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Herein we reported an asymmetric Pd/PC‐Phos‐catalyzed denitrogenative cyclization of benzotriazoles with allennes and N‐allenamides, which represents the first example of enantioselective denitrogenative cyclization of benzotriazoles. A series of optically active 3‐methyleneindolines were obtained in good yields with high ees. The use of inexpensive and readily available starting materials, high regio‐ and enantioselectivity, a broad substrate scope, mild reaction conditions, base free, as well as versatile functionalization of the 3‐methyleneindoline make this approach quite attractive.
Thermoresponsive nanoparticles (NPs) represent an important hybrid material comprising functional NPs with temperature‐sensitive polymer ligands. Strikingly, significant discrepancies in optical and catalytic properties of thermoresponsive noble metal NPs have been widely recognized yet to be unraveled in the literature. Herein, we report on in‐situ crafting of Au NPs intimately and permanently ligated by thermoresponsive poly(N‐isopropylacrylamide) (PNIPAM) using star‐like block copolymer nanoreactor as model system to resolve the paradox noted above. As temperature rises, plasmonic absorption of PNIPAM‐capped Au NPs red‐shifts with increased intensity in the absence of free linear PNIPAM, whereas greater red‐shift with decreased intensity.
S‐aryl phosphorothioates are privileged motifs in pharmaceuticals, agrochemicals and catalysts; yet, the challenge of devising a straightforward synthetic route to enantioenriched S‐aryl phosphorothioates has remained unsolved to date. We herein demonstrate the first direct C‐SP(=O)(OR')(OR'') coupling of diverse and chiral phosphorothioate salts with aryl iodides, enabled by an air‐ and moisture‐stable Pd(I) dimer. Our mechanistic and computational data suggest distinct dinuclear Pd(I) catalysis to be operative, which allows for operationally simple couplings with broad scope and full retention of stereochemistry.
Heterogeneous electrocatalysis typically involves charge transfer between surface active sites and adsorbed species. Therefore modulating the surface charge state of an electrocatalyst can be used to enhance performance. Here, we fabricate a series of negatively‐charged transition‐metal e.g. Fe, Co, Ni, Cu, and NiCo, phosphides by designing strong electronic coupling with hydr(oxy)oxides formed in‐situ. Physicochemical characterizations, together with density functional theory (DFT) computations, demonstrate that strong electronic coupling renders transition‐metal phosphides negatively‐charged. This facilitates destabilization of alkaline water–adsorption and dissociation‐ to result in significantly improved H2 evolution. Negatively‐charged.
Blue thermally activated delayed fluorescence (TADF) emitters that can simultaneously achieve high efficiency in doped and non‐doped organic light‐emitting diodes (OLEDs) are rarely reported. Herein, we proposed a tri‐spiral donor strategy for such versatile blue TADF emitters. Impressively, by simply elongating the non‐conjugated fragment and molecular length, aggregation‐caused emission quenching (ACQ) can be greatly alleviated to achieve as high as 90% horizontal orientation dipole ratio and external quantum efficiencies (EQEs) up to 33.3% in doped and 20.0% in non‐doped sky‐blue TADF‐OLEDs. More fascinatingly, high efficiency purely organic white OLED with an outstanding EQE up to 22.8% was also achieved by employing TspiroS‐TRZ as a bl.
Supported Pd catalysts are active in catalyzing the highly exothermic methane combustion reaction but tend to deactivate due to local hyperthermal environments. Herein we report an effective approach to stabilize Pd/SiO2 catalysts with porous Al2O3 overlayers coated by atomic layer deposition (ALD) method. 27Al magic angle spinning NMR characterization results show that Al2O3 overlayers on Pd particles coated by ALD method have rich penta‐coordinated Al3+ sites capable of strongly interacting with adjacent surface PdOx phases on supported Pd particles. Consequently Al2O3‐decorated Pd/SiO2 catalysts exhibit active and stable PdOx and Pd‐PdOx structures to efficiently catalyze methane combustion between 200 and 850 °C. These results reveal th.
The first catalytic method for diastereo‐ and enantioselective synthesis of allylic boronates bearing a Z‐trisubstituted alkenyl fluoride is disclosed. Boryl substitution is performed with a Z‐ or an E‐allyldifluoride and is catalyzed by bisphosphine–Cu complexes, affording products in up to 99% yield, >98:2 Z:E selectivity, and 99:1 enantiomeric ratio. A variety of subsequent modifications are feasible; notable examples are diastereoselective additions to aldehydes/aldimines to access homoallylic alcohols/amines containing a fluoro‐substituted stereogenic quaternary center.
A non‐spinel model for the structure of γ‐Al2O3, with 25% of the Al3+ cations at tetrahedral positions, has been the subject of wide interest. However, 17O NMR measurements and, more recently, 27Al NMR measurements have shown that there are considerably more Al3+ cations at tetrahedral positions. This means that the Al3+ vacancies in γ‐Al2O3 are not at tetrahedral but at octahedral positions, as in isostructural γ‐Fe2O3 and in accordance with DFT predictions. This has consequences with regard to the surface structure of γ‐Al2O3 and, thus, for catalysis.
