically relevant products containing C-F tertiary stereogenic center. Read More

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http://dx.doi.org/10.1002/anie.202006903DOI Listing

Atomic Insights into Aluminium-Ion Insertion in Defective Anatase for Batteries.

Angew Chem Int Ed Engl 2020 Jul 10. Epub 2020 Jul 10.

Forschungszentrum Julich GmbH, Chemistry, GERMANY.

Aluminium batteries constitute a safe and sustainable high-energy-density electrochemical energy-storage solution. Viable Al-ion batteries require suitable electrode materials that can readily intercalate high-charge Al 3+ ions. Here, we investigate the Al 3+ intercalation chemistry of anatase TiO 2 and how chemical modifications influence the accommodation of Al 3+ ions. Read More

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http://dx.doi.org/10.1002/anie.202007983DOI Listing

Engineering Polar Oxynitrides: Hexagonal Perovskite BaWON2.

Angew Chem Int Ed Engl 2020 Jul 10. Epub 2020 Jul 10.

Institut de Ciencia de Materials de Barcelona(CSIC), Solid State Chemistry, Campus UAB, 08193, Bellaterra, SPAIN.

Non-centrosymmetric polar compounds have important technological properties. Reported perovskite oxynitrides show centrosymmetric structures and for some of them high permittivities have been observed, ascribed to local dipoles induced by partial order of nitride and oxide. Here we report the first hexagonal perovskite oxynitride BaWON2, that shows a polar 6H polytype. Read More

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http://dx.doi.org/10.1002/anie.202006519DOI Listing

Peptide-conjugated long-lived theranostic imaging toolbox for targeting GRPr in cancer and immune cells.

Angew Chem Int Ed Engl 2020 Jul 10. Epub 2020 Jul 10.

Hong Kong Baptist University, Department of Chemistry, 224 Waterloo Road, 852, Hong Kong, CHINA.

Gastrin-releasing peptide receptor (GRPr) plays proliferative and inflammatory roles in living systems. Here, we report a highly selective GRPr antagonist (JMV594)-tethered iridium(III) complex for probing GRPr in living cancer cells and immune cells. This probe not only exhibited desirable photophysical properties, but also displayed negligible cytotoxicity, overcoming the inherent toxicity of the iridium(III) complex. Read More

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http://dx.doi.org/10.1002/anie.202007920DOI Listing

Expanded Analogs of Three-Dimensional Lead-Halide Hybrid Perovskites.

Angew Chem Int Ed Engl 2020 Jul 10. Epub 2020 Jul 10.

Stanford University, Department of Chemistry, 333 Campus Drive, Mudd Building, 94305-4401, Stanford, UNITED STATES.

Replacing the Pb-X octahedral building unit of A I PbX 3 perovskites (X = halide) with a pair of edge-sharing Pb-X octahedra affords the expanded perovskite analogs: A II Pb 2 X 6 . We report eight members of this new family of materials. In 3D hybrid perovskites, orbitals from the organic molecules do not participate in the band edges. Read More

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http://dx.doi.org/10.1002/anie.202005012DOI Listing

DNA Origami meets polymers A powerful tool for defined nanostructure design.

Angew Chem Int Ed Engl 2020 Jul 10. Epub 2020 Jul 10.

Max-Planck-Institut fur Polymerforschung, MPI, GERMANY.

While the art of DNA origami has been investigated extensively in recent years and demonstrated to work in a reliable manner, precise engineering of such patterns with polymers represents an emerging topic. Compared to conventional top-down approaches ( i.e. Read More

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http://dx.doi.org/10.1002/anie.202005907DOI Listing

Construction of Flexible-on-Rigid Hybrid-Phase Metal-Organic Frameworks (MOFs) for Controllable Multi-Drug Delivery.

Angew Chem Int Ed Engl 2020 Jul 10. Epub 2020 Jul 10.

Wuhan University, Chemistry, Wuhan University, 430072, Wuhan, CHINA.

Multi-component MOFs contain multiple sets of unique and hierarchical pores, with different functions for different applications, distributed in their inter-linked domains. Herein, we report the construction of a class of precisely aligned flexible-on-rigid hybrid-phase MOFs with unique rods-on-octahedron morphology. We demonstrated that hybrid-phase MOFs can be constructed based on two prerequisites: the partially matched topology at the interface of the two frameworks, and the structural flexibility of MOFs with acs topology, which can compensate for the differences in lattice parameters. Read More

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http://dx.doi.org/10.1002/anie.202008858DOI Listing

Probing the design rationale of a high-performing faujasitic zeotype engineered with hierarchical porosity and moderated acidity.

