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Carbon nanotubes (CNTs) have unusual physical properties which are valuable for nanotechnology and electronics but the chemical synthesis of chirality‐ and diameter‐specified CNTs and π‐conjugated CNT segments is still a great challenge. Herein we report the selective synthesis, isolation, characterizations, and photophysical properties of two novel chiral conjugated macrocycles ([4]cyclo‐2,6‐anthracene, [4]CAn2,6) as (‐)/(+)‐(12,4) carbon nanotube segment. These conjugated macrocyclic molecules were achieved using a bottom‐up assembly approach and subsequent reductive elimination reaction. The hoop‐shaped molecules can be directly viewed by STM technique. In addition, chiral enantiomers with (‐)/(+)‐helicity of the [4]CAn2,6 were successfu.
The current research of thermally activated fluorescence (TADF) emitters is mainly based on the molecular levels, while the aggregation states of TADF emitters are to be explored deeply. Here we report two multifunctional emitters with simultaneous TADF, aggregation induced emission (AIE), and multicolor mechanochromic luminescence (MCL) features. Moreover, both emitters show polymorph‐dependent TADF emission. Crystal structure analysis reveals that the polymorphism is ascribed to the mutable conformations in different aggregation states. This work brings new insight into the TADF emitters from a perspective of aggregation states.
Two‐dimensional (2D) Ti 3 C 2 nanosheets have been widely used as co‐catalysts for photocatalysis. However, how 2D Ti 3 C 2 enhances the photocatalytic efficiency remains unclear. Here, we, for the first time, report that it is graphene quantum dots (GQDs) derived from Ti 3 C 2 , other than 2D Ti 3 C 2 itself, that play as the co‐catalyst for La 2 Ti 2 O 7 /Ti 3 C 2 (LTC) composites during the photocatalytic reaction. After modification of Ti 3 C 2 derivatives, the photocatalytic efficiency of La 2 Ti 2 O 7 is enhanced by 16 times in comparison with pure La 2 Ti 2 O 7 . Solid state NMR, Raman and HRTEM results firstly confirm the existence of GQDs in Ti 3 C 2 and LTC composites. These GQDs are formed during the chemical change from Ti 3 AlC.
We developed cobalt‐catalyzed highly ( E )‐selective cross‐dimerization of terminal alkynes with terminal silylacetylenes, tert ‐butylacetylene, or 1‐trimethylsilyloxy‐1,1‐diphenyl‐2‐propyne in the presence of dichlorocobalt(II) complex 1a bearing a sterically demanding 2,9‐bis(2,4,6‐triisopropylphenyl)‐1,10‐phenanthroline upon activation with two equivalents of EtMgBr, giving a variety of ( E )‐1,3‐enynes.
Zeise’s salt, KPt(C2H4)Cl3, was the first characterized organometallic compound; it was also the first olefin pi‐complex. But as it was discovered in 1827‐30 in the middle of a fight between Dumas on the one hand and Berzelius and Liebig on the other, defending the etherin (ethylene) and radical theories, respectively, Zeise was unavoidably drawn into the fierce and highly personal dispute. Although Zeise’s formulation as a compound containing ethylene was vindicated, the fight went on, with bitter enmity finally ending in friendship between Liebig and Dumas, and the initial friendship between Berzelius and Liebig ending in bitter enmity. This was a time when the theories of organic chemistry were being developed, before any clear understan.
It remains a challenge to precisely tailor the morphology of polymer monolayers to control charge transport. Herein, the effect of dissolution temperature ( T dis ) is investigated as a powerful strategy for morphology control. Low T dis s generate extended polymer aggregation in solution, and induce larger nanofibrils in a monolayer network with more pronounced π−π stacking. The field‐effect mobility of the corresponding monolayer transistors are significantly enhanced by 4 times compared to devices from high T dis with a value approaching 1 cm 2 V ‐1 s ‐1 . Besides, the solution kinetics reveal higher growth rate of aggregates at low T dis , and filtration experiments further confirm that the dependence of fibril width in monolayer on T d.
The 1,2,3‐triazole group is one of the most important connective linkers and functional aromatic heterocycles in modern chemistry. The boom in growth of 1,4‐disubstituted triazole products, in particular, since the early 2000’s, can be largely attributed to the birth of click chemistry and the discovery of the Cu(I)‐catalyzed azide‐alkyne cycloaddition (CuAAC). Yet the synthesis of relatively simple, albeit important, 1‐substituted‐1,2,3‐triazoles, has been surprisingly more challenging. We report a straightforward and scalable click‐inspired protocol for the synthesis of 1‐substituted‐1,2,3‐triazoles from organic azides and the bench stable acetylene‐surrogate, ethenesulfonyl fluoride (ESF). The new transformation tolerates a wide selectio.
An N‐confused phlorin isomer bearing a dipyrrin moiety at the α‐position of the confused pyrrole ring (1) was synthesized. PdII and BIII coordination at the peripheral prodigiosin‐like moiety of 1 afforded the corresponding complexes 2 and 3, respectively. Reflux of 2 in triethylamine (TEA) converted the meso‐phenyl to the PdII‐ coordinating phenoxy group to afford 4. Under the same conditions, TEA was linked to the α‐position of the dipyrrin unit in 3 as an N,N‐diethylaminovinyl group to afford 5 . Furthermore, peripheral coordination of BIII in 3 and 5 improved the planarity of the phlorin macrocycle and thus facilitated the coordination of AgIII at the inner cavity to afford 3‐Ag and 5‐Ag, respectively. These results provide an effective.
