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The α‐catenin/β‐catenin complex serves as a critical molecular interface involved in the cadherin‐catenin based mechanosensing at cell‐cell adherence junction (AJ) that plays a critical role in tissue integrity, repair and embryonic development. The α‐catenin/β‐catenin complex is subject to tensile forces due to internal actomyosin contractility and external mechanical micro‐environmental perturbation. However, the mechanical stability of this critical inter‐molecular complex has yet to be quantified. In this work, by direct quantification of the mechanical stability of the α‐catenin/β‐catenin complex, we found that the complex has sufficient mechanical stability to survive for tens to hundreds of seconds within physiological level of force.
In contrast to the notion that enantiospecific chemical reactions require a chiral reagent molecule or catalyst, this work shows that enantioselective chemical transformations can be induced by the electron spin itself. As electrons are injected from a magnetized electrode into an adsorbed molecule, they have a distinct spin orientation relative to their velocity; i.e., they have a well‐defined helicity. Thus, it is possible to replace a conventional enantiopure chemical reagent by spin‐polarized electrons that provide the chiral bias for enantioselective reactions. Three examples of enantioselective chemistry, resulting from electron spin polarization, are presented. The first example demonstrates enantioselective association of a chiral m.
The Ψ[CH2NH] reduced amide bond is a peptide isostere widely used in the development of bioactive pseudopeptides. Here we report a method of chemoenzymatic posttranslational modification for the synthesis of Ψ[CH2NH]‐containing peptides converted from ribosomally expressed peptides. The posttranslational conversion composed of an enzymatic cyclodehydration and facile 2‐step chemical reduction achieves deoxygenation of a specific amide bond present on non‐protected peptide in water. This method generating the Ψ[CH2NH] bond in peptide is applicable to various peptide sequences, potentially enabling for the library preparation of Ψ[CH2NH]‐containing peptides.
Metal‐Lewis acid cooperation provides new opportunities in catalysis. In this work, we report a new type of palladium‐borane cooperation involving anionic Pd(0) species. The air‐stable DPB palladium complex 1 (DPB = diphosphine‐borane) was prepared and reacted with KH to give the Pd(0) borohydride 2, the first monomeric anionic Pd(0) species to be structurally characterized. The boron moiety acts as an acceptor towards Pd in 1 via Pd→B interaction, but as a donor in 2 thanks to B–H–Pd bridging. This enables the activation of C–Cl bonds and the system is amenable to catalysis, as demonstrated by the hydro‐ / deutero‐dehalogenation of a variety of (hetero)aryl chlorides (20 examples, average yield 85%).
Live wire: A Hg‐DNA helical wire containing HgII‐mediated T:T and T:G base pairs and water‐mediated C:C pairs was obtained by mixing the short oligonucleotide 5′‐d(TTTGC)‐3′ and HgII ions. This novel DNA nanowire, which contains no Watson–Crick base pairs, was structurally characterized by X‐ray crystallography. Abstract. Numerous applications of metal‐mediated base pairs (metallo‐base‐pairs) to nucleic acid based nanodevices and genetic code expansion have been extensively studied. Many of these metallo‐base‐pairs are formed in DNA and RNA duplexes containing Watson–Crick base pairs. Recently, a crystal structure of a metal–DNA nanowire with an uninterrupted one‐dimensional silver array was reported. We now report the crystal structure of a.
This work demonstrates a new non‐conventional ligand design, imidazole/pyridine‐based non‐symmetrical ditopic ligands ( 1 and 1 S ), to construct a dynamic open coordination cage from non‐symmetrical building constituents. Upon complex formation with Pd 2+ at a 1:4 molar ratio, 1 and 1 S initially form mononuclear PdL 4 complexes (Pd 2+ ( 1 ) 4 and Pd 2+ ( 1 S ) 4 ) without formation of a cage. The PdL 4 complexes undergo a stoichiometrically controlled structural transition to Pd 2 L 4 open cages ((Pd 2+ ) 2 ( 1 ) 4 and (Pd 2+ ) 2 ( 1 S ) 4 ) capable of anion binding, leading to turn‐on anion binding. The structural transitions between the Pd 2 L 4 open cage and the PdL 4 complex are reversible. Thus, stoichiometric addition (2 eq) of free.