Angew Chem Int Ed Engl 2020 Jul 10. Epub 2020 Jul 10.

University of Southampton, Chemistry, University Road, Highfield, SO171BJ, Southampton, UNITED KINGDOM.

Porosity and acidity are influential properties in the rational design of solid-acid catalysts. Probing the physicochemical characteristics of an acidic zeotype framework at the molecular level can provide valuable insights in understanding intrinsic reaction pathways, for affording structure-activity relationships. Herein, we employ a variety of probe-based techniques (including positron annihilation lifetime spectroscopy (PALS), FTIR and solid-state NMR) to demonstrate how a hierarchical design strategy for a faujasitic (FAU) zeotype (synthesized for the first time, via a soft-templating approach, with high phase-purity) can be used to simultaneously modify the porosity and modulate the acidity for an industrially-significant catalytic process (Beckmann rearrangement). Read More

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http://dx.doi.org/10.1002/anie.202005108DOI Listing

An Ultrastable, Small {Ag } Nanocluster within a Triangular Hollow Polyoxometalate Framework.

Angew Chem Int Ed Engl 2020 Jul 10. Epub 2020 Jul 10.

Department of Applied Chemistry, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-8656, Japan.

Small Ag nanoclusters (n<10) have been emerging as promising materials as sensing, biolabeling, and catalysis because of their unique electronic states and optical properties. However, studying synthesis, structure determination, and exploration of their properties remain major challenges as a result of the low stability of small Ag nanoclusters. Herein, we synthesized an atomically precise face-centered-cubic-type small {Ag } nanocluster supported by a novel triangular hollow polyoxometalate (POM) framework [Si W O ] . Read More

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http://dx.doi.org/10.1002/anie.202008402DOI Listing

Mechanistic Insights into C(sp2)-C(sp)N Reductive Elimination from Gold(III) Cyanide Complexes.

Angew Chem Int Ed Engl 2020 Jul 10. Epub 2020 Jul 10.

Universitat Zurich, chemistry, SWITZERLAND.

A new family of phosphine-ligated dicyanoarylgold(III) complexes has been prepared and their reactivity towards reductive elimination has been studied in detail. Both, a highly positive entropy of activation and a primary 12/13 C KIE suggest a late concerted transition state while Hammett analysis and DFT calculations indicate that the process is asynchronous. As a result, a distinct mechanism involving an asynchronous concerted reductive elimination for the overall C(sp 2 )-C(sp)N bond forming reaction is characterized here for the first time complementing previous studies reported for C(sp 3 )-C(sp 3 ), C(sp 2 )-C(sp 2 ) and C(sp 3 )-C(sp 2 ) bond formation processes taking place on gold(III) species. Read More

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http://dx.doi.org/10.1002/anie.202005731DOI Listing

A novel separation-sensing membrane performing precise real-time serum analysis during blood drawing.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Nanjing Tech University, State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, 30 Puzhu South Road, Nanjing 211800, P.R. China, 211800, Nanjing, CHINA.

Dynamic and on-site analysis of serum from human blood is crucial particularly for making decisions during clinical surgery and emergency treatments. However, state-of-the-art blood assay methods can only collect single or discrete data of physiological analytes, remaining great challenge in online report of dynamic fluctuation of key analytes. Here we propose a novel separation-sensing membrane by constructing a heterogeneous-nanostructured architecture in which a surface nanoporous layer continuously extracts serum and underneath biosensing nanochannels dynamically recognize biotargets, achieving continuous testing of vital clinical indices as blood drawn. Read More

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http://dx.doi.org/10.1002/anie.202008241DOI Listing

General Formation of Macro-/Mesoporous Nanoshells from Interfacial Assembly of Irregular Mesostructured Nanounits.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

University of Queensland, Australian Institute for Bioengineering and Nanotechnology, AUSTRALIA.

Mesoporous core-shell nanostructures holding controllable ultra-large open channels in their nanoshells are of great interests for the development of new catalytic platforms, electrochemical energy systems, and biological macromolecular carriers. However, soft template-directed cooperative assembly to mesoporous nanoshells with highly accessible pores larger than 30 nm, or even above 50 nm into macroporous range, remains a significant challenge. Herein we report a general approach for precisely tailored coating of hierarchically macro-/mesoporous polymer and carbon shells, possessing highly accessible radial channels with extremely wide pore size distribution from ~10 nm to ~200 nm, on diverse functional materials. Read More

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http://dx.doi.org/10.1002/anie.202007031DOI Listing

Revealing the A-site effect of lead-free A3Sb2Br9 perovskite in photocatalytic C (sp3)-H bonds activation.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Peking University, College of Chemistry and Molecular Engineering, Chengfu Road No.292, 100871, Beijing, CHINA.

