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Self‐assembly is important for creating photonic structures, and structural color is tunable typically relying on size‐varied building blocks obtained by time‐consuming chemical synthesis. Herein, molecular conformation of bottlebrush block copolymers (BBCPs) in solution is successfully manipulated to create libraries of photonic structures . Amphiphilic BBCPs bearing oxidation‐responsive ferrocene groups on the hydrophilic block are used to fabricate porous particles via evaporation‐induced self‐assembly of water‐in‐oil‐in‐water (O/W/O) double emulsions stabilized by the BBCP surfactant. In‐situ oxidation of the ferrocene groups by hydrogen peroxide at the W/O interface leads to enhanced hydrophilicity, more hydration, and chain extension
Transient signaling orchestrates complex spatiotemporal behaviour in living organisms via (bio)chemical reaction networks (CRNs). Compartmentalization of signal‐processing is an important aspect for controlling such networks. However, artificial CRNs mostly focus on homogeneous solutions to program autonomous self‐assembling systems, which limits their accessible behaviour and tuneability. Here, we introduce layered compartments housing antagonistic pH‐modulating enzymes, and demonstrate that transient pH signals in a supernatant solution can be programmed based on spatial delays. This overcomes limitations of activity mismatches of antagonistic enzymes in solution and allows to flexibly program acidic and alkaline pH lifecycles beyond poss.
The construction of artificial structures through hierarchical self‐assembly via noncovalent interactions, as well as the monitoring during self‐assembly process, play significant roles in dynamic supramolecular chemistry. We managed complex dynamics of newly designed chiral N,N’‐diphenyl‐dihydrodibenzo[a,c]phenazines derivatives (S)/®‐DPAC that involved different assemblies with distinct optical and morphological characteristics. With the ratiometric fluorescence originated from the vibration‐induced emission (VIE) feature, the self‐assembly process from the kinetic traps to the thermodynamic equilibrium state can be real‐timely monitored by optical spectrometry effectively. Besides, accompanying with the morphology transformation from par.
A new approach to C–S couplings is reported that relies on nickel catalysis under mild conditions, enabled by micellar catalysis in recyclable water as reaction medium. The protocol tolerates a wide range of heteroaromatic halides and thiols, including alkyl and heteroaryl thiols, leading to a variety of thioethers in good isolated yields. The method is scalable, results in low residual metal in the products, and is applicable to syntheses of targets in the pharmaceutical area. The procedure also features an associated low E Factor, suggesting a far more attractive entry than is otherwise currently available, especially those based on unsustainable loadings of Pd catalysts.
Υ‐Glutamyltranspeptidase (GGT) is overexpressed in several types of cancer. Existing GGT‐targeting fluorescence probes can image these cancers, but the fluorescent hydrolysis product leaks from the target cancer cells during prolonged incubation or fixation. Here, we present a functionalized fluorescence probe for GGT, 4‐CH 2 F‐HMDiEtR‐gGlu, which is designed to generate an azaquinone methide intermediate during activation by GGT; this intermediate reacts with intracellular nucleophiles to generate a fluorescent adduct that is trapped inside the cells, without loss of the target enzyme activity. Application of the probe to patient‐derived xenograft (PDX) mice enabled in vivo cancer imaging for a prolonged period, and was also compatible wit.
Polar materials attract wide research interest due to their unique properties, such as ferroelectricity and the bulk photovoltaic effect (BPVE), which are not accessible with nonpolar materials. However, in general, rationally designing polar materials is difficult because nonpolar materials are more favorable in terms of dipoledipole interactions. Here, we report a rational strategy to form polar assemblies with bowl‐shaped π‐conjugated molecules and a molecular design principle for this strategy. We synthesized and thoroughly characterized 12 single crystals with the help of various theoretical calculations. Furthermore, we demonstrated that it can be possible to predict whether polar assemblies become more favorable or not by estimating
Amyloid proteins such as amyloid‐β peptide (Aβ) assemble into both rigid amyloid fibrils and metastable oligomers termed AβO or protofibrils. In Alzheimer’s disease, Aβ fibrils constitute the core of senile plaques, but Aβ protofibrils may represent the main toxic species. Aβ protofibrils accumulate at the exterior of senile plaques, yet the protofibril‐fibril interplay is not well understood. Applying chemical kinetics and atomic force microscopy to the assembly of Aβ as well as lysozyme, we observe that protofibrils bind to the lateral surfaces of amyloid fibrils. Utilizing Aβ variants with different critical oligomer concentrations we find that this interaction inhibits the autocatalytic proliferation of amyloid fibrils through secondary.
