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Ion atmosphere: The condensation of cations around DNA and their release upon DNA–protein association have been proposed to contribute to binding thermodynamics and kinetics. In this work, NMR spectroscopy has been used to characterize the ion atmosphere around DNA and directly detect the release of cations upon DNA–protein association. This release is observed as an increase in the apparent diffusion coefficient Dapp of cations. Abstract. Due to a high density of negative charges on its surface, DNA condenses cations as counterions, forming the so‐called “ion atmosphere”. Although the release of counterions upon DNA–protein association has been postulated to have a major contribution to the binding thermodynamics, this release remains to be.
Mechanical stress sensors were prepared from cellulose nanocrystal‐elastomer composites, which provide a reversible visible color readout. Abstract. Responsive photonic crystals have potential applications in mechanical sensors and soft displays; however, new materials are constantly desired to provide new innovations and improve on existing technologies.
Hype in science is commonplace, compounded by the hypocrisy of those who engage in or tolerate it while disapproving of the consequences. These are first steps along a slippery slope of hype, hypocrisy, data falsification, and dissemination of fake science, encouraged by systemic drivers in the contemporary structure of the science establishment. Collective, concerted intervention is required to discourage entry to this dangerous pathway; chemists must play and active role. Abstract. In chemistry and other sciences, hype has become commonplace, compounded by the hypocrisy of those who tolerate or encourage it while disapproving of the consequences. This reduces the credibility and trust upon which all science depends for support. Hype and hy.
Construction of hybrid architectures for electrode materials has been demonstrated as an efficient strategy to boost the sodium storage properties because of the synergetic effect from each component. However, the fabrication of hybrid nanostructures with rational structure and desired composition for decent sodium storage is still challenging. Herein, an integrated nanostructure composed of Cu‐substituted CoS 2 @Cu x S double‐shelled nanoboxes (denoted as Cu‐CoS 2 @Cu x S DSNBs) is synthesized through a rational metal‐organic framework (MOF)‐based templating strategy. The unique shell configuration and complex composition endow the Cu‐CoS 2 @Cu x S DSNBs electrode with enhanced electrochemical performance in terms of superior rate capabili.
The first total synthesis of the potent anti‐trypanosomal macrolides (+)‐actinoallolides A–E has been achieved using the stereocontrolled aldol reactions of three chiral ketone building blocks. Trypanosoma parasites cause two key neglected tropical diseases, currently affecting over 8 million people. This convergent strategy features a challenging “do or die” ring‐closing metathesis to form the trisubstituted macrocyclic (8E)‐alkene. Abstract. Trypanosoma protozoan parasites are the causative agents of Chagas disease and sleeping sickness, two neglected tropical diseases where there is an urgent need for improved treatments and the evaluation of promising drug leads like the actinoallolides. Enabled by the highly stereocontrolled aldol react.
Photochemistry: A mild, metal‐free and easy‐to‐execute protocol for the direct photochemical hydroacylation of unactivated olefins was developed using phenylglyoxylic acid as the photoinitiator. Abstract. Direct alkylation of C(sp2)−H bonds to convert an aldehyde into a ketone is a notorious transformation, due to the laborious challenge of the formation of ketyl or acyl radicals.
Pianostool: The first example of an f‐element half‐sandwich cyclobutadienyl complex, which is only the second example of an actinide–cyclobutadienyl complex, is reported. Calculations suggest that U−C π‐bonding dominates, with no δ‐bonding component. Abstract. Despite there being numerous examples of f‐element compounds supported by cyclopentadienyl, arene, cycloheptatrienyl, and cyclooctatetraenyl ligands (C5–8), cyclobutadienyl (C4) complexes remain exceedingly rare. Here, we report that reaction of [Li2{C4(SiMe3)4}(THF)2] (1) with [U(BH4)3(THF)2] (2) gives the pianostool complex [U{C4(SiMe3)4}(BH4)3][Li(THF)4] (3), where use of a borohydride and preformed C4‐unit circumvents difficulties in product isolation and closing a C4‐ring at urani.