We report a switchable synthesis of acylindoles and quinoline derivatives via gold‐catalyzed annulations of anthranils and ynamides. With an N,O‐ligand on a gold(III) catalyst α‐imino gold carbenes, in situ generated from anthranils, could undergo electrophilic attack to the aryl π‐bond followed by unexpected and highly selective 1,4‐ or 1,3‐acyl migrations to form 6‐acylindoles or 5‐acylindoles. With the JohnPhos ligand gold(I) carbenes experienced carbene/carbonyl additions to deliver quinoline oxides. Some of these epoxides represent valuable substrates for the preparation of 3‐hydroxylquinolines, quinolin‐3(4H)‐ones and polycyclic compounds via facile in situ rearrangements. The reaction can be efficiently conducted on gram scale and th.
Organic single crystals with the elastic bending capability have been known recently, and potential applications of this type of unusual crystals in flexible devices and sensors have been elucidated. Exploring the temperature compatibility of elasticity is essential for defining application boundaries of elastic materials. However, related studies have rarely been reported for elastic organic crystals. Here, we show an organic crystal which displays elasticity even in liquid nitrogen (77 K). The elasticity can be maintained below ca. 150 °C. At higher temperatures, the heat setting property enabling us to make various shapes of crystals based on this single kind of crystal can be achieved. Through detailed crystallographic analyses and cont.
Strong and stable. ZnO nanocrystals derived from a one‐pot self‐supporting organometallic (OSSOM) approach have a stable and organized surface‐ligand union. Conversely, a sol‐gel approach provides limited stable cold spots with the majority of native ligands having their surface‐supporting roles taken by foreign solvent molecules. This highlights the superiority of the OSSOM approach for the preparation of quantum‐sized ZnO crystals. Abstract. The unambiguous characterization of the coordination chemistry of nanocrystal surfaces produced by wet‐chemical synthesis presently remains highly challenging. Here, zinc oxide nanocrystals (ZnO NCs) coated by monoanionic diphenyl phosphate (DPP) ligands were derived by a sol‐gel process and a one‐pot
A new polymorph of L‐tryptophan has been prepared by crystallization from the gas phase, with structure determination carried out directly from powder XRD data augmented by periodic DFT‐D calculations. The new polymorph (denoted β) and the previously reported polymorph (denoted α) are both based on alternating hydrophilic and hydrophobic layers, but with substantially different hydrogen‐bonding arrangements. The β polymorph exhibits the energetically favourable L2‐L2 hydrogen‐bonding arrangement, which is unprecedented for amino acids with aromatic side‐chains; the specific molecular conformations adopted in the β polymorph facilitate this hydrogen‐bonding scheme while avoiding steric conflict of the side‐chains.
Bonding scenarios: The synthesis and spectroscopic identification of the trisbenzene complexes of strontium and barium M(Bz)3 (M=Sr, Ba) in low‐temperature Ne matrix is reported. The complexes exhibit metal–ligand bonds that are typical for transition metal compounds. The results suggest that the heavier alkaline earth atoms exhibit the full bonding scenario of transition metals. Abstract. We report the synthesis and spectroscopic identification of the trisbenzene complexes of strontium and barium M(Bz)3 (M=Sr, Ba) in low‐temperature Ne matrix. Both complexes are characterized by a D3 symmetric structure involving three equivalent η6‐bound benzene ligands and a closed‐shell singlet electronic ground state. The analysis of the electronic stru.