Lead-free halide perovskite of A 3 Sb 2 Br 9 is utilized as photocatalyst for the first time to C (sp 3 )-H bonds activation. A 3 Sb 2 Br 9 nanoparticles (A 3 Sb 2 Br 9 NPs) with different ratios of Cs and MA show different photocatalytic activity for toluene oxidation and the photocatalytic performance is enhanced when increasing the amount of Cs. We reveal that the octahedron distortion caused by A-site cations can change the electronic property of X-site ions and further affect the electron transfer from toluene molecules to Br sites. Read More

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http://dx.doi.org/10.1002/anie.202005495DOI Listing
July 2020
11.261 Impact Factor

Functional genome mining reveals a novel class V lanthipeptide containing a D-amino acid introduced by an F420H2-dependent reductase.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Shanghai Jiao Tong University, School of Life Sciences and Biotechnology, CHINA.

Lantibiotics are a type of ribosomally synthesized and post-translationally modified peptides (termed lanthipeptides) with often potent antimicrobial activity. Herein, we report the discovery of a new lantibiotic, lexapeptide, using the Library EXpression Analysis System (LEXAS) approach. Lexapeptide has rare structural modifications, including N-terminal (N,N)-dimethyl phenylalanine, C-terminal (2-aminovinyl)-3-methyl-cysteine, and D-Ala. Read More

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http://dx.doi.org/10.1002/anie.202008035DOI Listing

Axial modification of cobalt complexes on heterogeneous surface with enhanced electron transfer for carbon dioxide reduction.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Southern University of Science and Technology, Department of Physics, CHINA.

Efficient electron communication between molecular catalyst and support is critical for heterogeneous molecular electrocatalysis and yet it is often overlooked during the catalyst design. Taking CO 2 electro-reduction on tetraphenylporphyrin cobalt (PCo) immobilized onto graphene as an example, we demonstrate that adding a relay molecule improves the interfacial electron communication. While the directly immobilized PCo on graphene exhibits relatively poor electron communications, it is found that diphenyl sulfide serves as an axial ligand for PCo and it improves the redox activity of PCo on the graphene surface to facilitate the generation of [PCo] • ‾ active sites for CO 2 reduction. Read More

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http://dx.doi.org/10.1002/anie.202008759DOI Listing

Titanium defective sites in TS-1: structural insights by combining spectroscopy and simulation.

Angew Chem Int Ed Engl 2020 Jul 10. Epub 2020 Jul 10.

Universita degli Studi di Torino Dipartimento di Chimica, Dipartimento di Chimica, ITALY.

Ti silicates, and in particular Titanium Silicalite-1 (TS-1), are nowadays important catalysts for several partial oxidation reactions in the presence of aqueous H 2 O 2 as oxidant. Despite the numerous studies dealing with this material, some fundamental aspects are still unfathomed. In particular, the structure and the catalytic role of defective Ti sites, other than perfect tetrahedral sites recognized as main active species, has not been quantitatively discussed in the literature. Read More

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http://dx.doi.org/10.1002/anie.202005841DOI Listing

Non-Interpenetrated Single-Crystal Covalent Organic Frameworks.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Lanzhou University, State Key Laboratory of Applied Organic Chemistry, New Chem Building, Room 501, Lanzhou University, 222 S Tianshui Road, 730000, Lanzhou, CHINA.

Growth of covalent organic frameworks (COFs) as single crystals is extremely challenging. Inaccessibility of open-structured single-crystal COFs prevents the exploration of structure-oriented applications.  Herein we report for the first time a non-interpenetrated single-crystal COF, LZU-306, which possesses the open structure constructed exclusively via covalent assembly. Read More

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http://dx.doi.org/10.1002/anie.202007230DOI Listing

Atom Exchange Versus Reconstruction: (GexAs4-x)x- (x = 2, 3) as Building Blocks for the Supertetrahedral Zintl Cluster [Au6(Ge3As)(Ge2As2)3]3.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Philipps-Universitat Marburg, Fachbereich Chemie, GERMANY.

