Supramolecular eutectogels are an emerging class of materials that offer a new opportunity for generating functional gel materials in biocompatible anhydrous or low‐water media. Two guanosine‐based supramolecular G4 eutectogels with high ionic conductivity and solvent‐induced chiral inversion were developed that can be applied to fabricate a flexible electrochromic device. Abstract Supramolecular eutectogels, an emerging class of materials that have just developed very recently, offer a...
Tue Aug 18, 2020 10:47
The reaction between α,β‐unsaturated lactones and 1,3‐dienes looks like a Diels–Alder reaction, but it is a vinylogous Michael addition as indicated by experimental results and DFT calculations. A short sequence was established accessing (natural) mellein and angelicoin derivatives. Abstract The reactions of α,β‐unsaturated δ‐lactones with activated dienes such as 1,3‐dimethoxy‐1‐[(trimethylsilyl)oxy]‐1,3‐butadiene (Brassard's diene) are barely known in literature and show high potential...
Tue Aug 18, 2020 10:47
A highly active and extremely stable Al2O3 modified Pd/MgAl2O4 catalyst was developed via forming epitaxially matched Pd‐MgAl2O4 interface and adding irreducible oxide to alter the reducibility of PdO. The study provides new insight into the interaction between Pd and oxide on CH4 combustion, offering an avenue to construct stable and active combustion catalysts for industrial application. Abstract Catalytic combustion is promising in removing trace amounts of CH4 to address serious environmental...
Tue Aug 18, 2020 10:47
A class of precisely aligned flexible‐on‐rigid hybrid‐phase MOFs were synthesized by the heteroepitaxially growth of acs‐topology MOF on the surface of fcu‐topology MOF. Domain‐selective loading of multiple guests into the hybrid‐phase MOFs was achieved by size‐selective encapsulation or selective binding. A dual‐drug delivery system with controllable loading ratio and release kinetics was developed based on the hybrid‐phase MOF. Abstract Multi‐component MOFs contain multiple sets of unique...
Tue Aug 18, 2020 10:47
By employing a single‐crystal‐to‐single‐crystal post‐synthetic transformation, electrical‐ and photo‐conductivity were activated by cation exchanges of dimethylammonium with tetrathiafulvalenium (TTF.+) and N,N′‐dimethyl‐4,4′‐bipyridinium (MV2+) into a redox‐active metal–organic framework containing TTF‐tetrabenzoate, (Me2NH2)[InIII(TTFTB)]⋅0.7 C2H5OH⋅DMF. Abstract To activate electronic and optical functions of the redox‐active metal–organic framework, (Me2NH2)[InIII(TTFTB)]⋅0.7 C2H5OH⋅DMF...
Tue Aug 18, 2020 10:47
A series of solvent‐free thermotropic liquid crystals are fabricated by the introduction of a flexible layer around the rigid core of rare‐earth nanomaterials. All of the engineered anisotropic fluids show typical nematic LC phases with size‐ and shape‐dependent microstructure. Such intrinsic ordering and fluidity endow these materials with unique anisotropic luminescence properties. Abstract The self‐assembly of inorganic nanoparticles into well‐ordered structures in the absence of solvents...
Tue Aug 18, 2020 10:47
The effective degradation of structurally defined graphene nanoribbons (GNRs) was achieved by the enzymatic action of human myeloperoxidase and the photo‐Fenton reaction. These findings ensure the potential applications of GNRs in a wide range of fields. Abstract 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...
Tue Aug 18, 2020 10:47
The intracellular delivery of a bacterial effector phospho‐lyase OspF by using AMPA‐O16B lipid‐based nanoparticles for rewiring malignant cell signaling is presented. Irreversible inactivation of ERK, the terminal component of the MAPK signaling cascade, enables efficient tumor suppression in vitro and in vivo and modulates macrophages immune responses. Abstract The abundance of bacterial effectors have inspired us to explore their potential in rewiring malignant cell signaling. Their incapability...
Tue Aug 18, 2020 10:47
Storage‐stable and air‐insensitive PEG‐amine with high‐fidelity functionality was constructed via integrating carbamate linkage with finely tuned amine basicity. The carbamate strategy provides a general approach towards PEG derivatives with diverse functionalities. Carbamate linkage at the diblock junction facilitates self‐assembly into higher‐order nanostructures with improved stability towards both hydrolysis and drug encapsulation. Abstract Commercial PEG‐amine is of unreliable quality,...
