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Replacing the Pb–X octahedral building unit of A I PbX 3 perovskites (X = halide) with a pair of edge‐sharing Pb–X octahedra affords the expanded perovskite analogs: A II Pb 2 X 6 . We report eight members of this new family of materials. In 3D hybrid perovskites, orbitals from the organic molecules do not participate in the band edges. In contrast, the more spacious inorganic sublattice of the expanded analogs accommodates larger pyrizinium‐based cations with low‐lying π* orbitals that form the conduction band, substantially decreasing the expanded lattice’s bandgap. The molecular nature of the conduction band allows us to electronically dope the materials by reducing the organic molecules. By synthesizing derivatives with A II = pyridiniu.
You got the silver: An ultrastable, small {Ag7}5+ nanocluster was synthesized within an unprecedented triangular hollow polyoxometalate (POM) framework [Si3W27O96]18−. The cluster showed unique {Ag7}5+‐to‐POM charge transfer bands in both visible‐ and UV‐light regions. Abstract. Small Agn nanoclusters (n <10) have been emerging as promising materials as sensing, biolabeling, and catalysis because of their unique electronic states and optical properties. However, studying synthesis, structure determination, and exploration of their properties remain major challenges as a result of the low stability of small Ag nanoclusters. Herein, we synthesized an atomically precise face‐centered‐cubic‐type small {Ag7}5+ nanocluster supported by a novel tri.
Aluminium batteries constitute a safe and sustainable high–energy‐density electrochemical energy‐storage solution. Viable Al‐ion batteries require suitable electrode materials that can readily intercalate high‐charge Al 3+ ions. Here, we investigate the Al 3+ intercalation chemistry of anatase TiO 2 and how chemical modifications influence the accommodation of Al 3+ ions. We use fluoride‐ and hydroxide‐doping to generate high concentrations of titanium vacancies. The coexistence of these hetero‐anions and titanium vacancies leads to a complex insertion mechanism, attributed to three distinct types of host sites: native interstitials sites, single vacancy sites, and paired vacancy sites. We demonstrate that Al 3+ induces a strong local disto.
Non‐centrosymmetric polar compounds have important technological properties. Reported perovskite oxynitrides show centrosymmetric structures and for some of them high permittivities have been observed, ascribed to local dipoles induced by partial order of nitride and oxide. Here we report the first hexagonal perovskite oxynitride BaWON2, that shows a polar 6H polytype. Synchrotron X‐ray and neutron powder diffraction, and annular bright‐field in scanning transmission electron microscopy indicate that it crystalizes in the non‐centrosymmetric space group P63mc, with total order of nitride and oxide at two distinct coordination environments in cubic and hexagonal packed BaX3 layers. Synergetic second order Jahn‐Teller effect supported by firs.
A conceptually novel approach is described for the synthesis of six‐membered cyclic carbonates derived from carbon dioxide. The approach utilizes homoallylic precursors that are converted into five‐membered cyclic carbonates having a beta‐positioned alcohol group in one of the ring substituents. The activation of the pendent alcohol group through an N ‐heterocyclic base allows for equilibration towards a thermodynamically disfavored six‐membered carbonate analogue that can be conveniently trapped by an acylation agent. Various control experiments and computational analysis of this manifold are in line with a process that is primarily dictated by a kinetically controlled acylation step. This cascade process delivers an ample diversity of nov.
Multi‐component MOFs contain multiple sets of unique and hierarchical pores, with different functions for different applications, distributed in their inter‐linked domains. Herein, we report the construction of a class of precisely aligned flexible‐on‐rigid hybrid‐phase MOFs with unique rods‐on‐octahedron morphology. We demonstrated that hybrid‐phase MOFs can be constructed based on two prerequisites: the partially matched topology at the interface of the two frameworks, and the structural flexibility of MOFs with acs topology, which can compensate for the differences in lattice parameters. Furthermore, we achieved domain selective loading of multiple guest molecules into the hybrid‐phase MOF, as observed by scanning transmission electron m.
Porosity and acidity are influential properties in the rational design of solid‐acid catalysts. Probing the physicochemical characteristics of an acidic zeotype framework at the molecular level can provide valuable insights in understanding intrinsic reaction pathways, for affording structure‐activity relationships. Herein, we employ a variety of probe‐based techniques (including positron annihilation lifetime spectroscopy (PALS), FTIR and solid‐state NMR) to demonstrate how a hierarchical design strategy for a faujasitic (FAU) zeotype (synthesized for the first time, via a soft‐templating approach, with high phase‐purity) can be used to simultaneously modify the porosity and modulate the acidity for an industrially‐significant catalytic pr.
