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A novel N‐hetero‐Rh(I)‐metallacyclic silanone has been synthesized. This silanone, showing an extremely large dimerization energy (ΔG = +86.2 kcal/mol), displays considerable stability and persists in solution up to 60 °C. Above 120 °C, an intramolecular C(sp3)‐H insertion occurs slowly over a period of two weeks leading to the bicyclic silanol. The exceptional stability of the silanone, related to the unusual electronic and steric effects of Rh(I)‐substituent, should allow for a more profound study and understanding of these new species. Furthermore, the metallacyclic silanone presents two reactive centers (Si=O and Rh), which can be involved depending upon the nature of reagents. Of particular interest, the reaction with H2 starts with th.
Heteroatom‐stabilized transition‐metal carbene complexes are useful building blocks for organic synthesis, but their catalytic generation from substrates with common functional groups is still challenging. In their Communication (DOI: 10.1002/anie.202002710), F. Kakiuchi and co‐workers report a novel hydroaminative cyclization of enynes with secondary amines catalyzed by phosphine‐quinolinolato rhodium complexes to form cyclic enamines via catalytic construction of an aminocarbene intermediate.
Haloesterifications using easily obtainable alkenes and carboxylic acids have unique industrial benefits. The first general catalytic asymmetric iodoesterification of simple alkenes was achieved by T. Arai et al. in their Communication (DOI: 10.1002/anie.202003886) by using a dinuclear zinc‐3,3′‐(R,S,S)‐bis(aminoimino)binaphthoxide (di‐Zn) complex. The picture represents a harmonizing quartet of metal ionic bond, hydrogen bond, halogen bond, and π–π stacking, acting together to enable the asymmetric iodoesterification of simple alkenes.
A silver orthophosphate cluster (SOC) can be stabilized in the cavity of a giant silver nanocluster. In their Communication (DOI: 10.1002/anie.202003143), G.‐G. Luo, D. Sun et al. present a multi‐shell 102‐silver nanocluster in which a rare rhombicosidodecahedral 60‐silver nanocluster accommodates an unprecedented sodalite‐type SOC {(Ag3PO4)8} concomitantly encapsulating an octahedral Ag6 core. This study is the first presentation of the SOC concept.
A potential strategy for the rapid discovery of anti‐viral therapeutic agents is delineated by J. Dash et al. in their Communication (DOI: 10.1002/anie.202003461). HIV‐1 TAR RNA promotes azide–alkyne cycloaddition to generate a new class of triazole‐linked thiazole peptidomimetics as the RNA's own binders.
Mn2+ complexes are more biocompatible alternatives to Gd3+‐based MRI agents, and 52Mn is an emerging radionuclide for positron emission tomography. Both applications require highly inert chelates which, given the labile nature of Mn2+, remains a challenge. In their Research Article (DOI: 10.1002/anie.202003685), L. Charbonnière, É. Tóth and co‐workers demonstrate that a strongly preorganized 2,4‐pyridyl‐disubstituted bispidol ligand provides exceptional kinetic inertness to its Mn2+ complex.
We report a molecular investigation of cobalt phthalocyanine (CoPc) catalyzed CO 2 reduction reaction by electrochemical scanning tunneling microscopy (ECSTM). An ordered adlayer of CoPc is prepared on Au(111). Approximately 14% of the adsorbed species appear with high contrast in CO 2 purged electrolyte environment. The ECSTM experiments indicate the proportion of high contrast species correlated with the reduction of Co II Pc (~‐0.2 V). The high contrast species is ascribed to CoPc‐CO 2 complex, which is further confirmed by theoretical simulation. T he sharp contrast change from CoPc‐CO 2 to CoPc is revealed by in situ ECSTM in the reaction. Potential step experiments provide dynamic information for the initial stage of the reaction, whi.
Aqueous zinc (Zn) battery has been considered as a promising candidate for grid‐scale energy storage. However, their cycle stability is generally limited by the structure collapse of cathode materials and the dendrite formation coupled with undesired hydrogen evolution on Zn anode. Here we propose a Zn‐organic battery, which involves a phenanthrenequinone macrocyclic trimer (PQ‐MCT) cathode, a Zn foil anode and a nonaqueous electrolyte of N, N‐dimethylformamide (DMF) solution containing Zn2+.The non‐aqueous nature and formation of Zn2+‐DMF complex can efficiently eliminate the undesired hydrogen evolution and dendrite growth on Zn anode, respectively. Furthermore, the organic cathode can store Zn2+ through reversible coordination reaction w.
Enantiomeric discrimination is achieved by tip‐enhanced Raman scattering (TERS) using a silver tip chemically modified by an achiral para ‐mercaptopyridine ( p MPY) probe molecule. Differences in the relative intensities of the p MPY spectra were monitored for three pairs of enantiomers containing hydroxyl (–OH) and/or amino (–NH 2 ) groups. The N: or N + –H functionality of the p MPY‐modified tip participates in hydrogen bond interactions with a particular molecular orientation of each chiral isomer. The asymmetric arrangement of silver atoms at the apex of the tip induces an asymmetric electric field, which causes the tip to become a chiral center. Differences in the charge‐transfer (CT) states of the metal–achiral probe system in conjunc.