Tue Aug 18, 2020 10:47
Functionalize through thiiranium ions: Sulfenyl group transfer to alkenes has emerged as a versatile tool for introduction of organosulfur moieties into molecules with high stereochemical control. Understanding the structure, formation, stability, and reactivity of the key intermediate thiiraniium ion, led to the development of catalytic enantioselective sulfenofunctionalizations highlighted in this Review. Abstract The last decade has witnessed a burgeoning of new methods for the enantioselective...
Tue Aug 18, 2020 10:47
A separation‐sensing membrane is constructed into a heterogeneous nano‐architecture wherein a nanoporous surface layer continuously extracts serum and the biosensing nanochannels underneath dynamically detect the biotarget fluctuation, thereby achieving online and dynamic tests of various vital clinical indices during blood drawing in patients from a variety of medical scenarios, including liver transplantation and endometrial cancer. Abstract Dynamic and on‐site analysis of serum from...
Tue Aug 18, 2020 10:47
A meta junction is introduced to promote efficient TADF in D‐A conjugated polymers. As a result of the enhanced hole–electron separation, the singlet–triplet energy splitting (ΔE ST) is found to be significantly decreased from 0.44 eV to 0.10 eV with the para‐to‐meta modification. A strong delayed fluorescence is achieved for the meta‐linked polymer, revealing a peak EQE of 15.4 % in solution‐processed devices. Abstract The meta junction is proposed to realize efficient thermally activated...
Tue Aug 18, 2020 10:47
Lexapeptide is a lantibiotic showing potent antibacterial activity against Gram‐positive bacteria such as MRSA and MRSE, featured by the lanthionine (Lan) and d‐Ala formation in its structure. The formation of Lan is catalyzed by a class V lanthionine synthetase comprised of three standalone proteins. The d‐Ala28 is installed by the F420H2‐dependent reductase LxmJC, which can introduce d‐stereocenters into lanthipeptides. Abstract Lantibiotics are a type of ribosomally synthesized and post‐translationally...
Tue Aug 18, 2020 10:47
Highly Concentrated Electrolyte towards Enhanced Energy Density and Cycling Life of Dual‐Ion Battery
A 7.5 mol kg−1 LiFSI highly concentrated electrolyte was developed for a dual‐ion battery (DIB). A proof‐of‐concept DIB based on this concentrated electrolyte exhibits a discharge capacity of 94.0 mAh g−1 at 200 mA g−1, 96.8 % capacity retention after 500 cycles, and an energy density up to approximately 180 Wh kg−1 based on the electrode materials and electrolyte, which is among the best performances of previously reported DIBs. Abstract Dual‐ion batteries (DIBs) have attracted much attention...
Tue Aug 18, 2020 10:47
2D single‐crystal Bi2O2Se nanoplates show a unique surficial amorphous Se atomic layer and an improved specific surface area for efficient adsorption and detection of trace oxygen. 2D Bi2O2Se‐based oxygen sensor presents ultrahigh sensitivity of 0.25 ppm detection minimum, wide‐range response, strong selectivity, good stability, and high durativity at room temperature. Abstract We exploit a high‐performing resistive‐type trace oxygen sensor based on 2D high‐mobility semiconducting Bi2O2Se...
Tue Aug 18, 2020 10:47
Organics materials are considered a promising alternative to inorganic electrode materials in the construction of aqueous batteries because they possess tunable structures, are renewable, and they can be environmentally benign. This article reviews the latest advances in carbonyl‐containing organics applied to aqueous electrolytes in energy storage and conversion. The discussion addresses the challenges remaining before such materials may be widely applied. Abstract Aqueous batteries using...
Tue Aug 18, 2020 10:47
An activatable dCas9 transcriptional circuit is designed utilizing the strategy of hybridization‐mediated structure switching for gRNA activation. The designed circuit enables sensing and silencing of mRNA in living cells. Abstract CRISPR‐dCas9 systems that are precisely activated by cell‐specific information facilitate the development of smart sensors or therapeutic strategies. We report the development of an activatable dCas9 transcriptional circuit that enables sensing and silencing...
Tue Aug 18, 2020 10:47
Esters are synthesized from phenols and aldehydes through coupling of phenoxyl and acyl radicals that are transiently generated. The reaction offers a convenient method to specifically acylate phenolic hydroxyl groups in the presence of aliphatic groups. Abstract A convenient method is reported to specifically acylate phenolic hydroxyl groups through a radical pathway. When a mixture of an aldehyde and a phenol in ethyl acetate is irradiated with blue light in the presence of iridium and...