The reaction of hexachlorophosphazene, P3N3Cl6, with SO3 leads to the new sulfur nitride‐oxide S6N2O15. The compound displays an extraordinarily low nitrogen content and exhibits a bicyclic cage structure according to the formulation N{S(O)2O(O)2S}3N, with both nitrogen atoms in trigonal planar coordination of sulfur atoms. Interestingly, the new nitride‐oxide can be also seen as the anhydride of nitrido‐tris‐sulfuric acid, N(SO3H)3.
A new family of phosphine‐ligated dicyanoarylgold(III) complexes has been prepared and their reactivity towards reductive elimination has been studied in detail. Both, a highly positive entropy of activation and a primary 12/13 C KIE suggest a late concerted transition state while Hammett analysis and DFT calculations indicate that the process is asynchronous. As a result, a distinct mechanism involving an asynchronous concerted reductive elimination for the overall C(sp 2 )‐C(sp)N bond forming reaction is characterized here for the first time complementing previous studies reported for C(sp 3 )‐C(sp 3 ), C(sp 2 )‐C(sp 2 ) and C(sp 3 )‐C(sp 2 ) bond formation processes taking place on gold(III) species.
Virus and virus‐like particles (VLPs) are very attractive biological subjects for self‐assembly manipulation and templated synthesis of nanomaterials. However, the fundamental studies and applications are often constrained by problems associated with their structural weakness. Here we present a strategy of interfacially bridging covalent network within tobacco mosaic virus (TMV) VLPs to bring outstanding structural properties and functionalities. We arranged T103C cysteine to laterally conjugate adjacent subunits. In the axis direction, we set A74C mutation and systematically investigated candidate from E50C to P54C as the other thiol function site, for forming longitudinal disulfide bond chains. Significantly, the T103C‐TMV‐E50C‐A74C shows.
The Zintl anion (Ge 2 As 2 ) 2− represents an isostructural and isoelectronic binary counterpart of yellow arsenic, yet without being studied with the same intensity so far. Upon introducing [(PPh 3 )AuMe] into the 1,2‐diaminoethane (en) solution of (Ge 2 As 2 ) 2− , the heterometallic cluster anion [Au 6 (Ge 3 As)(Ge 2 As 2 ) 3 ] 3− is obtained as its salt [K(crypt‐222)] 3 [Au 6 (Ge 3 As)(Ge 2 As 2 ) 3 ]·en·2tol ( 1 ). The anion represents a rare example of a superpolyhedral Zintl cluster, and it comprises the largest number of Au atoms relative to main group (semi)metal atoms in such clusters. The overall supertetrahedral structure is based on a (non‐bonding) octahedron of six Au atoms that is face‐capped by four (Ge x As 4−x ) x− (x = 2,
In soft matter, thermal energy causes molecules to continuously translate and rotate, even in crowded environments, thereby impacting the spatial organization and function of most molecular assemblies, such as lipid membranes. Directly measuring the orientation and spatial organization of large collections (>3000 molecules/µm 2 ) of single molecules with nanoscale resolution remains elusive. In this paper, we utilize SMOLM, single‐molecule orientation localization microscopy, to directly measure the orientation spectra (3D orientation plus "wobble") of lipophilic probes transiently bound to lipid membranes, revealing that Nile red’s (NR) orientation spectra are extremely sensitive to membrane chemical composition. SMOLM images resolve nanod.
Lead‐free halide perovskite of A 3 Sb 2 Br 9 is utilized as photocatalyst for the first time to C (sp 3 )‐H bonds activation. A 3 Sb 2 Br 9 nanoparticles (A 3 Sb 2 Br 9 NPs) with different ratios of Cs and MA show different photocatalytic activity for toluene oxidation and the photocatalytic performance is enhanced when increasing the amount of Cs. We reveal that the octahedron distortion caused by A‐site cations can change the electronic property of X‐site ions and further affect the electron transfer from toluene molecules to Br sites. After the regulation of A‐site cations, the photocatalytic activity is higher with A 3 Sb 2 Br 9 NPs than that with some classic photocatalysts (TiO 2 , WO 3 and CdS). The main active species involved in ph.