Chemical reduction of a benzo‐fused double [7]helicene ( 1 ) with two alkali metals, K and Rb, provided access to three different reduced states of 1 . The doubly‐reduced helicene 1 2− has been characterized by single‐crystal X‐ray diffraction as a solvent‐separated ion triplet with two potassium counterions. The triply‐ and tetra‐reduced helicenes, 1 3− and 1 4− , have been crystallized together in an equimolar ratio and both form the contact‐ion complexes with two Rb + ions each, leaving three remaining Rb + ions wrapped by crown ether and THF molecules. As structural consequence of the stepwise reduction of 1 , the central axis of helicene becomes more compressed upon electron addition (1.42 Å in 1 4– vs . 2.09 Å in 1 ). This is accompan.
The development of transition metal oxides (TMOs)‐based bifunctional catalysts toward efficient overall water splitting through delicate control of composition and structure is a challenging task. Herein, we report rational design and controllable fabrication of unique heterostructured inter‐doped ruthenium‐cobalt oxide ((Ru‐Co)O x ) hollow nanosheet arrays on carbon cloth. Benefiting from the desirable compositional and structural advantages of more exposed active sites, optimized electronic structure, and interfacial synergy effect, the (Ru‐Co)O x nanoarrays exhibited outstanding performance as a bifunctional catalyst. Particularly, they showed a remarkable hydrogen evolution reaction (HER) activity with an overpotential of 44.1 mV at 10
This article describes a synthetic approach to a new structurally diverse family of π‐expanded diketopyrrolopyrroles (DPPs). These red‐emissive dyes, based on a previously unknown skeleton, can be easily synthesized via a three‐step strategy involving the preparation of diketopyrrolopyrrole followed by N‐arylation and subsequent intramolecular palladium‐catalyzed direct arylation. A careful selection of the aryl substituents on DPP gives access to a. π‐extended DPP derivative with intense fluorescence reaching 750 nm. The fact that NO2 groups do not engage in the excited states is responsible for the lack of fluorescence quenching when this functional group is present. Comprehensive spectroscopic assays combined with first principle calculat.
A difluoromethyl group (CF 2 H) is considered to be a lipophilic and metabolically stable bioisostere of an amino (NH 2 ) group. Therefore, methods that can rapidly convert an NH 2 group into a CF 2 H group would be of great value to medicinal chemistry. We report herein an efficient Cu‐catalyzed approach for the conversion of alkyl pyridinium salts, which can be readily synthesized from the corresponding alkyl amines, to their alkyl difluoromethane analogues. This protocol tolerates a broad range of functional groups and can be applied to late‐stage modification of complex amino‐containing pharmaceuticals.
Water electrolysis is a promising strategy for high‐purity hydrogen production but restrained by the high electricity cost. Developing an oxygen evolution reaction (OER) electrocatalyst with excellent activity and low price is indispensable for reducing water electrolysis cost. The modulation of electronic structure of catalysts can be an efficient strategy to boost their activities. Herein, the oxygen vacancies of defective iron‐cobalt oxide (FeCoO x ‐Vo) nanosheets are modified by the homogeneously distributed sulfur (S) atoms. S atoms can not only effectively stabilize oxygen vacancies (Vo), but also form the Co‐S coordination with Co active site in the Vo, which can modulate the electronic structure of the active site, enabling FeCoO x
“3‐Point annulations”, or ‘‘phenalenannulations” transform a benzene ring directly into a substituted pyrene by “wrapping” two new cycles around the perimeter of the central ring at three consecutive carbon atoms. This efficient, modular, and general method for p‐extension opens access to non‐ symmetric pyrenes and their expanded analogues. Potentially, this approach can convert any aromatic ring bearing a ‐CH 2 Br or a –CHO group into a pyrene moiety. Depending upon the workup choices, the process can be directed towards either tin‐ or iodo‐substituted product formation, giving complementary choices for further various cross‐coupling reactions. The two‐directional bis‐double annulation adds two new polyaromatic extensions with a total of s.
The challenge of quantitatively forming self‐assembled hetero‐dimers without other equilibrium by‐products is overcome through self‐sorting favored by the introduction of designed shape‐complementary moieties. Such a supramolecular strategy based on CB[8]‐directed dimerization is further applied to generate hetero‐chromophore dimers quantitatively, leading to efficient energy transfer (> 85 %) upon photoexcitation.
This study explores a new mode of contortion in perylene diimides where the molecule is bent, like a bow along its long axis. We synthesize these bowed PDIs through a facile 4‐fold Suzuki macrocyclization with aromatic linkers and a tetraborylated perylene diimide that introduces strain and results in a bowed structure. By ‐altering the strings of the bow, the degree of bending can be controlled from flat to highly bent. Through spectroscopy and quantum chemical calculations, we demonstrate that the energy of the lowest unoccupied orbital can be controlled by the degree of bending in the structures and the energy of the highest occupied orbital can be controlled to a large extent by the constitution of the aromatic linkers. The important fi.

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