Tue Aug 18, 2020 10:47
Proton as a charge carrier offers a vast potential for battery systems with characteristics of high power and long longevity. Herein, we report a non‐aqueous proton electrolyte of anhydrous H 3 PO 4 solvated in acetonitrile for proton batteries, which facilitates stable cycle performance of electrode materials that otherwise lose capacity rapidly in aqueous electrolytes.
Mon Aug 17, 2020 22:40
Molecular photoswitches enable the reversible external control of biological systems, nanomachines, and smart materials. Recently, their developments are driven by the need for low energy (green‐red‐NIR) light switching, to allow for non‐invasive operation with deep tissue‐penetration. The lack of clear design principles for the adaptation and optimization of such systems strongly limits further applications. Here we provide such design rulebook for tetra‐ ortho ‐chloroazobenzenes, an emerging...
Mon Aug 17, 2020 22:00
The structure of titanium defective sites in TS‐1 is disclosed by deciphering the experimental results from electronic spectroscopies (UV/Vis, K‐edge XAS and L2,3‐edge NEXAFS) on the basis of quantum mechanical simulation of the spectroscopic observables. Within six considered models, isolated Ti sites with hexacoordinated geometry are revealed as the most probable structural motif for Ti defects in TS‐1 samples. Abstract Ti silicates, and in particular, titanium silicalite‐1 (TS‐1), are...
Mon Aug 17, 2020 21:58
One fits all: Co/Co3O4 core–shell nanoparticles prepared by pyrolysis of a Co‐pyromellitic acid template on silica served as stable and reusable catalysts for the selective hydrogenation of pyridines, quinolines, and other heteroarenes. Abstract Herein, we report the synthesis of specific silica‐supported Co/Co3O4 core–shell based nanoparticles prepared by template synthesis of cobalt‐pyromellitic acid on silica and subsequent pyrolysis. The optimal catalyst material allows for general...
Mon Aug 17, 2020 21:58
Reaction of CsF and ClF3 at low temperatures gives the compound Cs[Cl3F10] which crystallizes in a very rarely observed A[5]B[5] structure type. A propeller‐shaped [Cl3F10]− anion with a μ3‐bridging fluorine atom is present in the salt. Quantum‐chemical calculations show that the interaction of the ClF3 subunits with the μ3‐bridging fluorine atom are weak and the Cl−F bonds are essentially ionic. Abstract Reaction of CsF with ClF3 leads to Cs[Cl3F10]. It contains a molecular, propeller‐shaped...
Mon Aug 17, 2020 21:57
Micellar shape changes of sodium dodecyl sulfate are associated with different binding modes of the counterions. Morphological changes are caused by symmetry breaking of the irreducible building blocks, with the formation of transient surfactant dimers mediated by the counterions that promote the stabilization of cylindrical instead of spherical micelles. Abstract The shape and size of self‐assembled structures upon local organization of their molecular building blocks are hard to predict...
Mon Aug 17, 2020 21:57
Analysis of the use of differential scanning calorimetry (DSC) for thermal hazard assessment in 2019 shows some alarming trends. Many reports are not reproducible, do not follow established best practices and the conclusions drawn are not supported by the data presented. This Viewpoint discusses these issues and offer simple guidance on how to avoid them. Abstract Differential scanning calorimetry (DSC) is increasingly used as evidence to support a favourable safety profile of novel chemistry,...
Mon Aug 17, 2020 21:54
A bent/planar dual‐channel donor was introduced to establish new donor–linker–acceptor (D–L–A) dyads in which the excited‐state bent‐to‐planar structure relaxation of the donor can be used as a clock to harness the electron/energy‐transfer processes. Several new D–L–A structures were designed and synthesized by tuning the energy gaps and frontier‐orbital levels of the acceptors. Abstract Herein, we introduce the cyclic 8π‐electron (C8π) molecule N,N′‐diaryl‐dihydrodibenzo[a,c]phenazine...
Mon Aug 17, 2020 21:52
31P NMR spectra are highly sensitive to the morphology of high‐density lipoprotein nanoparticles when oriented on glass surfaces. The spectra reveal new molecular insights that are relevant to the protective function of the lipoprotein nanoparticles against cardiovascular disease. Abstract The biological function of high‐density lipoprotein (HDL) nanoparticles, the so‐called good cholesterol that is associated with a low risk of heart disease, depends on their composition, morphology, and...
Mon Aug 17, 2020 21:51
An efficient copper‐catalyzed cascade cyclization of azide‐ynamides via α‐imino copper carbene intermediates is disclosed, enabling divergent synthesis of polycyclic N‐heterocycles in generally good to excellent yields with broad substrate scope and excellent diastereoselectivities, representing the first generation of α‐imino copper carbenes directly from alkynes. The asymmetric azide–ynamide cyclization has been achieved with high enantioselectivities. Abstract Here an efficient copper‐catalyzed...