The Zintl anion (Ge 2 As 2 ) 2- represents an isostructural and isoelectronic binary counterpart of yellow arsenic, yet without being studied with the same intensity so far. Upon introducing [(PPh 3 )AuMe] into the 1,2-diaminoethane (en) solution of (Ge 2 As 2 ) 2- , the heterometallic cluster anion [Au 6 (Ge 3 As)(Ge 2 As 2 ) 3 ] 3- is obtained as its salt [K(crypt-222)] 3 [Au 6 (Ge 3 As)(Ge 2 As 2 ) 3 ]·en·2tol ( 1 ). The anion represents a rare example of a superpolyhedral Zintl cluster, and it comprises the largest number of Au atoms relative to main group (semi)metal atoms in such clusters. Read More

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http://dx.doi.org/10.1002/anie.202008108DOI Listing

S6N2O15 - a nitrogen-poor sulfur nitride-oxide, and the anhydride of nitrido-tris-sulfuric acid.

Angew Chem Int Ed Engl 2020 Jul 10. Epub 2020 Jul 10.

Universitat zu Koln, Department of Chemistry, GERMANY.

The reaction of hexachlorophosphazene, P3N3Cl6, with SO3 leads to the new sulfur nitride-oxide S6N2O15. The compound displays an extraordinarily low nitrogen content and exhibits a bicyclic cage structure according to the formulation N{S(O)2O(O)2S}3N, with both nitrogen atoms in trigonal planar coordination of sulfur atoms. Interestingly, the new nitride-oxide can be also seen as the anhydride of nitrido-tris-sulfuric acid, N(SO3H)3. Read More

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http://dx.doi.org/10.1002/anie.202005056DOI Listing

Diversified Excited-State Relaxation Pathways of Donor-Linker-Acceptor Dyads Controlled by the Bent-to-Planar Motion of Donor.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

National Taiwan University, Dept Chemistry, TAIWAN.

Herein, we introduce the cyclic 8π-electron (C8π) molecule N , N '-diaryl-dihydrodibenzo[ a , c ]phenazines ( DPAC ) as a dual-functional donor to establish a series of new donor-linker-acceptor (D-L-A) dyads DLA1 ~ DLA5 . The excited-state bent-to-planar dynamics of DPAC regulate the donor's energy gap, while the acceptors A1 ~ A5 are endowed with different energy gaps and HOMO/LUMO levels. As a result, the rate and efficiency of the excited-state electron transfer versus energy transfer can be finely harnessed, which is verified via the steady-state spectroscopy and time-resolved emission measurements. Read More

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http://dx.doi.org/10.1002/anie.202005466DOI Listing

Single-molecule 3D orientation imaging reveals nanoscale compositional heterogeneity in lipid membranes.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Washington University in Saint Louis, Electrical and Systems Engineering, 1 Brookings Dr, Campus Box 1042, 63130, St. Louis, UNITED STATES.

In soft matter, thermal energy causes molecules to continuously translate and rotate, even in crowded environments, thereby impacting the spatial organization and function of most molecular assemblies, such as lipid membranes. Directly measuring the orientation and spatial organization of large collections (>3000 molecules/µm 2 ) of single molecules with nanoscale resolution remains elusive. In this paper, we utilize SMOLM, single-molecule orientation localization microscopy, to directly measure the orientation spectra (3D orientation plus "wobble") of lipophilic probes transiently bound to lipid membranes, revealing that Nile red's (NR) orientation spectra are extremely sensitive to membrane chemical composition. Read More

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http://dx.doi.org/10.1002/anie.202006207DOI Listing

Beyond polysulfides shuttle and Li dendrite formation: addressing the sluggish S redox kinetics for practical high energy Li-S batteries.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Argonne National Laboratory, Chemical Sciences & Engineering Division, 9700 South, Cass Ave, 60439, Argonne, UNITED STATES.

Electrolyte modulation has been reported to simultaneously suppress polysulfide shuttle effect and lithium dendrite formation of lithium-sulfur (Li-S) batteries. However, the sluggish S redox kinetics, especially under high S loading and lean electrolyte operation, has been intensively ignored, which dramatically limits the cycle life and energy density of practical Li-S pouch cells. Herein, we demonstrate that a rational combination of selenium doping, core-shell hollow host structure, and fluorinated ether electrolytes enables ultrastable Li stripping/plating and essentially no polysulfide shuttle as well as fast redox kinetics. Read More

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http://dx.doi.org/10.1002/anie.202007159DOI Listing

A General Approach to O-Sulfation via Sulfur(VI) Fluoride Exchange Reaction.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Boston College, Department of Chemistry, 2609 Beacon St., Merkert Chemistry Center 214B, 02467, Chestnut Hill, UNITED STATES.

