Non-noble metal catalysts are suitable for the oxygen evolution reaction (OER) owing to their original oxidation states and oxygen coordination environments, which can regulate the adsorption of OH− at the active sites to facilitate the formation of oxygen-containing intermediates. However, the difficulties encountered in the conversion of intermediates (M–OH, M–O, and M–OOH) lead to low efficiency

Protein aggregation causes alpha-synuclein (α-syn) to change from its original physiological role to a pathological state, which is a potential pathogenic mechanism in Parkinson’s disease (PD). Chiral l/d-CuxCoyS supraparticles (l/d-SPs) with a circular dichroism value of 35 mdeg at 805 nm were fabricated using a simple wet-chemical method. The l/d-SPs prevented the α-syn monomers from forming fibrils

CCS Chemistry, Ahead of Print.

Broadband white-light emission in metal halides has been intensely explored because of their facile solution processability, structural adjustability, and high color rendering index. However, the most reported quantum yields for white-light emission remain low despite great efforts. Herein, we report a metal-halide layered perovskite, (HOOC4H9NH3)2PbBr4, showing the typical white-light emission with

Herein, we report tunable asymmetric addition and telomerization of butadiene by synergistic chiral primary amine/achiral palladium catalysis. A selection of different achiral phosphine ligand in concert with the chiral primary amine-trifluoromethanesulfonic acid (TfOH) conjugates enables both chemo- and enantioselective control of the coupling with butadiene. Bidentate [(oxydi-2,1-phenylene)-bis-

Fluorinated organic compounds are of great importance to modern industries, while their release to the environment is inevitable, causing extreme environmental pollution and the subsequent hazardous effect on ecosystems. This is because the degradation of fluorinated compounds under mild conditions remains a challenging task due to the strong C–F bond strength. In this study, we report preparation

Isolation of RuIII-bda (17-electron specie) complex with an aqua ligand (2-electron donor) is challenging due to violation of the 18-electron rule. Although considerable efforts have been dedicated to mechanistic studies of water oxidation by the Ru-bda family, the structure and initial formation of the RuIII-bda aqua complex are still controversial. Herein, we challenge this often overlooked step

CCS Chemistry, Ahead of Print.

The engineering of switchable molecules with dramatic magnetic change is currently among the most active areas in chemical research. Here, two cyanide-bridged mixed-valence {FeIII4FeII4} cubes were prepared, both of which, interestingly, exhibited reversible thermally induced metal-to-metal charge transfer (MMCT) behavior between {FeIII,LS4FeII,HS4} and {FeII,LS4FeIII,HS4} configurations with the transition

Ketones serve as one of the most critical building blocks in organic synthesis, involving numerous functional group transformations. Herein, we report an unprecedented photoredox–nickel metallaphotoredox-catalyzed decarboxylative acylation of common aliphatic acids with readily available aromatic and aliphatic thioesters. A wide range of structurally diverse asymmetrical aryl alkyl and dialkyl ketones

Understanding how the diversity of glycolipids, including how their chemical structures and composition affect their biological functions, is a remarkable fundamental challenge. In this work, we employed a rare monosaccharide, 3-deoxy-d-manno-2-octulosonic acid (Kdo) to build a simple and biomimetic model to understand the diversity of glycolipids from the viewpoint of supramolecular chemistry. Kdo

Chiral superstructures in confined spaces are subtly affected by the complex interplay among various noncovalent interactions, details of which are still inadequately understood. Herein, we report the three-dimensional confined assembly of the chiral block co-polymers of polystyrene-block-poly(d-lactide) and its enantiomer in emulsion droplets and demonstrate unprecedented successive microphase transformations

Polyaniline (PANI)-based thermoelectric (TE) materials have attracted considerable attention for flexible electronic energy harvesting devices because of properties such as solution processibility, excellent environmental stability, and low cost. However, the typical opposite dependence between electrical conductivity and Seebeck coefficient impedes their development, and tremendous efforts have been

P–N and P=N bonds play important roles in the design and synthesis of functional molecules such as bioactive compounds and organic ligands for catalysis. Existing methods for P–N coupling mostly rely on Staudinger condensation or nucleophilic substitution between phosphorus electrophiles and amine nucleophiles. Herein, we report a nitrene-mediated intermolecular P–N coupling reaction between various

Stable organic radicals are promising materials for information storage, molecular magnetism, electronic devices, and biological probes. Many organic radicals have been prepared, but most are non- or weakly emissive and degrade easily upon photoexcitation. It remains challenging to produce stable and efficient luminescent radicals because of the absence of general guidelines for their synthesis. Herein

