Nanographenes (NGs) have gained increasing attention due to their immense potential as tailor-made organic materials for nanoelectronics and spintronics. They exhibit a rich spectrum of physicochemical properties that can be tuned by controlling the size, the edge structure or by introducing structural defects in the honeycomb lattice. Here, we report the design and on-surface synthesis of NGs containing

Porous MOFs capable of storing relatively high amount of dry methane (CH4) in adsorbed phase are largely explored, how-ever solid CH4 storage in confined pores of MOFs in the form of hydrates is yet to be discovered. Here we report a rational approach to form CH4 hydrates by taking advantage of the optimal pore confinement in relatively narrow cavities of hydro-lytically stable MOFs. Unprecedentedly

Metal-organic frameworks (MOFs) offer great promise in a variety of gas and liquid-phase separations. However, excellent performance on the lab-scale hardly translates into pilot or industrial-scale applications due to their microcrystalline nature. Therefore, MOF structuring into pellets or beads is a highly solicited and timely requirement. In this work, a general structur-ing method is developed

The application scope of metal-organic frameworks (MOFs) is severely restricted by their weak chemical stability and limited pore size. A robust MOF with large mesopores is highly desired, yet poses a great synthetic challenge. Herein, two chemically stable Ni(II)-pyrazolate MOFs, BUT-32 and -33 were constructed from a conformation-matched elongated pyrazolate ligand through the isoreticular expansion

Large singlet exciton diffusion lengths are a hallmark of high performance in organic based devices such as photovoltaics, chemical sensors, and photodetectors. In this study, exciton dynamics of a two-dimensional covalent organic framework, COF-5, is investigated using ultrafast spectroscopic techniques. Following photoexcitation, the COF-5 exciton decays via three pathways: 1) excimer formation (4

Isotope-selective responsive system based on molecular recognition in porous materials has potential for the storage and purification of isotopic mixtures but is considered unachievable because of the almost identical physicochemical properties of the isotopes. Herein, a unique isotope-responsive breathing transition of the flexible metal-organic framework (MOF), MIL-53(Al), which can selectively recog-nize

Covalent organic frameworks (COFs) with intrinsic, tunable, and uniform pores are potent building blocks for separation membranes, yet poor processing ability and long processing time remain grand challenges. Herein, we re-port an engineered solid-vapor interface to fabricate a highly crystalline two-dimensional COF membrane with a thickness of 120 nm in 9 hours, which is 8 times faster than the reported

Metal-organic Frameworks (MOFs) can act as a platform for the heterogenization of molecular catalysts, providing im-proved stability, allowing easy catalyst recovery and a route towards structural elucidation of the active catalyst. We have developed a MOF, 1, possessing vacant N,N-chelating sites which are accessible via the porous channels that penetrate the structure. In the present work, cationic

We demonstrate the formation of uniform and oriented metal-organic frameworks using a combination of anion-effects and surface-chemistry. Subtle but significant morphological changes result from the nature of the coordinative counter-anion of the following metal salts: NiX2 with (X = Br-, Cl-, NO3-, and OAc-). Crystals could be obtained in solution or by template surface growth. The latter resulting

The synthetic tunability, flexibility, and rich spin physics of semiconductor quantum dots make them promising candidates for quantum information science applications. However, the rapid spin relaxation observed in colloidal quantum dots limits their functionality. In the current work, we demonstrate a method to harness photoexcited spin states in QDs to produce long-lived spin polarization on an appended

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While halogenation is of key importance in synthesis and radioimaging, the currently available repertoire is largely designed to introduce a single halogen per molecule. This report makes the selective introduction of several different halogens accessible. We showcase the privileged stability of non‐toxic aryl germanes under harsh fluorination conditions (that allow for selective fluorination in their

Like other discotic molecules, self‐assembled supramolecular structures of perylene bisimides (PBIs) are commonly limited to columnar or lamellar structures due to their distinct π‐conjugated scaffolds and unique rectangular shape of perylene cores. The discovery of PBIs with supramolecular structures beyond layers and columns may expand the scope of PBI‐based materials. Herein, we report a series

Catalytic combustion is promising in removing trace amount of CH4 to address serious environmental concerns. Supported Pd based catalysts are most effective but often suffer from low stability in practice application due to the water vapor induced sintering. Herein, we developed a universal strategy to prepare irreducible‐oxide modified Pd/MgAl2O4 catalysts which show high activity and excellent stability