O-Sulfation is an important chemical code widely existing in bioactive molecules, but the scalable and facile synthesis of complex bioactive molecules carrying O-sulfation remains challenging. Herein, we report a general approach to O-sulfation via the Sulfur (VI) Fluoride Exchange (SuFEx) reaction between aryl fluorosulfates and silylated hydroxyl groups. Efficient sulfate diester formation was achieved through systematic optimization of the electronic properties of aryl fluorosulfates. Read More

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http://dx.doi.org/10.1002/anie.202007211DOI Listing

HIP to be Square: Simplifying Nitridophosphate Synthesis in a Hot Isostatic Press.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Ludwig-Maximilians-Universitat Munchen, Department Chemie Lehrstuhl f. Anorganische Festkörperchemie, Butenandtstr. 5-13, 81377, München, GERMANY.

(Oxo)Nitridophosphates have recently been identified as a promising compound class for application in the field of solid-state lighting. Especially, the latest medium-pressure syntheses under ammonothermal conditions draw attention of the semi-conductor and lighting industry on nitridophosphates. In this contribution, we introduce hot isostatic presses as a new type of medium-pressure synthetic tool, further simplifying nitridophosphate synthesis. Read More

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http://dx.doi.org/10.1002/anie.202008570DOI Listing

Continuous Synthesis of Aryl Amines from Phenols Utilizing Integrated Packed-Bed Flow Systems.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Interdisciplinary Research Center for Catalytic Chemistry (IRC3), National Institute of Advanced Industrial Science and Technology (AIST), Central 5, Higashi 1-1-1, Tsukuba, Ibaraki, 305-8565, Japan.

Aryl amines are important pharmaceutical intermediates among other numerous applications. Herein, an environmentally benign route and novel approach to aryl amine synthesis using dehydrative amination of phenols with amines and styrene under continuous-flow conditions was developed. Inexpensive and readily available phenols were efficiently converted into the corresponding aryl amines, with small amounts of easily removable co-products (i. Read More

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http://dx.doi.org/10.1002/anie.202005109DOI Listing

Degradation of Structurally Defined Graphene Nanoribbons by Myeloperoxidase and Photo-Fenton Reaction.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Shanghai Jiao Tong University, School of Chemistry and Chemical Engineering, CHINA.

As an emerging member of the graphene family, structurally defined graphene nanoribbons (GNRs) have shown promising applications in various fields. The evaluation of the degradability of GNRs is particularly important for assessing the persistence level and risk of these materials in living organisms and the environment. However, there is a void in the study of the degradation of GNRs. Read More

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http://dx.doi.org/10.1002/anie.202008925DOI Listing

Unravelling the Enigma of Nonoxidative Conversion of Methane on Iron Single-Atom Catalysts.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Xi'an Jiaotong University, school of mechanical engineering, CHINA.

The direct, nonoxidative conversion of methane on silica-confined single-atom iron catalyst (Fe 1 ©SiO 2 ) by Bao et al . ( Science , 2014, 344 , 616) is a landmark discovery in catalysis science. However, the initially proposed gas-phase reaction mechanism has been much debated. Read More

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http://dx.doi.org/10.1002/anie.202003908DOI Listing

Exploiting Two-Dimensional Bi2O2Se for Trace Oxygen Detection.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Peking University, Room Number: A411, No.202 Chengfu Road, Haidian District, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P.R.CHINA, CHINA.

Two-dimensional (2D) materials host great potential for environmental gaseous molecules detection in the age of emerging Internet of things owing to their fascinating electronic properties, large surface-to-volume ratio and feasibility to high integration. However, it remains a challenge to develop trace oxygen sensing 2D materials and devices with low detection limit at sub-ppm range. Here, we exploit a high-preforming resistive-type trace oxygen sensor based on 2D high-mobility semiconducting Bi 2 O 2 Se nanoplates. Read More

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http://dx.doi.org/10.1002/anie.202006745DOI Listing

Interfacially Bridging Covalent Network Yields Hyperstable and Ultralong Virus-based Fibers for Engineering Functional Materials.

Angew Chem Int Ed Engl 2020 Jul 9. Epub 2020 Jul 9.

Emory University, Biomedical Engneering, UNITED STATES.