Eight new macrocycles with reactive functional handles were synthesized through metalloid‐assisted self‐assembly. “Design of experiments” was utilized to optimize reaction conditions for multiple systems to significantly increase the yield of a single, targeted macrocycle. Abstract. Cyclophanes are a venerable class of macrocyclic and cage compounds that often contain unusual conformations, high strain, and unusual properties. However, synthesis of complex, functional derivatives remains difficult due to low functional group tolerance, high dilution, extreme reaction conditions, and sometimes low yields using traditional stepwise synthetic methods. “Design of experiments” (DOE) is a method employed for the optimization of reaction conditions.
Solid state packing in a series of azatriangulenetrione (TANGO) derivatives controls their luminescence properties. Co‐alignment of transition dipoles in π‐stacks leads to efficient room temperature phosphorescence while their 60° rotation caused by sterically hindering tert‐butyl groups results in an almost pure fluorescence. The phosphorescence quantum yield of 42 % is achieved for pure HTANGO crystals without heavy atoms. Abstract. We report a series of highly emissive azatriangulenetrione (TANGO) solids in which the luminescent properties are controlled by engineering the molecular packing by adjusting the steric size of substituents. The co‐alignment of “phosphorogenic” carbonyl groups within the π‐stacks results in an almost pure tripl.
Segments: For the first time, two chiral conjugated macrocycles ([4]CAn2,6), as (−)/(+)‐(12,4) carbon nanotube segments, are synthesized and the physical properties studied. The hoop‐shaped molecules can be directly viewed by an STM technique. Chiral enantiomers with (−)/(+) helicity of the [4]CAn2,6 were successfully isolated. These new tubular chiral carbon nanotube segments exhibit strong circularly polarized luminescence (glum≈0.1). Abstract. Carbon nanotubes (CNTs) have unusual physical properties that are valuable for nanotechnology and electronics, but the chemical synthesis of chirality‐ and diameter‐specific CNTs and π‐conjugated CNT segments is still a great challenge. Reported here are the selective syntheses, isolations, characte.
Photoredox Catalysis (PRC) and Synthetic Organic Electrochemistry (SOE) are often considered competing technologies in organic synthesis and their fusion has been largely overlooked. We review state‐of‐the‐art synthetic organic photoelectrochemistry, grouping examples into three categories: 1) electrochemically‐mediated PhotoRedox Catalysis (e‐PRC), 2) decoupled PhotoElectrochemistry (dPEC) and 3) interfacial PhotoElectrochemistry (iPEC). Such synergies prove beneficial not only for synthetic ‘greenness’ and chemical selectivity, but also in the accumulation of energy for accessing super‐oxidizing or reducing single‐electron‐transfer (SET) agents. Opportunities and challenges in this emerging and exciting field are discussed.
To design a new anticancer drug capable of inhibiting not only the proliferation of the differentiated tumor cells but also reducing the tumorigenic capability of cancer stem cells (CSCs), the new Pt(IV) prodrugs with axial cinnamate ligands were synthesized.
Over the past several decades, the Nobel Prize program has slowly but steadily been modified in both transparent and opaque ways. A transparent change has been the creation of the Nobel Prize in Economic Sciences, more officially known as the Sveriges Riksbank Prize in Economic Sciences in Memory of Alfred Nobel. An opaque change has been the mutation of the Nobel Prize in Chemistry into what is effectively the “Nobel Prize in Chemistry or Life Sciences.” This paper presents a detailed study of this opaque change, including evidence that the disciplines of chemistry and biochemistry cover, today, intellectually quite distinct and generally scientifically unrelated intellectual territory. This paper supports the evolution of the Nobel Prizes.
