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Despite the widespread applications of manganese oxide nanomaterials (MONs) in biomedicine, the intrinsic immunogenicity of MONs is still unclear. Herein, MnOx nanospikes (NSs) as tumor microenvironment (TME)‐responsive nanoadjuvants and immuogenic cell death (ICD) drugs are proposed firstly for cancer nanovaccine‐based immunotherapy. MnOx NSs with large mesopores structures show ultrahigh loading efficiencies for ovalbumin and tumor cell fragment. The combination of ICD via chemodynamic therapy and ferroptosis inductions as well as antigen stimulations presents a better synergistic immunopotentiation action. Furthermore, the obtained nanovaccines can not only achieve TME‐responsive magnetic resonance/photoacoustic dual‐mode imaging contras.
The exhaustive trichlorosilylation of hexachloro‐1,3‐butadiene was achieved in one step by using a mixture of Si 2 Cl 6 and [ n Bu 4 N]Cl (7:2 equiv) as the silylation reagent. The corresponding butadiene dianion salt [ n Bu 4 N] 2 [ 1 ] was isolated in 36% yield after recrystallization. The negative charges of [ 1 ] 2– are mainly delocalized across its two carbanionic (Cl 3 Si) 2 C termini (α effect of silicon) such that the central bond possesses largely C=C double‐bond character. Upon treatment with 4 equiv of HCl, [ 1 ] 2– is converted to neutral 1,2,3,4‐tetrakis(trichlorosilyl)but‐2‐ene, 3 . The Cl – acceptor AlCl 3 , induces a twofold ring‐closure reaction of [ 1 ] 2– to form a six‐membered bicycle 4 in which two silacyclobutene rings.
Treatment of [Ph3EMe][I] with [Na{N(SiMe3)2}] affords the ylides [Ph3E=CH2] (E = As, 1As; P, 1P). For 1As this overcomes prior difficulties in the synthesis of this classical arsonium‐ylide that have historically impeded its wider study. The structure of 1As has now been determined, 45 years after it was first convincingly isolated, and compared to 1P, confirming the long‐proposed hypothesis of increasing pyramidalisation of the ylide‐carbon, highlighting the increasing dominance of E+‐C‐ dipolar resonance form (sp3‐C) over the E=C ene p‐bonded form (sp2‐C), as group 15 is descended. The uranium(IV)‐cyclometallate complex [U{N(CH2CH2NSiPri3)2(CH2CH2SiPri2CH(Me)CH2)}] reacts with 1As and 1P by a‐proton abstraction to give [U(TrenTIPS)(CHEPh3.
Recently, it is still challenging and attractive to construct single crystalline hybrid lead halides with highly stable and efficient blue light emissions through accurate structural design strategy considering the instability and low photoluminescence quantum yield (PLQY) of blue‐ emitting perovskites.
Porous carbons are an important class of porous materials with many applications including gas separation, while N 2 adsorption isotherm at 77 K is the most widely used approach to characterize porosity. Conventionally, textual properties such as surface area and pore volumes are derived from the N 2 adsorption isotherm at 77 K via fitting to an adsorption theory and then correlated to gas separation performance (uptake and selectivity). Here we use the N 2 isotherm at 77 K directly as input (representing feature descriptors for the porosity) to train convolutional neural networks that predict gas separation performance (using CO 2 /N 2 as a test case) for porous carbons more accurately. We then explore the porosity space for porous carbons.
Potassium (K) cations are spontaneously formed upon thermal deposition of low‐coverage K onto an ultrathin CuO monolayer grown on Cu(110) and explored by low‐temperature scanning tunneling microscopy (STM) and X‐ray photoemission spectroscopy. The formed K cations are highly immobile and thermally stable. The local work function around an individual K cation decreases by 1.5 ± 0.3 eV, and a charging zone underneath it establishes within ~ 1.0 nm. The cationic and neutral states of the K atom are switchable upon application of an STM bias voltage pulse, which is simultaneously accompanied by an adsorption site relocation.