Mon Aug 17, 2020 21:51
MIL‐100(Fe) is demonstrated to serve as an ideal “SERS‐active” and “sensory array” platform for multiplex sensing of volatile organic compounds (VOCs) as well as the gaseous biomarkers of diseases with low Raman cross‐section. Abstract The application of metal–organic frameworks (MOFs) as SERS‐active platforms in multiplex volatile organic compounds (VOCs) detection is still unexplored. Herein, we demonstrate that MIL‐100 (Fe) serves as an ideal SERS substrate for the detection of VOCs....
Mon Aug 17, 2020 21:51
Diphenyl sulfide can be used as an axial ligand for tetraphenylporphyrin cobalt. The axial coordination promotes the redox activity of tetraphenylporphyrin cobalt immobilized onto graphene surface through van der Waals interaction, and facilitates the generation of a reduced state of tetraphenylporphyrin cobalt to serve as the active site for electrochemical CO2 reduction. Abstract Efficient electron communication between molecular catalyst and support is critical for heterogeneous molecular...
Mon Aug 17, 2020 21:50
A synergistic enhancement strategy is realized for ultralong bright RTP, involving polymerization between phosphor monomers and acrylamide and host–guest complexation interaction between phosphors and cucurbit[6, 7, 8]urils (CB[6, 7, 8]). The phosphorescence lifetime and efficiency is up to 2.81 s and 76 %. Multiple lifetime‐encoding for digit and character encryption are achieved. Abstract An enhancement strategy is realized for ultralong bright room‐temperature phosphorescence (RTP),...
Mon Aug 17, 2020 21:48
Hot isostatic pressing is introduced as easy and fast synthetic access to nitridophosphate phosphors, while providing large‐scale quantities. In particular, the calcium nitridophosphate Ca2PN3:Eu2+ was synthesized under medium‐pressure conditions (150 MPa N2, 1200 °C), revealing single crystals with remarkable size (>100 μm) and quality. Further, Ca2PN3:Eu2+ shows a rather narrow deep‐red emission and notable high internal quantum efficiency. Abstract (Oxo)Nitridophosphates have recently...
Mon Aug 17, 2020 21:45
A multifunctional COF‐based nanoagent, which is equipped with BODIPY‐2I photosensitizer, CaCO3 nanoparticle, and glycosaminoglycan (GAG) targeting agent, can be a highly efficient and selective antitumor nanomedicine for colon tumor via photodynamic therapy (PDT) and Ca2+ overload synergistic therapy. Abstract Ca2+, a ubiquitous but nuanced modulator of cellular physiology, is meticulously controlled intracellularly. However, intracellular Ca2+ regulation, such as mitochondrial Ca2+ buffering...
Mon Aug 17, 2020 21:44
A universal irregular‐type mesostructured nanounit assembly method is developed to form hierarchically macro‐/mesoporous polymer and carbon nanoshells on various functional materials. With structural and compositional advantages, Fe,N‐doped porous carbon nanoshells exhibit enhanced electrocatalytic performance for the oxygen reduction reaction in an alkaline electrolyte. Abstract Mesoporous core–shell nanostructures with controllable ultra‐large open channels in their nanoshells are of...
Mon Aug 17, 2020 21:44
Hydrogenase mimic encapsulation in M12L24 nanospheres allows to create a special environment around synthetic mimics leading to a reduction of the proton reduction overpotential by 250 mV at the expense of catalytic rates while the creation of a proton‐rich environment leads to catalytic rates that are two orders of magnitude higher than without substrate preorganization. Abstract Hydrogenase enzymes are excellent proton reduction catalysts and therefore provide clear blueprints for the...
Mon Aug 17, 2020 21:44
Biocatalysis has developed into a mature technology for chemical and pharmaceutical synthesis as well as other areas where high selectivity and mild reaction conditions are required. This Review highlights recent achievements with a special focus on industrialized applications including the introduction of key performance indicators (KPIs) to judge the efficiency of enzymes. Abstract Biocatalysis has found numerous applications in various fields as an alternative to chemical catalysis....
Mon Aug 17, 2020 21:44
An impossible triangle? Iodine(III) promotes the α‐cyclopropanation of simple ketone derivatives. Mechanistic studies reveal that an unusual intermediate might be involved. Abstract The reactivity of iodine(III) reagents towards nucleophiles is often associated with umpolung and cationic mechanisms. Herein, we report a general process converting a range of ketone derivatives into α‐cyclopropanated ketones by oxidative umpolung. Mechanistic investigation and careful characterization of side...