The mRNA modification m 6 A is associated with multiple roles in cell function and disease. The methyltransferases METTL3‐METTL14 and METTL16 act as “writers” for different target transcripts and sequence motifs. The modification is perceived by dedicated “reader” and “eraser” proteins, but not by polymerases. We report that METTL3‐14 shows remarkable cosubstrate promiscuity, enabling sequence‐specific internal labeling of RNA without additional guide RNAs. The transfer of ortho‐nitrobenzyl and 6‐nitropiperonyl groups allowed enzymatic photocaging of RNA in the consensus motif, which impaired polymerase‐catalyzed primer extension in a reversible manner. METTL16 was less promiscuous but suitable for chemo‐enzymatic labeling using different t.
(C 6 F 5 )Te(CH 2 ) 3 NMe 2 ( 1 ), a perfluoro­phe­nyltellurium deriva­tive capable of forming intra­molecular N∙∙∙Te interactions, was prepared and charac­terized. The donor‐free reference substance (C 6 F 5 )TeMe ( 2 ) and the unsupported adduct (C 6 F 5 )(Me)Te∙NMe 2 Et ( 2b ) were studied in parallel. Mole­cular structures of 1 , 2 and 2b were determined by single crystal X‐ray diffraction and for 1 and 2 by gas‐phase electron diffraction. The structure of 1 shows N∙∙∙Te distan­ces of 2.639(1) Å (solid) and 2.694(53) Å (gas). Ab initio plus NBO and QTAIM calculations show significant charge transfer effects within the N∙∙∙Te interactions and indicate sigma‐hole interactions.
To elevate the perf­­­­­­ormance of polymer solar cells (PSC) processed by non‐halogenated solvents, a dissymmetric fused‐ring acceptor BTIC‐2Cl‐γCF3 with chlorine and trifluoromethyl end groups has been designed and synthesized. X‐ray crystallographic data suggests that BTIC‐2Cl‐γCF3 has a 3D network packing structure as a result of synergistic H‐ and J‐aggregations between adjacent molecules, which will strengthen its charge transport as an acceptor material. When PBDB‐TF was used as a donor, the toluene‐processed binary device realized a high power conversion efficiency (PCE) of 16.31%, which was further improved to 17.12% when PC71ThBM was added as the third component. An efficiency of over 17% is currently the highest record among poly.
A highly enantio‐ and regioselective hydrosulfonylation of 1,3‐dienes with sulfonyl hydrazides has been realized by using palladium catalyst containing monodentate chiral spiro phosphoramidite ligand. The reaction provided efficient approach to the synthetically useful chiral allylic sulfones. Mechanistic studies suggest that the reaction proceeds through a formation of allyl hydrazine intermediate and subsequent rearrangement to the chiral allylic sulfone product. The transformation of the allyl hydrazine intermediate to the product is enantioselectivity‐determining step.
Nanomaterials with enzyme‐mimicking activity (nanozyme) are at the targeted frontier for therapeutic interventions. However, it still remains a formidable challenge to selectively kill tumor cells through enzymatic reactions, while leaving normal cells unharmed. Herein, a new strategy is presented by developing single‐site cascade enzymatic reaction for tumor‐specific therapy while avoiding off‐target toxicity to normal tissues. Copper hexacyanoferrate (Cu‐HCF) nanozyme with active single‐site copper exhibits cascade enzymatic activity (i.e., glutathione oxidase and peroxidase) within tumor microenvironment. Results show that Cu‐HCF single‐site nanozymes (SSNEs) first exert tumor‐specific glutathione oxidase ability through depleting intrac.