γ-Aminobutyric acid is a major inhibitory neurotransmitter in the mammalian central nervous system that plays a substantial role in brain disorders. γ-Amino phosphonic acid is a unique surrogate of both natural and unnatural γ-amino acid. Because of their unique biological activity, γ-amino acid and γ-amino phosphonic acid derivatives have attracted considerable attention. However, an efficient and

Chloride is the most abundant anion in living systems. Most natural or synthetic chloride anionophores function via hydrogen-bonding interactions. However, dynamic metal-anion coordination can also be an efficient way of transporting chloride across membranes. Here, we investigate anion transport by manganese(III) meso-tetraphenylporphyrin chloride {[Mn(TPP)Cl], TPP = meso-tetraphenylporphyrin} complex

It is highly desirable to develop a solar-driven interfacial water evaporator with a self-healing ability and high-efficiency water evaporation performance for water distillation and desalination; however, this process is considerably challenging. Herein, by exploiting the advantages of a self-healing hydrophilic polymer, a self-healing hydrophilic porous photothermal (SHPP) membrane was fabricated

Thermoelectric generators (TEGs) demonstrate great potential for flexible and wearable electronics due to the direct electrical energy harvested from waste heat. Good wearability requires high mechanical flexibility and preferable stretchability, while current TEGs are primarily developed with rigid or non-stretchable components, which do not conform well to human skin or accommodate human motions

Typically, conducting polymers transfer either electrons or holes. It is rare to see high bipolar (p- and n-type) electrical conductivities within a single bulk doped organic polymer without the assistant of gate voltage. Herein, we report that FeCl3-doped solution-processable D–A copolymer poly (2,5-bis(2-octyldodecyl)-3,6-di(thiophen-2-yl)diketopyrrolo[3,4-c]pyrrole-1,4-dione-alt-thieno[3,2-b]thiophen)

Herein, we report on the guest-responsive hierarchical self-assembly of dissymmetric cage DC-1 with an intrinsic dipole along its C3-symmetric axis. DC-1 molecules self-assemble into supramolecular columns with the molecular dipoles aligned along the columnar axis. Mediated by different host–guest interactions of ethyl acetate (EtOAc) and chloroform (CHCl3), the columns are arranged in an antiparallel

The ability to precisely monitor temperature at a high resolution is an important task, particularly in terms of safety. Inspired by natural thermosensitive transient receptor potential cation channels, we developed a temperature sensor based on thermal-driven ionic charge separation. To mimic the function of nature, an ionic covalent organic framework-based nanofluidic membrane was fabricated. By

The lipid droplet (LD) is a dynamic organelle responsible for lipid storage and metabolism that plays important roles in maintaining lipid homeostasis. However, limited strategies are available for tracking the LD content exchange. In this contribution, we report a novel fluorescent probe, TPE-AmAl, for real-time LD content dynamics tracking. TPE-AmAl is LD-specific, but emits faintly due to its intramolecular

Enhancing the charge separation efficiency is highly effective strategy in improving the photocatalytic activity of covalent organic frameworks (COFs) which have the problems of low conductivity and difficult dissociation of excitons. In this work, we report the sevenfold increase in apparent quantum efficiency resulting from the use of a near-single layer COF (SLCOF) in photocatalytic hydrogen evolution

Increasingly infectious diseases from microbial pathogens (including bacteria and fungi) threaten human health: a situation that has aroused public health concern around the world. Unfortunately, broad-spectrum antimicrobial agents for treatment resistance pathogens and molecular research on their antimicrobial mechanisms are still scarce. Thus, the development of smart agents against microbial infection

The large-scale preparation of monolayer two-dimensional (2D) material remains a great challenge, which hinders its real-world applications. Herein, we report a novel layered metal–organic framework (MOF), IPM-1, which was synthesized from a cage-like organic linker, with extremely weak interlaminar interaction. When subjected to external disturbance, IPM-1 degenerated into an intermediate state between

Recently, organic materials have emerged as next-generation thermoelectric (TE) materials because of their unique advantages including low cost, high mechanical flexibility, low or no toxicity, and low intrinsic thermal conductivity over inorganic TE materials. However, the Seebeck coefficient of organic materials with high TE properties is remarkably lower than that of its inorganic counterparts.