Mon Aug 17, 2020 21:43
Understanding how cells regulate their bioenergetic demands, adjust to the microenvironment, or respond to stimuli is the aim of molecular biology. Yet, methods able to describe the molecular content, histological identity, and spatial context of a single cell do not exist. The presented method integrates morphometric image analysis to delineate and classify individual cells with their cell‐specific molecular profiles obtained by MALDI‐MSI. Abstract The large‐scale and label‐free molecular...
Mon Aug 17, 2020 21:41
A protein‐based biosensor architecture was designed to leverage protein folding. The sensor can discriminate between different peptide ligands and responds rapidly and quantitatively to its target even when challenged directly in undiluted whole blood. As this sensor architecture is likely compatible with many proteins, it has the potential to drastically widen the chemical space accessible to reagentless, real‐time electrochemical biosensors. Abstract The ability to monitor drug and biomarker...
Mon Aug 17, 2020 21:40
A design strategy is proposed that plants immobile repulsion centers near the diffusion channel to achieve faster ionic diffusion in superionic conductors. The repulsion centers locally induce the formation of high‐energy sites, leading to a fast track for ionic diffusion. One order of magnitude higher ionic conductivity is obtained by simply doping Cs ions as the repulsion centers in the model system Na11Sn2PS12. Abstract The successful launch of solid‐state batteries relies on the discovery...
Mon Aug 17, 2020 21:39
A JMV594‐conjugated iridium(III) complex is presented as a long‐lived, potent and selective imaging probe for GRPr in GRPr‐positive living cancer cells. This probe enables the discrimination of GRPr‐positive cancer cells from normal cells, while it is also capable of probing the modulatory functions of GRPr in immune cells. Abstract Gastrin‐releasing peptide receptor (GRPr) plays proliferative and inflammatory roles in living systems. Here, we report a highly selective GRPr antagonist (JMV594)‐tethered...
Mon Aug 17, 2020 21:39
A highly enantio‐ and regioselective hydroarylation process of vinylarenes with aryl halides has been developed using a NiH catalyst and a new chiral bis imidazoline ligand. A broad range of structurally diverse, enantioenriched 1,1‐diarylalkanes, a structure found in a number of biologically active molecules, have been obtained with excellent yields and enantioselectivities under extremely mild conditions.
Mon Aug 17, 2020 20:12
Valuing diversity leads to scientific excellence, the progress of science and most importantly, it is simply the right thing to do. We can value diversity not only in words, but also in actions.
Mon Aug 17, 2020 18:05
An emerging class of heterostructures with unprecedented (photo)electrocatalytic behavior, involving the combination of fullerenes and low‐dimensional (LD) nanohybrids, is currently expanding the field of energy materials. The unique physical and chemical properties of fullerenes have offered new opportunities to tailor both the electronic structures and the catalytic activities of the nanohybrid structures. Here, we comprehensively review the synthetic approaches to prepare fullerene‐based hybrids...
Mon Aug 17, 2020 18:02
A catalytic enantioselective formal [2+2] cycloaddition between α‐halo acroleins and electronically diverse arylalkenes is described. In the presence of ( S )‐oxazaborolidinium cation as the catalyst, densely functionalized cyclobutanes containing two vicinal quaternary stereocenters were produced in high yield and high diastereoselectivities with excellent enantioselectivities. Mechanistic studies revealed that the cis isomer could be transformed into the trans isomer via an enantiocontrolled...
Mon Aug 17, 2020 14:06
Quasi‐two‐dimensional (2D) perovskites have been proved to be promising candidates for light generation owing to their high radiative rates. However, strong exciton‐phonon interactions caused by mechanical softening of the surface act as a bottleneck in improving their suitability for a wide range of lighting and display applications. Moreover, it is not easily available to tune the phonon interactions in bulk films. Here, we adopt bottom‐up fabricated blue emissive perovskite nanoplatelets (NPLs)...
Mon Aug 17, 2020 11:05
Fine mechanics: A systematic experimental and computational study explains why tiny structural changes in the extremities of a molecular axle can allow or prevent its insertion in the cavity of a macrocycle. These results provide guidelines to design interlocked molecules with predetermined dynamic features, that can be used to make nanostructured machines, motors and materials. Abstract The general principles guiding the design of molecular machines based on interlocked structures are...
Mon Aug 17, 2020 11:0No more articles here.
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