Virus and virus-like particles (VLPs) are very attractive biological subjects for self-assembly manipulation and templated synthesis of nanomaterials. However, the fundamental studies and applications are often constrained by problems associated with their structural weakness. Here we present a strategy of interfacially bridging covalent network within tobacco mosaic virus (TMV) VLPs to bring outstanding structural properties and functionalities. Read More

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http://dx.doi.org/10.1002/anie.202008670DOI Listing

Highly Efficient and Air Stable Lanthanide Eu(II) Complex: New Emitter in Organic Light Emitting Diodes.

Angew Chem Int Ed Engl 2020 Jul 8. Epub 2020 Jul 8.

Peking University, Chemistry, CHINA.

Luminescent Eu(II) complexes with characteristic 5d-4f transition have potential applications in many fields. However, their instability in ambient conditions impedes further exploration and application. Herein, we report two new Eu(II) complexes, bis[hydrotris(3-trifluoromethylpyrazolyl)borate]europium(II) ( Eu-1 ) and bis[hydrotris(3-methylpyrazolyl)borate]europium(II) ( Eu-2 ). Read More

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http://dx.doi.org/10.1002/anie.202008423DOI Listing

trans-Selective Aryldifluoroalkylation of Endocyclic Enecarbamates and Enamides via Nickel Catalysis.

Angew Chem Int Ed Engl 2020 Jul 8. Epub 2020 Jul 8.

Shanghai Institute of Organic Chemistry Chinese Academy of Science, Key Laboratory of Organofluorine Chemistry, 345 Lingling Lu, 200032, Shanghai, CHINA.

2-Pyrroline and 2-azetine are useful synthons for the synthesis of pyrrolidines and azetidines that widely exist in natural products, pharmaceuticals, and agrochemicals. But efficient methods for dicarbofuntionalization of these cyclic alkenes are limited. Particularly, the dicarbofunctionalization of endocyclic enecarbamates to achieve fluorinated compounds remains an unsolved issue, despite of the wide applications of organofluorinated molecules in life and materials science. Read More

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http://dx.doi.org/10.1002/anie.202008498DOI Listing

Micron-sized zeolite Beta single crystals featuring intracrystal interconnected ordered macro-meso-microporosity displaying superior catalytic performance.

Angew Chem Int Ed Engl 2020 Jul 8. Epub 2020 Jul 8.

Jilin University, Chemistry, 2699 Qianjin Street, 130012, Changchun, CHINA.

Serious diffusional limitations are frequently observed for the conversion of bulky molecules over conventional zeolite Beta crystals, which invoke for hierarchical structure to improve the mass transportation property and the accessibility to reactive sites. Zeolite single crystals with intracrystalline hierarchical porosity at macro-, meso- and micro-length scales is of great significance and provides the best solution . However, the construction of large zeolite Beta single crystals with such intracrystalline hierarchical porosity remains a critical challenge. Read More

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http://dx.doi.org/10.1002/anie.202007069DOI Listing

High-Fidelity End-Functionalization of Poly(ethylene glycol) Using Stable and Potent Carbamate Linkages.

Angew Chem Int Ed Engl 2020 Jul 8. Epub 2020 Jul 8.

University of Science and Technology of China, Department of Polymer Science and Engineering, 96 Jinzhai Road, 230026, Hefei, CHINA.

It is an open "secret" that commercial PEG-amine is of unreliable quality, for which we ascribe to both flawed manufacturing protocols and storage stability issues. In addition, conventional PEG functionalization relies on esterification and etherification steps, suffering from incomplete conversion, harsh reaction condition, and functional group incompatibility. To solve these practical challenges, we propose an efficient strategy for PEG functionalization through carbamate linkages. Read More

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http://dx.doi.org/10.1002/anie.202006687DOI Listing
July 2020
11.261 Impact Factor

Carrier-Free Delivery of Precise Drug-Chemogene Conjugates for Synergistic Treatment of Drug-Resistant Cancer.

Angew Chem Int Ed Engl 2020 Jul 8. Epub 2020 Jul 8.

Shanghai Jiao Tong University, School of Chemistry & Chemical Engineering, 800 Dongchuan Road, Shanghai Jiao Tong University, 200240, Shanghai, CHINA.

Combinatorial antitumor therapies using different chemodrug combo or chemo/gene agent combo emerge as promising ways to overcome the drug resistance, a major cause for the failure of cancer treatment. However, dramatic pharmacokinetic differences of adopted drugs greatly impede the combinatorial antitumor practices, raising the great demand of developing appropriate drug delivery systems (DDSs) for tumor treatment. By employing fluorescent dithiomaleimide (DTM) as a linker, herein, we conjugate two paclitaxel (PTX) molecules with a floxuridine (FdU)-integrated antisense oligonucleotide (termed as chemogene) to form a precise macromolecular drug-chemogene conjugate. Read More

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http://dx.doi.org/10.1002/anie.202006895DOI Listing

Borane-Catalyzed Chemoselective and Enantioselective Reduction of 2-Vinyl-Substituted Pyridines.