‘ Supramolecular eutectogels ’ are an emerging class of materials that have just developed very recently, which offer a new opportunity for generating functional supramolecular gel materials in biocompatible anhydrous or low‐water media. As the first example of supramolecular G4 eutectogels, complexes of natural guanosine and H 3 BO 3 exhibited excellent gelation capacity in choline chloride/alcohol

Presented herein is an unprecedented Ir/f‐amphox‐catalyzed asymmetric hydrogenation of racemic 2,3‐syn‐dihydroxy‐1,4‐diones via dynamic kinetic resolution to produce (1R,2R,3R,4R)‐tetraols. This protocol constitutes an efficient and straightforward approach to accessing sugar alcohols bearing four contiguous stereocenters. The strategy exhibits various advantages over existing methods, including excellent

In the scientific race to build up photoactive electron donor‐acceptor systems with increasing efficiencies, little is known about the interplay of their building blocks when integrated into supramolecular nanoscale arrays, particularly in aqueous environments. Here, we describe an aqueous donor‐acceptor ensemble whose emergence as a nanoscale material renders it remarkably stable and efficient. We

We report a new mass spectrometric method for detecting electrogenerated intermediates. This approach is based on simultaneous activation of electrospray ionization and redox reaction on a wireless bipolar ultramicroelectrode, which is fabricated in the tip of a quartz nanopipette. The hollow structure of the ultramicroelectrode permits rapid transferring the transient species from electrode‐electrolyte

To activate electronic and optical functions of the redox‐active metal‐organic framework, (Me 2 NH 2 )[In III (TTFTB)]·0.7C 2 H 5 OH· DMF (Me 2 NH 2 @ 1, TTFTB = tetrathiafulvalene‐tetrabenzoate, DMF = N,N ‐dimethylformamide), has been exchanged by tetrathiafulvalenium (TTF •+ ) and N,N ' ‐dimethyl‐ 4,4 ' ‐bipyridinium (MV 2+ ). These cations provide electron carriers and photosensitivity. The exchange

Dealkenylative alkenylation of alkene C(sp3)‐C(sp2) bonds has been an unexplored area for C‐C bond formation. Herein, we report 64 examples of β‐alkylated styrene derivatives synthesized through the reactions of readily accessible feedstock olefins with β‐nitrostyrenes through ozone/Fe(II)‐mediated radical substitution. These reactions proceed with good efficiency and high stereoselectivity under mild

An enantioselective bifunctional squaramide‐catalyzed detrifluoroacetylative alkylation reaction under electrochemical conditions has been developed. The unified strategy based on this key tandem methodology has been divergently explored for the asymmetric synthesis of fluorine‐containing target molecules with good stereocontrol (up to 95% ee ). Furthermore, this catalytic asymmetric detrifluoroacetylative

Two‐dimensional (2D) mesoporous heterostructures combining ultrathin nanosheet morphology, periodic porous surface structures and diverse hybrid compositions have recently emerged and become increasingly important for renewable energy storage and electronics. However, it remains a great challenge to develop a universal method to prepare 2D mesoporous heterostructures. Here, we report a composite micelle‐directed

Spatial organization of electron donor‐acceptor (D‐A) supramolecular assembly is critical to the photophysical processes involved in solar energy conversion systems. Subtle variation in geometry, i.e. D‐A distance and transition dipole arrangement can influence kinetics and thermodynamics of the electron transfer (ET) process. To acquire an insight into the structure‐function correlation, making of

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

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

As substantial progress has been made in improving the performance of anion exchange membrane fuel cells (AEMFCs) over the last decade, the durability of AEMFCs has become the most critical requirement to deploy competitive energy conversion system. Because of different operating environments from proton exchange membrane fuel cells, several AEMFC-specific component degradations have been identified

Correction for ‘Twists or turns: stabilising alpha vs. beta turns in tetrapeptides’ by Huy N. Hoang et al., Chem. Sci., 2019, 10, 10595–10600, DOI: 10.1039/C9SC04153B.

