Abstract Interface engineering has been recognized as one of the most promising strategies for regulating physical and chemical properties materials. However, constructing well‐defined nanointerfaces with efficient oxygen evolution reaction (OER) still remains a challenge. Herein, cross columnar NiTe nanoarrays supported on nickel foam are prepared. Subsequently, NiTe/NiS constructed by an ion‐exchange process. Importantly, electrocatalytic performance OER can be facilitated coupling NiS. As...

Abstract Exploring effective electrocatalysts for oxygen evolution reaction (OER) is a crucial requirement of many energy storage and conversion systems, involving fuel cells, water splitting, metal–air batteries. Herein, heterogeneity metal‐organic framework (MOF) prepared by the assembling metals, terephthalic (A) 2‐aminoterephthalic ligands (B), defined as A 2.7 B‐MOF‐FeCo 1.6 . More importantly, exhibits excellent OER activity with an ultralow overpotential 288 mV at 10 mA cm −2 Tafel...

The development of an earth-abundant, first-row water oxidation catalyst that operates at neutral pH and low overpotential remains a fundamental chemical challenge. Herein, we report the first nickel-based robust homogeneous catalyst, which can electrocatalyze in phosphate buffer. results DFT calculations verify O-O bond formation catalytic prefers HO-OH coupling mechanism from cis-isomer catalyst.

Disclosed herein is a novel, redox-neutral protocol for the visible-light-induced radical alkynylation of unactivated olefins. The intramolecular migration an alkynyl group, by cleaving inert C-C σ bond, realized first time. A wide range synthetically useful trifluoroethylated linear alkynes are readily obtained under mild reaction conditions.

Abstract The exploration of novel porous core–shell materials is great significance because their prospectively improved performance and extensive applications in separation, energy conversion, catalysis. Here, mesoporous metal–organic frameworks (MOFs) NH 2 ‐MIL‐101(Fe) as a core generate shell with covalent organic (COFs) NUT‐COF‐1(NTU) by linking process, the composite ‐MIL‐101(Fe)@NTU keeping retentive crystallinity hierarchical porosity well. Importantly, shows significantly enhanced...

Electroreduction of CO2 to acetate provides a promising strategy reduce emissions and store renewable energy, but is usually by-product. Here, we show stable conductive two-dimensional phthalocyanine-based covalent-organic framework (COF) as an electrocatalyst for reduction with single-product Faradaic efficiency (FE) 90.3(2)% at -0.8 V (vs. RHE) current density 12.5 mA cm-2 in 0.1 M KHCO3 solution. No obvious degradation was observed over 80 hours continuous operation. Combined the...

Photosynthesis of hydrogen peroxide (H2O2) in ambient conditions remains neither cost effective nor environmentally friendly enough because the rapid charge recombination. Here, a photocatalytic rate as high 114 μmol⋅g-1⋅h-1 for production H2O2 pure water and open air is achieved by using Z-scheme heterojunction, which outperforms almost all reported photocatalysts under same conditions. An extensive study at atomic level demonstrates that electron transfer realized improving photoresponse...

Carbon-carbon bond formation is the central method by which synthetic chemists add complexity, often represents value, to molecules. Uniting a carbon chain with an aromatic substrate yield alkyl arene product thus molecular means of creating value-added materials. A traditional for generating arenes Friedel-Crafts catalysis, in halide or olefin activated react substrate. Unfortunately, despite development new generations solid-state catalysts, reaction requires relatively harsh conditions...

The first example of room temperature non-noble metal homogeneous system catalyzed selective N-alkylation anilines with alcohols by a bis-NHC manganese complex is presented. This was applied to large range and anilines, including biologically relevant motifs challenging methanol. Experimental computational studies suggest an outer-sphere mechanism for this NHC-Mn system.

We demonstrate a facile ligand-assisted synthetic method, promoting the transformation of 2D layered double hydroxides (LDHs) into metal–organic frameworks (MOFs) with superior water oxidation reaction performance and durable stability.