Harvesting water from air is a promising strategy for fresh water production, particularly desirable for areas that lack direct access to clean water. While high concentration liquid sorbent is well‐known for high sorption, it has not been widely used for atmospheric water collection, primarily limited by the difficulty in desorption. In this paper we show that interfacial solar heating based on a salt‐resistant GO‐based aerogel can enable high concentration liquid sorbent (CaCl2 50 wt% solution) based atmospheric water generator. Fresh water of 2.89 kg m‐2 day‐1 can be produced at ~70% relative humidity, with only solar energy input and energy efficiency of desorption as high as 66.9%. This low‐cost and effective approach provides an attra.
Hydrogen sulfide (H2S) is an important signalling molecule whose up‐ and down‐regulation have specific biological consequences. Although significant advances in H2S up‐regulation, via the development of H2S donors, have been achieved in recent years, precise H2S down‐regulation in biological systems is still challenging. The lack of potent and specific inhibitors for H2S‐producing enzymes contributes to this problem. We expect the development of H2S scavengers is an alternative approach to address this problem. Since H2S’s chemical sensors and scavengers share almost the same criteria, we have constructed a H2S sensor database, which summarizes key parameters of all reported chemical sensors. Data‐driven analysis led to the selection of 30
Toxic gases that are colorless and odorless such as CO are a major environmental concern and require early detection to prevent serious toxicological effects. In this study, a unique system (Pt/HMSs‐BRC) was successfully fabricated via combination catalyst (Pt/hollow mesoporous silica spheres, Pt/HMSs) with the silica gel containing adsorbed chromogenic probe (binuclear rhodium complexes, BRC). The process is a simple method to prepare well‐dispersed and uniform Pt nanoparticles (NPs). The Pt/HMSs‐BRC materials demonstrate early CO detection and excellent catalytic performance for CO oxidation. The probe exhibits remarkable color modulation from gray‐violet to light‐yellow when exposed to CO concentration levels >50 ppm. And the color of th.
Direct polarity inversion of conjugate acceptors provides a valuable, although underdeveloped entry to homoenolates. As part of studies focused on this topic we have designed and developed N‐heterocyclic carbene (NHC) catalyzed reactions in which b‐unsubstituted conjugate acceptors undergo homoenolate formation and C‐C bond formation twice. Specifically, this has allowed all‐carbon (5 + 1) annulations to give a range of mono‐ and bicyclic cyclohexanones (31‐examples). In the first family of annulations, b‐unsubstituted acrylates tethered to a divinyl ketone undergo cycloisomerization provide hexahydroindenes and tetralins. In the second, partially untethered substrates undergo an intermolecular (5 + 1) annulation involving dimerization foll.
Exploring cost‐effective and efficient metal‐free electrocatalysts for oxygen reduction reaction (ORR) is crucial for the development of energy conversion and storage technologies. Here we report a novel heterocyclization strategy to construct efficient ORR catalysts based‐on linear conjugated polymers (LCPs), which are composed of N‐, S‐ or Se‐heterocycles. Among these polymers, the covalently linked pyridine‐N and thiophene‐S molecule (P‐T) with reduced graphene oxide (rGO) exhibits a remarkable half‐wave potential of 0.79 V (vs. RHE) and excellent electrochemical stability, which is among the highest values with metal‐free polymers as ORR catalysts. Further density functional theory (DFT) calculations reveal that the molecule with phenyl.
Chiral aldehyde catalysis opens new avenues for the activation of simple amines. However, the lack of easy access to structurally diverse chiral aldehyde catalysts has hampered the development of this cutting‐edge field. Herein, we report a Pd‐catalyzed atroposelective C‐H naphthylation with 7‐oxabenzonorbornadienes for the preparation of axially chiral biaryls with excellent enantioselectivities (up to >99% ee). This reaction is scalable and robust, which serves as a key step to provide a rapid access to axially chiral aldehyde catalysts via a three‐step C‒H functionalization sequence. These chiral aldehydes exhibit better activities and enantioselectivities than the previously reported organocatalyst in the asymmetric activation of glycin.
The fundamental understanding and rational manipulation of catalytic site preference at extended solid surfaces is crucial in our efforts to search for advanced catalysts. Herein we find that the Ru top sites at metallic ruthenium surface have efficient Pt‐like activity for the hydrogen evolution reaction (HER), but they are relatively recessive to their adjacent, less active Ru3‐hollow sites due to the stronger hydrogen‐binding ability of the latter. We also present an interstitial incorporation strategy for the transformation of the Ru top sites from recessiveness to dominance, while maintaining Pt‐like catalytic activity. Our joint theoretical and experimental studies further identify RuSi intermetallic as a highly active, non‐Pt materia.
In order to effectively synthesize chiral ɑ‐amino aldehydes, which have a wide range of potential applications in organic synthesis and medicinal chemistry, a highly chemo‐ and enantioselective hydrogenation of ɑ‐formyl enamides has been developed, catalyzed by a rhodium complex of a P‐stereogenic bisphosphine ligand.

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