Angew Chem Int Ed Engl 2020 Jul 8. Epub 2020 Jul 8.

Nankai University, State Key Laboratory and Institute of Elemento-Organic Chemistry, 94 Weijin Rd, 300071, Tianjin, CHINA.

Herein, we report that highly chemoselective and enantioselective reduction of 2-vinyl-substituted pyridines has been achieved for the first time. The reaction, which uses chiral spiro-bicyclic bisboranes as catalysts and HBpin and an acidic amide as reducing reagents, proceeds via a cascade process involving 1,4-hydroboration followed by transfer hydrogenation of a dihydropyridine intermediate. The retained double bond in the reduction products permits their conversion to natural products and other useful heterocyclic compounds via simple transformations. Read More

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http://dx.doi.org/10.1002/anie.202007352DOI Listing

Endowing zeolite LTA superballs with multifold light manipulation ability.

Angew Chem Int Ed Engl 2020 Jul 7. Epub 2020 Jul 7.

Jilin University, Chemistry, Qianjin Street 2699, 130012, Changchun, CHINA.

Advances in zeolites research emerging from interdisciplinary efforts have opened new opportunities beyond conventional applications. Colloids drive much current research owing to their distinct collective behaviors , but so far, zeolite used as a colloidal building block to construct ordered superstructures remains unexplored. Here we show that self-assembly of colloidal zeolite LTA superball (ZAS) by tilted angle sedimentation forms macroscopic films with micro-mesoporosity and 3D long-range periodicity featuring a photonic bandgap (PBG) that is tunable by superball geometry and responds reversibly to chemical vapors. Read More

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http://dx.doi.org/10.1002/anie.202007064DOI Listing

Boosting Quantum Efficiency of Ultralong Organic Phosphorescence up to 52% via Intramolecular Halogen Bonding.

Angew Chem Int Ed Engl 2020 Jul 7. Epub 2020 Jul 7.

Sun Yat-sen University, No.135, Xingang W. Rd., 510275, Guangzhou, CHINA.

Ultralong organic phosphorescence (UOP) has attracted increasing attention due to its potential applications in optoelectronics, bioelectronics, and security protection. However, achieving UOP with high quantum efficiency (QE) over 20% is still full of challenges due to the forbidden intersystem crossing (ISC) and fast non-radiative transitions in organic molecules. Here, we present a novel strategy to enhance the QE of UOP materials by modulating intramolecular halogen bonding via structural isomerism. Read More

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http://dx.doi.org/10.1002/anie.202007343DOI Listing

Hydrophobic organic electrolyte protected Zn anodes for aqueous Zn batteries.

Angew Chem Int Ed Engl 2020 Jul 7. Epub 2020 Jul 7.

University of Maryland, Department of Chemical & Biomolecular Engineering, 1223A Chemical and Nuclear Engineering, 20742, College Park, UNITED STATES.

Aqueous Zn batteries are promising energy-storage device due to low cost and high energy density. However, their lifespan is limited by irreversible Zn anodes due to water decomposition and Zn dendrite growth. Here, we separate aqueous electrolyte from Zn anode by coating a thin metal-organic framework (MOF) layer on anode and filling the pores of MOF with hydrophobic Zn(TFSI)2-tris(2,2,2-trifluoroethyl)phosphate (TFEP) organic electrolyte that is immiscible with aqueous Zn(TFSI)2-H2O bulk electrolyte. Read More

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http://dx.doi.org/10.1002/anie.202008634DOI Listing

Solvation Rule for Solid-Electrolyte Interphase Enabler in Lithium Metal Batteries.

Angew Chem Int Ed Engl 2020 Jul 7. Epub 2020 Jul 7.

Argonne National Laboratory, Chemical Sciences & Engineering Division, 9700 South, Cass Ave, 60439, Argonne, UNITED STATES.