An unusual cobalt(III)-catalyzed cross-coupling/cyclization of aryl C–H bonds N-nitrosoanilines with α-diazo-β-ketoesters has been achieved. This protocol features a unique combination Csp2-H activation/Wolff rearrangement process, allowing for the rapid assembly quaternary 2-oxindoles. The empirical evidence and density functional theory (DFT) calculations reveal trapping process transient acceptor ketene intermediates by cobalt metallocycles.

Optically active organoboronic acids and their derivatives are an important family of target compounds in organic chemistry, catalysis, medicinal chemistry. Yet there rare asymmetric catalytic examples reported for the synthesis these via atom step economic ways. Herein, we report a chelate-directed iridium-catalyzed C(sp2)–H borylation aromatic C–H bonds directed by free amine groups. The success transformations relies on novel chiral bidentate boryl ligands (L). They can be synthesized...

Copper(I)-catalyzed 5-sulfonation of quinolines via bidentate-chelation assistance has been developed. The reaction is compatible with a wide range quinoline substrates and arylsulfonyl chlorides. Experimental theoretical (DFT) investigation implicated that single-electron-transfer process involved in this sulfonylation transformation.

The unusual nonbifunctional outer-sphere strategy was successfully utilized in developing an easily accessible N-heterocyclic carbene manganese (NHC-Mn) system for highly active α-alkylation of ketones with alcohols. This efficient a wide range and alcohols under mild reaction conditions, also the green synthesis quinoline derivatives. direct mechanism high activity present demonstrate potential catalyst design acceptorless dehydrogenative transformations.

A bifunctional strategy for efficient Ir-catalyzed <italic>N</italic>-alkylation of amines and sulfonamides with alcohols under aqueous base-free conditions.

Catalytic oxidative functionalization of alkynes has emerged as an effective method in synthetic chemistry recent decades. However, enantioselective transformations via metal carbene intermediates are quite rare due to the lack robust chiral catalysts, especially intermolecular versions. Herein, we report first asymmetric three-component reaction commercially available with nitrones and alcohols, which affords α-alkoxy-β-amino-ketones good yields high excellent enantioselectivity using...

The sunlight-driven reduction of CO2 into carbonaceous fuels can lower the atmospheric concentration and provide renewable energy simultaneously, attracting scientists to design photocatalytic systems for facilitating this process. Significant progress has been made in designing high-performance photosensitizers catalysts regard, further improvement be realized by installing additional interactions between abovementioned two components, however, strategies mechanistic investigations on such...

Ferrocenes with planar chirality are an important class of privileged scaffolds for diverse chiral ligands and organocatalysts. The development efficient catalytic asymmetric methods under mild reaction conditions is a long-sought goal in this field. Though many transition-metal-catalyzed C–H activation have been recorded during the last decade, most them related to C–C bond-forming reactions. Owing useful attribute C–B bond, we herein report amide-directed iridium-catalyzed enantioselective...

Multifunctionalization from the interception of active intermediates is an attractive synthetic strategy for efficient construction complex molecular scaffolds in atom and step economic fashion. However, design reactions involving metal carbynoids that exhibit carbene/carbocation behavior currently limited, developing catalyst-controlled highly enantioselective versions poses significant challenges. In this study, we present first asymmetric trifunctionalization with rhodium carbynoids. This...

Direct asymmetric Suzuki coupling between arylboronic acids and 2-diarylphosphinyl-1-naphthyl bromides was successfully developed for the first time with use of Pd–L1 or Pd–(Cy-MOP) as catalyst. A variety axially chiral 2-functionalized-2′-diarylphosphinyl-1,1′-biaryls were afforded in 34–99% yields up to 94% ee. This methodology provides a highly efficient practical strategy synthesis novel biaryl monophosphine oxides corresponding phosphines. The existence an ortho formyl group greatly...

A general mechanism for H2 activation by Lewis acid–transition metal (LA-TM) bifunctional catalysts has been presented via density functional theory (DFT) studies on a representative nickel borane system, (PhDPBPh)Ni. There are four typical modes LA-TM catalysts: (1) the cis homolytic mode, (2) trans (3) synergetic heterolytic and (4) dissociative mode. The feature of each mode characterized key transition state structures natural bond orbital analysis. Among these modes, (PhDPBPh)Ni...