Metallic zinc is a promising anode candidate of aqueous zinc‐ion batteries due to its high theoretical capacity and low redox potential. However, Zn anodes usually suffer from dendrite and side reactions, which will degrade their cycle stability and reversibility. Herein, we developed an in‐situ spontaneously reducing/assembling strategy to assemble a thin and uniform MXene layer on the surface of Zn anodes. The MXene layer endows the Zn anode with a lower Zn nucleation energy barrier and a more uniformly distributed electric field through the favorable charge redistribution effect in comparison with pure Zn. Therefore, MXene‐integrated Zn anode exhibits obviously low voltage hysteresis and excellent cycling stability with dendrite‐free beh.
Using the DNA origami technique, we constructed a DNA nanodevice functionalized with small interference RNA (siRNA) within its inner cavity and the chemotherapeutic drug doxorubicin (DOX), intercalated in the DNA duplexes. The incorporation of disulfide bonds allows the triggered mechanical opening and release of siRNA in response to intracellular glutathione (GSH) in tumors to knockdown genes key to cancer progression. Combining RNA interference and chemotherapy, the nanodevice induced potent cytotoxicity and tumor growth inhibition, without observable systematic toxicity. Given its autonomous behavior, exceptional designability, potent antitumor activity and marked biocompatibility, this DNA nanodevice represents a promising strategy for
Zero‐dimensional (0D) hybrid metal halides are promising light emitters. However, it is still challenging to accurately design their structures with targeted photoluminescence properties. Here, high pressure is adopted to engineer the self‐trapped exciton (STE) emission of 0D (bmpy)9[ZnBr4]2[Pb3Br11] (bmpy: 1‐butyl‐1‐methylpyrrolidinium). Under initial compression, the simultaneous contraction and distortion of photoactive [Pb3Br11]5‐ vary the equilibrium of STE emissions between different excited states, tuning the emission color from yellow green to cyan. Notably, sufficient structural distortion under continuous compression leads to the formation of more and deeper STE states, exhibiting an unprecedented broadband white‐light emission. T.
Buried salt bridges widely exist in protein structures, but are rarely used in synthetic systems for molecular recognition in water. By mimicking the binding pocket of bioreceptors, we designed and synthesized a pair of endo ‐functionalized macrocyclic hosts with secondary ammoniums in a hydrophobic cavity. We found that these macrocycles are able to selectively recognize carboxylic acids in water through salt bridges and the hydrophobic effect. Moreover, it was demonstrated that these macrocyclic receptors can be used in CD‐based optical chirality sensing of chiral carboxylic acids and fluorescent sensing of phenylpyruvic acid – a biomarker for phenylketonuria. This research showcases that buried salt bridges can be effectively used by end.
The regio‐ and enantioselective (3+3) cycloaddition of nitrones with 2‐indolylmethanols was accomplished by the cooperative catalysis of hexafluoroisopropanol (HFIP) and chiral phosphoric acid (CPA). Using this approach, a series of indole‐fused six‐membered heterocycles were synthesized in high yields (up to 98%), with excellent enantioselectivities (up to 96% ee) and exclusive regiospecificity. This approach enabled not only the first organocatalytic asymmetric (3+3) cycloaddition of nitrones but also the first C3‐nucleophilic asymmetric (3+3) cycloaddition of 2‐indolylmethanols. More importantly, theoretical calculations elucidated the role of the cocatalyst HFIP in helping CPA control the reactivity and enantioselectivity of the reactio.
Long‐range electron transfer (ET) in metalloenzymes is a general and fundamental process governing activation and O 2 reduction. Lytic polysaccharide monooxygenases (LPMOs) are key enzymes for the oxidative cleavage of insoluble polysaccharides, but their reduction mechanism by cellobiose dehydrogenase (CDH), one of the most used enzymatic electron donors, via long‐range ET, is still an enigma. Using multiscale simulations, we reveal that interprotein ET between CDH and LPMO is mediated by the heme propionates of CDH and solvent waters. Interestingly, we find that oxygen binding to the copper center of LPMO is coupled with the long‐range interprotein ET. This process, which is spin‐regulated and enhanced by the presence of O 2 , directly le.

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