Despite the exceptionally high energy density of lithium metal anodes, the practical application of lithium metal batteries (LMBs) is still impeded by the instability of the interphase between the lithium metal and the electrolyte. To formulate a functional electrolyte system that can stabilize the lithium metal anode, one must understand the solvation behavior of the solvent molecules since the electrochemical properties of a solvent can be heavily influenced by its solvation status. We unambiguously demonstrated the solvation rule for the solid-electrolyte interphase (SEI) enabler in an electrolyte system. Read More

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http://dx.doi.org/10.1002/anie.202008081DOI Listing

-Recoding Cancer Epigenome by Intervening Metabolism and Iron Homeostasis with Mitochondria-Targeted Re(I) Complexes.

Angew Chem Int Ed Engl 2020 Jul 7. Epub 2020 Jul 7.

School of Chemistry, Sun Yat-Sen University, Chemistry Department, No. 135 Xingang Xi Road, 510275, Guangzhou, CHINA.

The development and malignancy of cancer cells are closely related to the changes of epigenome. In this work, a mitochondria-targeted rhenium(I) complex ( DFX-Re3 ) integrating the clinical iron chelating agent deferasirox ( DFX ) has been designed. By relocating iron to mitochondria and changing the key metabolic species related to epigenetic modifications, DFX-Re3 can elevate the methylation levels of histone, DNA and RNA. Read More

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http://dx.doi.org/10.1002/anie.202008624DOI Listing

Synthesis of robust MOFs@COFs porous hybrid materials via aza-Diels-Alder reaction: towards high performance supercapacitor materials.

Angew Chem Int Ed Engl 2020 Jul 7. Epub 2020 Jul 7.

Universite de Strasbourg, ISIS, Strasbourg, FRANCE.

Metal-organic frameworks (MOFs) and covalent organic frameworks (COFs) attracted enormous attention in recent years. Recently, MOF@COF are emerging as hybrid architectures combining the unique features of the individual components to enable the generation of materials displaying novel physicochemical properties. Herein we report an unprecedented use of aza-Diels-Alder cycloaddition reaction as postsynthetic modification of MOF@COF-LZU1, to generate aza-MOFs@COFs hybrid porous materials with extended π-delocalization. Read More

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http://dx.doi.org/10.1002/anie.202008408DOI Listing

Recent Advances of Synthetic Macrocycle-Based Nonporous Adaptive Crystals for Molecular Separation.

Angew Chem Int Ed Engl 2020 Jul 7. Epub 2020 Jul 7.

Jilin University, College of Chemistry, 2699 Qianjin Street, 130012, Changchun, CHINA.

The exploitation of new materials for adsorptive separation of industrially important hydrocarbons is of great importance in both scientific research and petrochemical industry. Nonporous adaptive crystals (NACs) as a robust class of synthetic materials have drawn much attention during the past five years for their superior performance in adsorption and separation. Pillararenes are the main family of macrocyclic arenes used for NACs construction, where the structure-function relationship has been intensively studied. Read More

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http://dx.doi.org/10.1002/anie.202006999DOI Listing

Engineered Anisotropic Fluids of Rare Earth Nanomaterials.

Angew Chem Int Ed Engl 2020 Jul 7. Epub 2020 Jul 7.

Tsinghua University, Department of Chemistry, Shuangqing road, 100084, Beijing, CHINA.

The self-assembly of inorganic nanoparticles into well-ordered structures in the absence of solvents is generally hindered by van der Waals forces, leading to random aggregates between them. To address the problem, we functionalized rigid rare earth (RE) nanoparticles with a layer of flexible polymers by electrostatic complexation. Consequently, an ordered and solvent-free liquid crystal (LC) state of RE nanoparticles was realized. Read More

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http://dx.doi.org/10.1002/anie.202007676DOI Listing

Multiexcitonic Triplet Pair Generation in Oligoacene Dendrimers as Amorphous Solid-state Miniatures.

Angew Chem Int Ed Engl 2020 Jul 7. Epub 2020 Jul 7.

Yonsei University, Chemistry, Seodaemoon ku,shinchon dong, 120-749, Seoul, KOREA, REPUBLIC OF.

Singlet fission in organic semiconducting materials has attracted great attention for the potential application in photovoltaic devices as the exciton multiplication process effectively compensates for thermal energy losses. Research interests have been concentrated on identifying working mechanisms of coherent SF processes in crystalline solids as ultrafast SF is hailed for efficient multiexciton generation. However, as long lifetime of the intermediate state, multiexcitonic triplet pair, in amorphous solids facilitates the decorrelation process for triplet exciton extractions, a precise examination of incoherent SF processes is demanded in delicate model systems to represent heterogeneous structures. Read More

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http://dx.doi.org/10.1002/anie.202008533DOI Listing