Porous single crystals which combine ordered lattice structures and disordered inter‐connected pores would provide an alternative to create twisted surface in porous microstructures. Here we grow transition metal nitrides Nb4N5 and MoN single crystals at 2 cm scale to create well‐defined active structures at twisted surfaces and we present high catalytic activity and stability toward non‐oxidative dehydrogenation of ethane to ethylene. Unsaturated metal‐nitrogen coordination structures including Nb‐N1/5, Nb‐N2/5, Mo‐N1/3 and Mo‐N1/6 at twisted surface mainly account for the C‐H activation with chemisorption of H in molecular ethane at twisted surface, which not only improves dehydrogenation performance but also avoids the deep cracking of e.
High‐speed atomic force microscopy (HS‐AFM) is widely employed in the investigation of dynamic biomolecular processes at a single‐molecule level. However, it remains an open and somewhat controversial question, how these processes are affected by the rapidly scanned AFM tip. While tip effects are commonly believed to be of minor importance in strongly binding systems, weaker interactions may significantly be disturbed. Here, we quantitatively assess the role of tip effects in a strongly binding system using a DNA origami‐based single‐molecule assay. Despite its fM dissociation constant, we find that HS‐AFM imaging can disrupt monodentate binding of streptavidin (SAv) to biotin (Bt) even under gentle scanning conditions. To a lesser extent,
Herein we report a facile, mild reaction protocol to form carbon‐carbon bonds in the absence of transition metal catalysts. We demonstrate the metal‐free alkenylation reactions of aryl esters with α‐diazoesters to give highly functionalized enyne products. Catalytic amounts of tris(pentafluorophenyl)borane (10–20 mol%) are employed to afford the C=C coupled products (31 examples) in good to excellent yields (36–87%). DFT studies have been undertaken to elucidate the mechanism for this alkenylation reaction.
Vinyl fluorides play an important role in drug development as bioisosteres for peptide bonds and are found in a range of bioactive molecules. The discovery of safe, general and practical procedures to prepare vinyl fluorides from readily available precursors remains a synthetic challenge. The metal‐free hydrofluorination of alkynes constitutes an attractive though elusive strategy for their preparation. Here we introduce an inexpensive and easily‐handled reagent that enabled the development of simple and scalable protocols for the regioselective hydrofluorination of alkynes to access both the E and Z isomers of vinyl fluorides. These conditions were suitable for a diverse collection of alkynes, including several highly‐functionalized pharma.
C7–H functionalized indoles are ubiquitous structural units of biological and pharmaceutical compounds for numerous antiviral agents against SARS‐CoV or HIV‐1. Thus, achieving site‐selective functionalizations of C7–H of indoles, while discriminating among other bonds, is highly demand. Herein, we disclose site‐selective C7–H activations of indoles accomplished by ruthenium(II)biscarboxylate catalysis under mild conditions. Base‐assisted internal electrophilic‐type substitution C–H ruthenation by weak O‐coordination enabled the C7–H functionalizations of indoles, offering ample scope including C–N and C–C bond formation. The versatile ruthenium‐catalyzed C7–H activations were characterized by gram‐scale syntheses and the traceless removal o.
We report the two‐step hysteretic Fe(II) spin crossover (SCO) effect achieved in programmed layered Cs{[Fe(3‐CNpy)2] [Re(CN)8]}·H2O (1) assembly consisting of cyanido‐bridged FeII–ReV square grid sheets bonded by Cs+ ions. The presence of two non‐equivalent FeII sites and the conjunction of 2‐D bimetallic coordination network with non‐covalent interlayer interactions involving Cs+, [ReV(CN)8]3– ions, and 3‐CNpy ligands, leads to the occurrence of two steps of thermal SCO with strong cooperativity giving a double thermal hysteresis loop. The resulting spin transition phenomenon could be tuned by an external pressure giving the room temperature range of SCO as well as by visible light irradiation inducing an efficient recovery of the high spi.
Reducing the amount of iridium in oxygen evolution electrocatalysts without compromising their catalytic performances is one of the major requirements in proton exchange membrane water electrolyzers. Here, with the help of theoretical studies, we show that anatase‐type TiO 2 ‐IrO 2 solid solutions possess more active iridium catalytic sites for the oxygen evolution reaction (OER) than IrO 2 , the benchmark OER catalyst. It is worth adding that the same is not observed for their rutile‐type counterparts. However, due to their thermodynamic metastablity, anatase‐type TiO 2 ‐IrO 2 solid solutions are generally hard to synthesize. Our additional theoretical studies demonstrate that such catalytically active anatase‐type solid‐solution phases ca.