To understand the relationships between channel size and ion selectivity, we have developed a new type of artificial ion channel based on pore-forming helical polymers consisting of phenanthroline-oxadiazole units with a pore aperture 2.3 Å close to the diameter of the Na+ ion (2.04 Å). Successful preparation of high molecular weight helical polymers ( HP1) gives rise to a 4.6 nm long artificial unimolecular

Metathesis reactions represent powerful synthetic tools that have been used in a number of fields from the synthesis of natural product to functional material preparation. However, the C–H metathesis reaction is extremely rare. Herein, we report the first Pd(II)-catalyzed C–H iodination of arenes using 2-nitrophenyl iodides as the mild iodinating reagents via a formal metathesis reaction. Unusual C–I

Complex biological environments and multiple physiological barriers significantly impede efficient accumulation and penetration of nanomaterials within tumor tissue for therapy. In situ energy conversion of nanomotors features autonomous movements and improves cancer treatment. However, one of the key challenges is to prepare nanomotors with an adequately small size, good biocompatibility, and precise

A new series of Ir(III) carbene complexes with luminescent mechanochromism derived from trans–cis isomerization has been developed. Through the introduction of π-conjugating groups into the acyclic carbene ligand, the mechanochromic trans- and cis-configurations can be readily interconverted, leading to dual emissive properties in the solid state. Moreover, the solid- or film-forming solvent system

The development of a facile cysteine-directed S-glycosylation strategy would facilitate the intensive investigation of the effect of glycosylation on protein translational modification. Herein, we introduce glycosyl Bunte salt as an efficient glycosyl donor for site-selective peptide/protein modification. The coupling reaction with cysteine thiols under alkaline buffer conditions proceeded chemoselectively

The uranyl with two U=O double bonds is a well-known and predominant form of uranium in the environment, but the carbon-based analog with two U=C double bonds has rarely been synthesized. Here, we describe the formation of an unprecedented uranium complex [(PyPh2P)2C]2UCl2]2+·2(BPh4−) from the reaction of UCl4 with carbodiphosphorane in the presence of NaBPh4. The nature of the U–C bonds was revealed

The covalent attachment of cargo molecules (e.g., drugs and fluorophores) in β-position to a disulfide moiety through carbamate and carbonate bonds finds many applications in responsiverelease systems. Recently, we showed that the combination of this release process with polymer mechanochemistry-induced disulfide scission enabled the remote-controlled release of small molecule drugs and fluorophores

A series of vibratile π-extended dihydrophenazines ( BPs) and a tetrahydrodiphenazine ( TP) were synthesized via direct C–N coupling reactions. Structural alterations of the fused acene wings lead to diverse intermolecular packing arrangements as well as tunable photophysical properties. These compounds exhibit intriguing features, including large Stokes shift, multiple emissions, and environmental

CCS Chemistry, Ahead of Print.

Thioredoxin reductase (TrxR) is an essential enzyme for regulating the redox balance in cells, promoting cell proliferation, and inhibiting cellular apoptosis. The biochemical pathway of TrxR metabolism involves a series of selenium-sulfur (Se-S) dynamic chemistry. Theoretically, nanomaterials with Se-S dynamic bonds could exhibit TrxR-mimetic activities to tune TrxR activity, affecting cellular activities

Magnetic fields are known as clean, economic, and effective tools to modify band and magnetic structures of materials. When coupled with catalytic processes such as the hydrogen evolution reaction (HER), they have the potential to control catalytic efficiency. Herein, we studied the magnetic response of a series of materials as HER catalysts, specifically ferromagnetic Co2VGa, Co2MnGa, and Ni, ferrimagnetic

Electrochemical microscopy has been developed in the past decades for imaging biomolecules in single cells; however, electrochemical visualization of an intracellular protein in one cell is difficult. Herein, for the first time, we have developed a model whereby the protein, KDM1/LSD1 antigen, in the nucleus of a single MCF 7 cell could be visualized using wireless bipolar electrochemiluminescence

Electron-deficient N-heteroaromatic polymers are crucial for the high-tech applications of organic materials, especially in the electronic and optoelectronic fields. Thus, the development of new polymerizations to afford adaptable electron-donating–accepting scaffolds in N-heteroaromatic polymers is in high demand. Herein, we have developed metal-free multicomponent polymerizations of diynes, diamines

Currently, reactive oxygen species (ROS) generation primarily depends upon light and O2, which hampers its further biomedical application. Here, we report that a manganese(III) salen-based complex (MnS) can continuously catalyze overexpressed hydrogen peroxide (H2O2) in the tumor microenvironment to 1O2, while the nanocarrier (MIL-100) as a Fenton reagent can convert H2O2 to hydroxyl radicals (•OH)

Aggregation plays a critical role in modulating the photophysical process of organic molecules. However, the rational control of the construction of a function-oriented stacking mode for efficient photothermal (PT) conversion in the second near-infrared region (NIR-II; 1000–1700 nm) remains a challenge. Herein, an H-aggregation of 3,3′,5,5′-Tetramethylbenzidine (TMB)–TMB dication (TMB++) complexes