Carbon dots (CDs) with dual‐emissive, robust, and aggregation‐induced room‐temperature phosphorescence (RTP) characteristics are reported. Potential applications of the as‐prepared CDs in advanced anti‐counterfeit and information encryption are also demonstrated. Abstract. Carbon dots (CDs) with dual‐emissive, robust, and aggregation‐induced RTP characteristics are reported for the first time. The TA‐CDs are prepared via hydrothermal treatment of trimellitic acid and exhibit unique white prompt and yellow RTP emissions in solid state under UV excitation (365 nm) on and off, respectively. The yellow RTP emission of TA‐CDs powder should be resulted from the formation of a new excited triplet state due to their aggregation, and the white prompt.
Transforming molecular motions into macroscopic scale is a topic of great interest to nanoscience. Photomechanical effect is a promising strategy to realize this purpose but remains challenging to design molecular materials with superior photomechanical effect that can be visually monitored under UV light. Herein, we wish to report intriguing photomechanical luminescence driven by photodimerization of 2‐phenylbenzo[b]thiophene 1,1‐dioxide (P‐BTO) in molecular crystals, and elucidate working mechanism and substituent effect via crystallography analysis and theoretical calculation. Striking splitting, hopping and bending mechanical behaviors accompanied by significant blue fluorescence enhancement are observed for P‐BTO crystals under UV ligh.
Beneath the mask: A novel and straightforward method for synthesizing aryl azides bearing a variety of functional groups by using flow microreactor system was achieved. This strategy is based on the generation and reaction of aryllithium species bearing a triazene as a masked azide group. Abstract. A novel straightforward method for aryl azides having functional groups based on generation and reactions of aryllithiums bearing a triazene group from polybromoarenes using flow microreactor systems was achieved. The present approach will serve as a powerful method in organolithium chemistry and open a new possibility in the synthesis of polyfunctional organic azides.
Immunotherapy has emerged as a promising new approach for cancer treatment. However, clinically available drugs have been limited until recently, and the antitumor efficacy of most cancer immunotherapies still needs to be improved. Herein, we develop diselenide‐pemetrexed assemblies that combine nature killer (NK) cell‐based cancer immunotherapy with radiotherapy and chemotherapy in a single system. The assemblies are prepared via co‐assembly between pemetrexed and cytosine‐containing diselenide through hydrogen bonds. Under γ‐radiation, the hydrogen bonds are cleaved, resulting in the release of pemetrexed. At the same time, diselenide can be oxidized to seleninic acid, which suppresses the expression of human leukocyte antigen E (HLA‐E) i.
Violet phosphorus single crystals and violet phosphorene have been synthesized. The structure was determined by single‐crystal X‐ray diffraction and observed by HRTEM. Violet phosphorus is more stable than black phosphorus. Violet phosphorene was obtained by mechanical and solvent exfoliation under ambient conditions. Abstract. Black phosphorene has attracted much attention as a semiconducting two‐dimensional material. Violet phosphorus is another layered semiconducting phosphorus allotrope with unique electronic and optoelectronic properties. However, no confirmed violet crystals or reliable lattice structure of violet phosphorus had been obtained. Now, violet phosphorus single crystals were produced and the lattice structure has been obtai.
Pores now found! The porous polymorph of guanidinium 1,4‐benzenedisulfonate, G2BDS, one of the simplest members of an archetypal class of hydrogen‐bonded frameworks, was prepared from its acetone solvate by single‐crystal‐to‐single‐crystal (SC‐SC) desolvation. The persistent porosity, phase behavior, and gas sorption characteristics are described. Abstract. Guanidinium organosulfonates (GSs) are a large and well‐explored archetypal family of hydrogen‐bonded organic host frameworks that have, over the past 25 years, been regarded as nonporous. Reported here is the only example to date of a conventionally microporous GS host phase, namely guanidinium 1,4‐benzenedisulfonate (p‐G2BDS). p‐G2BDS is obtained from its acetone solvate, AcMe@G2BDS, by.

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