An amide bond linking side chains of the first and fifth amino acids forms a cyclic pentapeptide that optimally stabilizes the smallest known alpha helix in water. The origin of stabilization is unclear. Dependence of alpha helicity on solvent and cyclization linker led us to discover a novel long‐range n to p* interaction between a mainchain amide oxygen and a uniquely positioned carbonyl group in the linker of cyclic pentapeptides. CD and NMR spectra, NMR and X‐ray structures, modelling and MD simulations reveal this first example of a synthetically incorporated long‐range n to p* CO…C=O interaction that uniquely enforces an almost perfect and remarkably stable peptide alpha helix in water, but not in DMSO. This unusual interaction with a.
Supramolecular macrocyclic hosts have been of great interest in smart materials for years, whereas their triplet emission and regulation at crystal level is still rarely excavated. Herein, ultralong and universal room temperature phosphorescence (RTP) phenomenon is evacuated for traditional crown ethers. Supramolecular strategy involving chain length adjustment and morphological locking through complexation with K+ was explored as general methods to tune phosphorescence lifetime in solid state. Significantly, B15C5 exhibits 10‐folds increasing of lifetime after forming complex accompany with invisible to visible phosphorescence. A deep encryption based on this activated RTP strategy was facile fabricated. This work open a new world for supr.
The reaction of aryl‐ and amino(dihydro)boranes with dibora[2]ferrocenophane 1 leads to the formation 1,3‐ trans ‐dihydrotriboranes by formal hydrogenation and insertion of a borylene unit into the B=B bond. The aryltriborane derivatives undergo reversible photoisomerization to the cis ‐1,2‐ μ ‐H‐3‐hydrotriboranes, while hydride abstraction affords cationic triboranes, which represent the first doubly base‐stabilized B 3 H 4 + analogues.
Precisely control the micro‐/nanostructures of nanomaterials, such as hollow multi‐shelled structure (HoMS), has shown its great advantages in various applications. In this paper, we moved forward our research direction to control the crystal structure of building blocks of HoMS, i.e., introducing the lattice distortion in HoMS, for the first time. The lattice distortion located at the nanoscale interface of SnS 2 /SnO 2 can provide additional active sites, which not only provide the catalytic activity under visible light but also improve the separation of photoexcited electron‐hole pairs. Combine with the efficient light utilization, the natural advantage of HoMS, a record catalytic activity was achieved in solid‐gas system for CO 2 reduct.
Material innovation on high‐performance Na‐ion cathodes and the corresponding understanding of structural chemistry still remain elusive. Herein, we report a new concept of high‐entropy chemistry for Na‐ion cathodes. An example of layered O3‐type NaNi 0.12 Cu 0.12 Mg 0.12 Fe 0.15 Co 0.15 Mn 0.1 Ti 0.1 Sn 0.1 Sb 0.04 O 2 has been designed and prepared successfully, which exhibits the l onger cycling stability ( ~ 83% of capacity retention after 500 cycles) and the outstanding rate capability ( ~ 80% of capacity retention at the rate of 5.0C). A highly reversible phase‐transition behavior is presented between O3 and P3 structures during the charge‐discharge process, and importantly, this behavior is delayed effectively with more than 60% of t.
Aculenes are a unique class of norsequiterpenes (C 14 ) produced from Aspergillus aculeatus. The nordaucane skeleton in aculenes A−D may be derived from an ent‐daucane precursor through a demethylation process. Despite their unprecedented structures, the genetic basis and enzymatic mechanisms involved in the biosynthesis of aculenes remained unexplored. Here, we identified the biosynthetic gene cluster of aculenes and characterized the biosynthetic pathway based on gene inactivation, feeding experiments and heterologous reconstitution in both Saccharomyces cerevisiae and Aspergillus oryzae. Notably, we discovered three cytochrome P450 monoxygenases that are required to catalyze the stepwise demethylation process. AneF converts the 12‐methyl.
The structural stability of cathode materials during electrochemical reactions, in particular, under high‐rate discharge, is pertinent to the design and development of new electrode materials that can satisfy the stringent requirements of high energy and power density for electric vehicles.


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