A water-in-water (W/W) emulsion consists of droplets formed by the spontaneous liquid–liquid separation of two immiscible aqueous phases. The inherent properties of the W/W interfaces, low or ultralow interfacial tension (γW/W = 1–1000 μN/m) and a large thickness of several nanometers, beget the poor inherent stability of emulsions. Herein, we report a nanofibril emulsifier having Schiff base reactivity

Organic thermoelectric (OTE) materials have gained widespread attention because of their potential for wearable power generators and solid cooling elements. Nevertheless, the development of state-of-the-art OTE materials still suffers from limited molecular categories because of the rarity of molecular design strategies, which limits further development of this emerging field. Recently, many efforts

Because nitric oxide (NO) plays important roles in nerve conduction, signal regulation, and immune protection, analysis of NO is of great significance for understanding the physiological and pathological processes related to neurological diseases. Herein, a highly stable and selective two-photon ratiometric fluorescent probe was developed for real-time sensing and imaging of NO in neurons, brain tissues

The stereoselective construction of vicinal all-carbon quaternary stereocenters has long been a formidable synthetic challenge. Direct asymmetric coupling of a tertiary carbon nucleophile with a tertiary carbon electrophile is the most straightforward approach, but it is sterically and energetically disfavored. Herein, we describe a catalytic asymmetric substitution, where racemic tertiary bromides

CCS Chemistry, Ahead of Print.

Probes for in vivo imaging of hypochlorous acid (HOCl), one of the most important reactive oxygen species in innate immunity, are urgently needed to understand the pathogenesis of autoimmune and neuroinflammatory disorders. As a strong oxidant, HOCl could bleach near-infrared sensors and inactivate luciferase readily, making in vivo imaging overwhelmingly challenging. Via fine-tuning of a selective

We report the first highly diastereo- and enantioselective C–C bond-forming reaction of racemic α-branched ketones to construct tertiary alcohols with adjacent stereocenters. Accordingly, a highly stereoselective cyanosilylation of racemic ketones is developed using our bifunctional cyanating reagent, Me2(CH2Cl)SiCN, giving Cα-tetrasubstituted silyl cyanohydrins with two vicinal stereocenters in up

Developing dual-state luminophores (DSLs) with strong fluorescence in both the monomer and aggregate states is urgently needed but remains a huge challenge because most current luminophores are either aggregation-induced emission or aggregation-caused quenching molecules. Moreover, limited by the structural conservation of the few existing DSLs, there are not enough response sites that can be used

CCS Chemistry, Ahead of Print.

Plasmonic metal nanostructures, possessing unique surface plasmon resonance properties, show excellent capabilities for light trapping and coupling. On this basis, various plasmonic metal nanostructures offer extraordinary opportunities to promote the conversion efficiency of solar energy to electric energy, hydrogen energy or thermal energy, and so on. In this review article, we highlight a number

CCS Chemistry, Ahead of Print.

CCS Chemistry, Ahead of Print.

CCS Chemistry, Ahead of Print.

Ambient electrochemical nitrogen fixation is a promising and environmentally benign route for producing sustainable ammonia, but has been limited by the poor performance of existing catalysts that promote the balanced chemisorption of N2 and subsequent electrochemical activation and hydrogenation. Herein, we describe the highly selective and efficient electrohydrogenation of nitrogen to ammonia using

Mechanically interlocked molecules (MIMs) and host–guest chemistry have received great attention in the past few decades. However, it remains challenging to design architectures with mechanically interlocked features and construct cavities for guest molecule recognition using similar building blocks. In this study, we designed and constructed a series of novel twisted supramolecular structures by assembling

The transition-metal-catalyzed cyanations of aryl halides are among the most used methods for synthesizing aryl nitriles. Despite tremendous advances, cyanating an aryl halide in a facile and benign fashion has generally been unsuccessful. The challenge in this significant transformation is the strong affinity of cyanide for metals, which hampers oxidative addition (OD) and reductive elimination (RE)

For the first time, a series of photochromic dyes SP1-3 with dual-responsive thermally activated delayed fluorescence (TADF) characteristics were reported in this research. Benefitting from the reversible light-responsive property of SP1-3, the eigen TADF of these compounds could be regulated between 588 and 678 nm or turned on/off by different wavelengths of light irradiation in a polyvinylpyrrolidone

The development and enrichment of organic materials with narrowband emission in longer wavelength regions beyond 515 nm still remains a great challenge. Herein, a synthetic methodology for narrowband emission materials has been proposed to functionalize multiple resonance (MR) skeletons and generate a universal building block, namely, the key intermediate DtCzB-Bpin, which can be utilized to construct