The iridium half‐sandwich complex [Ir(η 5 :κ 1 ‐C 5 Me 4 CH 2 py)(2‐phenylpyridine)]PF 6 is highly cytotoxic: ca. 15‐250x more potent than clinically used cisplatin in several cancer cell lines tested. Unequivocal determination of the intracellular fate of the compound is mandatory to rationalize its potency and improve metallodrug design. We have developed a correlative 3D cryo X‐ray imaging approach to specifically localize the iridium distribution within the whole hydrated cell at nanometer resolution. By means of cryo soft X‐ray tomography (cryo‐SXT), which provides the cellular ultrastructure at 50 nm resolution, and cryo hard X‐ray fluorescence tomography (cryo‐XRF), which provides the elemental sensitivity with a 70 nm step size, we
Getting into shape: This Minireview gives a summary of the latest progress in characterizing and modeling the equilibrium shape of metal nanoparticles (NPs) in reactive environments through the combination of state‐of‐the‐art in situ environmental transmission electron microscopy (ETEM) experiments and the multiscale structure reconstruction (MSR) model. Abstract. The shape of metal nanoparticles (NPs) is one of the key factors determining their catalytic reactivity.
Transition metal phosphonates present great potential in catalysis and other applications due to their versatile coordination chemistry and flexible structures. However, many of them grow into dense crystals with low practical use in catalysis. To circumvent this, a simple solvent ligation effect was successfully used to disrupt the growth of a model compound, Fe[(OH)(O 3 P(CH 2 ) 2 CO 2 H)]×H 2 O (MIL‐37), into the extended 2D structure by replacing water with dimethylformamide (DMF) as the solvent during the synthesis. Due to the lack of ‐OH group which provides the corner‐sharing (binding) oxygen atoms for the octahedra, amorphous and porous structure is formed. When Fe 3+ is partially replaced by Ni 2+ , the amorphous structure remains
Oxylipins are key lipid mediators of important brain processes, including pain, sleep, oxidative stress and inflammation. For the first‐time, an in‐depth profile of up to 52 oxylipins can be obtained from the brains of awake moving animals using in vivo solid‐phase microextraction (SPME) chemical biopsy tool in combination with liquid chromatography – high resolution mass spectrometry. Among these, 23 oxylipins are detectable in the majority of healthy wildtype samples. This new approach successfully eliminates the changes in oxylipin concentrations routinely observed during the analysis of post‐mortem samples, allows time‐course monitoring of their concentrations with high spatial resolution in specific brain regions of interest and can be.
With the goal of imposing shape and structure on supramolecular gels, we combine a low molecular weight gelator (LMWG) with the polymer gelator (PG) calcium alginate in a hybrid hydrogel. By imposing temporal and thermal control of the orthogonal gelation methods, the system either forms an extended inter‐penetrating network or core‐shell structured gel beads – a rare example of a supramolecular gel formulated inside discrete gel spheres. The self‐assembled LMWG retains its unique properties within the beads, such as remediating Pd(II) and reducing it in situ to yield catalytically‐active Pd(0) nanoparticles. A single PdNP‐loaded gel bead can catalyse the Suzuki‐Miyaura reaction, constituting a simple and easy‐to‐use reaction dosing form. T.
The advantages of being single: Organic semiconducting single crystals are perfect for both fundamental and applied research. This Review discusses recent progress in organic single‐crystal electronics, from fabrication to application. Abstract. Organic semiconducting single crystals are perfect for both fundamental and application‐oriented research due to the advantages of free grain boundaries, few defects, and minimal traps and impurities, as well as their low‐temperature processability, high flexibility, and low cost. Carrier mobilities of greater than 10 cm2 V−1 s−1 in some organic single crystals indicate a promising application in electronic devices. The progress made, including the molecular structures and fabrication technologies of.
Fluorinated alkyl groups are important motifs in bioactive compounds, positively influencing pharmacokinetics, potency and conformation. The oxidative difluorination of alkenes represents an important strategy for their preparation, yet current methods are limited in their alkene‐types and tolerance of electron‐rich, readily oxidized functionalities, as well as in their safety and scalability. Herein, we report a method for the difluorination of a number of unactivated alkene‐types that is tolerant of electron‐rich functionality, giving products that are otherwise unattainable. Key to success is the electrochemical generation of a hypervalent iodine mediator using an ‘ex‐cell’ approach, which avoids oxidative substrate decomposition. The mo.
Surface enhanced infrared spectra show that interfacial cations interact with the electrode surface by altering the interfacial water structure, rather than the specific adsorption. In their Research Article (DOI: 10.1002/anie.201909697) Y. Yan, B. Xu, and co‐workers demonstrate that interfacial water structure engineering could hold the key to improving the kinetics of the hydrogen oxidation and evolution reactions.
Connecting the dots: Energy transfer (ET) from carbon dots embedded in crystalline Mn‐containing open‐framework matrices results in high‐efficiency red room‐temperature phosphorescence (RTP) emissions. Varying the carbon dot precursors and the heteroatom coordination geometries enables the emissions to be tuned from red to green/yellow. Abstract. High‐efficiency red room‐temperature phosphorescence (RTP) emissions have been achieved by embedding carbon dots (CDs) in crystalline Mn‐containing open‐framework matrices. The rationale of this strategy relies on two factors: 1) the carbon source, which affects the triplet energy levels of the resulting CDs and thus the spectral overlap and 2) the coordination geometry of the Mn atoms in the crysta.

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