Lantibiotics are a type of ribosomally synthesized and post‐translationally modified peptides (termed lanthipeptides) with often potent antimicrobial activity. Herein, we report the discovery of a new lantibiotic, lexapeptide, using the Library EXpression Analysis System (LEXAS) approach. Lexapeptide has rare structural modifications, including N‐terminal (N,N)‐dimethyl phenylalanine, C‐terminal (2‐aminovinyl)‐3‐methyl‐cysteine, and D‐Ala. The characteristic lanthionine moiety in lexapeptide is formed by three proteins (LxmK, LxmX, and LxmY), which are distinct from enzymes known to be involved in lanthipeptide biosynthesis. Furthermore, a novel F420H2‐dependent reductase (LxmJ) from the lexapeptide biosynthetic gene cluster (BGC) is identi.
Mesoporous core‐shell nanostructures holding controllable ultra‐large open channels in their nanoshells are of great interests for the development of new catalytic platforms, electrochemical energy systems, and biological macromolecular carriers. However, soft template‐directed cooperative assembly to mesoporous nanoshells with highly accessible pores larger than 30 nm, or even above 50 nm into macroporous range, remains a significant challenge. Herein we report a general approach for precisely tailored coating of hierarchically macro‐/mesoporous polymer and carbon shells, possessing highly accessible radial channels with extremely wide pore size distribution from ~10 nm to ~200 nm, on diverse functional materials. This strategy creates opp.
Growth of covalent organic frameworks (COFs) as single crystals is extremely challenging. Inaccessibility of open‐structured single‐crystal COFs prevents the exploration of structure‐oriented applications. Herein we report for the first time a non‐interpenetrated single‐crystal COF, LZU‐306, which possesses the open structure constructed exclusively via covalent assembly. With a high void volume of 80%, LZU‐306 was applied to investigate the intrinsic dynamics of reticulated tetraphenylethylene (TPE) as the individual aggregation‐induced‐emission moiety. Solid‐state 2 H NMR investigation has determined that the rotation of benzene rings in TPE, being the freest among the reported cases, is as fast as 1.0 × 10 4 Hz at 203 K to 1.5 × 10 7 Hz
O‐Sulfation is an important chemical code widely existing in bioactive molecules, but the scalable and facile synthesis of complex bioactive molecules carrying O‐sulfation remains challenging. Herein, we report a general approach to O‐sulfation via the Sulfur (VI) Fluoride Exchange (SuFEx) reaction between aryl fluorosulfates and silylated hydroxyl groups. Efficient sulfate diester formation was achieved through systematic optimization of the electronic properties of aryl fluorosulfates. The versatility of this O‐sulfation strategy was demonstrated in the scalable syntheses of a variety of complex molecules carrying sulfate diesters at various positions, including monosaccharides, disaccharides, amino acid, and steroid. Selective hydrolytic.
Dynamic and on‐site analysis of serum from human blood is crucial particularly for making decisions during clinical surgery and emergency treatments. However, state‐of‐the‐art blood assay methods can only collect single or discrete data of physiological analytes, remaining great challenge in online report of dynamic fluctuation of key analytes. Here we propose a novel separation–sensing membrane by constructing a heterogeneous‐nanostructured architecture in which a surface nanoporous layer continuously extracts serum and underneath biosensing nanochannels dynamically recognize biotargets, achieving continuous testing of vital clinical indices as blood drawn. Through precisely controlling the pore structure and nanoshape of biosensing crysta.
Herein, we introduce the cyclic 8π‐electron (C8π) molecule N , N ′‐diaryl‐dihydrodibenzo[ a , c ]phenazines ( DPAC ) as a dual‐functional donor to establish a series of new donor‐linker‐acceptor (D‐L‐A) dyads DLA1 ~ DLA5 . The excited‐state bent‐to‐planar dynamics of DPAC regulate the donor’s energy gap, while the acceptors A1 ~ A5 are endowed with different energy gaps and HOMO/LUMO levels. As a result, the rate and efficiency of the excited‐state electron transfer versus energy transfer can be finely harnessed, which is verified via the steady‐state spectroscopy and time‐resolved emission measurements. These approaches unveil that DLA1 with poor donor/acceptor spectral overlap undergoes photoinduced electron transfer (PET) from the excite.

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