A catalytic stereodivergent intermolecular [5+2] cycloaddition of maltol-type oxidopyrylium through conjugative activation was reported, which featured high stereoselectivity, good compatibility and mild conditions, providing a convenient access to various seven-membered heterocycles in moderate to excellent yields. In addition, a discrete mechanism was proposed to illustrate the stereoselectivity

Ambient-stable radical cation of a Thiele’s hydrocarbon derivative has been synthesized and its properties have been explored by a combined experimental and computational approach. The radical cation exhibited several intense near-infrared absorption bands and its solution-processed thin films showed high electrical conductivity at room temperature.

A mononuclear cobalt(III)–bis(tert-butylperoxo) adduct (CoIII–(OOtBu)2) bearing a tetraazamacrocyclic ligand was synthesized and characterized by various physicochemical methods, such as X-ray, UV-vis, ESI-MS, EPR, and NMR analyses. The crystal structure of CoIII–(OOtBu)2 complex clearly showed that two OOtBu ligands bound to equatorial position of cobalt(III) center. Kinetic studies and product analyses

An enantioselective Au(I)-catalyzed cyclization/nucleophilic addition process is developed, starting from 1,5-enyne substrates. A broad scope of O-, N- and C-nucleophiles was introduced in order to provide the corresponding chiral cyclopentene derivatives in moderate to high yields and up to 96:4 enantiomeric ratio.

The construction of graft copolymer is an effective method to modify the properties of CO2-based aliphatic polycarbonate (CO2-APC) fitting for specific needs. Herein, we describe a facile route to the synthesis of CO2-based APC-graft-polystyrene copolymers by “grafting from” strategy. Firstly, the copolymerization of CO2 and epichlorohydrin (ECH) was performed to the synthesis of APC of poly(CO2/ECH)

Herein, use of “water-in-Deep eutectic solvents (DES)” system has been shown as an alternative platform for the low temperature conversion of alginic acid (AA) to multifunctional aliginate derived carbon (AAC) material with variable oxygen functionalities. Availing the in-built oxygenated functionalities in AAC, cytochrome-c (Cyt-c) was immobilised on the surface of AACs and peroxidase activity of

A photoredox-catalyzed three-component reaction of aryldiazonium tetrafluoroborates with sodium metabisulfite and 2,2-difluoro enol silyl ethers is described. By using sodium metabisulfite as the source of sulfur dioxide, this method provides an elegant access to α,α-difluoro-β-ketosulfones in moderate to good yields under mild conditions, which features a broad substrate scope and wide functional

Catalytic enantioselective synthesis of tetrahydrofurans, which are found in the structures of many biologically active natural products, via a transition-metal catalyzed-hydrogen atom transfer (TM-HAT) and radical-polar crossover (RPC) mechanism is described herein. Hydroalkoxylation of non-conjugated alkenes proceeded efficiently with excellent enantioselectivity (up to 94% ee) using a suitable chiral

Cyclo[18]carbon (C18, a molecular carbon allotrope) can be synthesized by dehalogenation of a bromocyclocarbon precursor, C18Br6, in 64% yield, by atomic manipulation on a sodium chloride bilayer on Cu(111) at 5 K, and imaged by high-resolution atomic force microscopy. This method of generating C18 gives a higher yield than that reported previously from the cyclocarbon oxide C24O6. The experimental

ABSTRACT: Quantum entanglement has been shown to imply correlations stronger than those allowed by classical models. The possibility of performing tasks, which are classically impossible has made quantum entanglement a powerful resource for the development of novel methods and applications in various fields of research such as quantum computing, quantum cryptography, and quantum metrology. There is

We have prepared a photoresponsive metal-organic framework by using an amide-based [2]rotaxane as linker and copper(II) ions as metal nodes. The interlocked linker was obtained by the hydrogen bond-directed approach employing a fumaramide thread as template of the macrocyclic component, this latter incorporating two carboxyl groups. Single crystal X-ray diffraction analysis of the metal-organic framework

While the icosahedral closo-[B12H12]2– cluster does not display reversible electrochemical behavior, perfunctionalization of this species via substitution of all twelve B–H vertices with alkoxy or benzyloxy (OR) substituents engenders reversible redox chemistry, providing access to clusters in the dianionic, monoanionic, and neutral forms. Here, we evaluated the elec-trochemical behavior of the electron-rich

Three-dimensional (3D) triply interlocked catenanes are a family of chemical topologies that consist of two identical, mechanically interlocked coordination cage components with intriguingly complex structures. Although only a few successful constructions of 3D interlocked catenanes have been achieved to date via metal-mediated assembly, these complex structures have thus far only been targeted by