Heteroatom‐doped polymers or carbon nanospheres have attracted a broad research interest because of their fascinating properties. However, rational synthesis of these nanospheres with controllable uniform morphologies, small particle sizes, and well‐designed functionalities is still a great challenge. Herein, we develop an approach to construct cross‐linked polyphosphazene nanospheres with tunable hollow structures via a facile template‐free one‐step method. As comonomers, hexachlorocyclotriphosphazene provides N and P atoms, tannic acid can coordinate with metal ions, and the replaceable third comonomer can endow the materials with various properties. After the carbonization, N/P‐doped mesoporous carbon nanospheres were obtained. In additi.
Photocatalytic hydrogenation of biomass‐derived organic molecules transforms solar energy to high‐energy‐density chemical bonds, and may enable the production of industrial building‐block chemicals with great economical values. Despite its great potential, photocatalytic hydrogenation remains poorly explored up to now. Existing researches are mostly based on broad bandgap inorganic semiconductors and require the assistance of noble metal based cocatalysts. Herein, we report the preparation of thiophene‐containing covalent triazine polymer as the photocatalyst with unique donor‐acceptor units, and for the first time demonstrate the metal‐free photocatalytic hydrogenation of unsaturated organic molecules exemplified by maleic acid and furfura.
[FeFe] hydrogenases are the most active H 2 converting catalysts in nature but their extreme oxygen sensitivity limits their use in technological applications. The [FeFe] hydrogenases from sulfate reducing bacteria can be purified in an O 2 ‐stable state called H inact . To date, the structure and mechanism of formation of H inact remain unknown. Our 1.65 Å crystal structure of this state reveals a sulfur ligand bound to the open coordination site. Furthermore, in‐depth spectroscopic characterization by X‐ray absorption spectroscopy (XAS), nuclear resonance vibrational spectroscopy (NRVS), resonance Raman (RR) spectroscopy and infrared (IR) spectroscopy, together with hybrid quantum mechanical and molecular mechanical (QM/MM) calculations,
A supramolecular/synthetic method was devised to affix a sterically hindered substituent onto a fullerene guest encapsulated in a tubular host. A two‐wheeled complex of (C 59 N)–(C 59 N) with a tubular host was oxidatively bisected to afford the C 59 N + cation captured in the tube. The C 59 N + cation in the tube was then trapped by ethanol or water, which led to an oxy substituent pinned on the guest. The guest motions within the tube were modulated by the pinned substituent, and up‐and‐down flipping motions were halted by an ethoxy substituent. A hydroxy substituent, however, was ineffective in halting the flipping motions despite the tight‐fitting relationship between the tubular host and the spherical guest. Theoretical calculations of.
Designing cost‐effective and efficient electrocatalysts plays a pivotal role in advancing the development of electrochemical water splitting for hydrogen generation. Herein, multifunctional active‐center‐transferable heterostructured electrocatalysts, platinum/lithium cobalt oxide (Pt/LiCoO2) composites with Pt nanoparticles (Pt NPs) anchored on LiCoO2 nanosheets, are designed towards highly efficient water splitting. In this electrocatalyst system, the active center can be alternatively switched between Pt species and LiCoO2 for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. Specifically, Pt species are the active centers and LiCoO2 acts as the co‐catalyst for HER, whereas the active center transfers t.
A series of new bowl‐shaped N ‐hydroxyimide derivatives has been designed and used as selective organoradical catalysts. A number of these bowl‐shaped N ‐hydroxyimide derivatives exhibit excellent site‐selectivity in the amination of benzylic C(sp 3 )‐H bonds in aromatic hydrocarbon substrates.
In the present study, we investigated the biotransformation of the neonicotinoid pesticide sulfoxaflor and the metabolic responses in Sprague‐Dawley rats. Sulfoxaflor was catalyzed by cytochrome P450 while five phase I and four phase II metabolites were identified for the first time in vivo . The experimental results demonstrated that sulfoxaflor brought about the metabolic profiling disturbances in liver and bile. Exposure to sulfoxaflor caused dysregulation of bile acid synthesis and reabsorption by the expression of farnesoid X receptor (FXR). Our data provided insights into biotransformation of chemicals while enabling the implementation of a new toolbox for sulfoximine compounds design.

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