The development of polymers from renewable resources is a promising approach to reduce reliance on petrochemicals. In addition, depolymerization is attracting significant attention for the breakdown of polymers at their end‐of‐life or to achieve specific stimuli‐responsive functions. However, the design of polymers incorporating both of these features remains a challenge. Herein, we report a new class

Hydrosilanes and Lewis bases are known to promote various reductive defunctionalizations, rearrangements, and silylation reactions, facilitated by enigmatic silicon/Lewis base‐derived reactive intermediates. Despite the wide variety of transformations enabled by this reagent combination, no examples of intermolecular C(sp3)–C(sp3) forming reactions have been reported. In this work, we’ve identified

Fluoromethyl triflate (superfluoromethyl, SFM, FCH2OSO2CF3) and fluoromethyl fluorosulfonate (magic fluoromethyl, MFM, FCH2OSO2F) are two easily synthesized, highly effective and non‐ozone depleting fluoromethylation reagents. They are analogous to the well‐known and widely used methylation re­agents CH3OSO2CF3 and CH3OSO2F. Both SFM and MFM have been fully characterized by multinuclear NMR spectroscopy

Self‐assembly of nanomaterials into hierarchical structure is of great interest to fabricate functional materials. However, programmable design of the assembled structures remains a great challenge. Herein, we reported a programmable self‐assembly strategy to customize the assembled structure. The self‐assembly strategy is designed to orderly transform the two‐dimensional (2D) Ca ions assembled F127

Bicyclo[1.1.0]butanes (BCBs) have recently garnered significant research interest as versatile precursors for synthesizing potential [n.1.1] bioisosteres and multi‐functionalized cyclobutanes in a straightforward and atom‐economical manner. Here, we report a solvent‐dependent divergent cyclization of BCBs that providecs highly diastereospecific decorated cyclobutanes and oxygen‐containing bicyclo[3

The rapid reaction between lead iodide (PbI2) and formamidinium iodide (FAI) complicates the fabrication of high‐quality formamidinium lead iodide (FAPbI3) films. Conventional methods, such as using nonvolatile small molecular additives to slow the reaction, often result in buried interfacial voids and molecule diffusion, compromising the devices' operational stability. In this study, we introduced

Linker installation has proven to be an effective strategy for introducing diverse functional groups into metal–organic frameworks (MOFs). Reductants and oxidants are found in various environments, but their accumulation poses a danger due to their high reactivity, necessitating prompt monitoring instantly, particularly in natural environments and industrial processes. In this study, a series of redox‐active

The heme paradigm where Fe=O acts as the C–H oxidant and Fe–OH rebounds with the formed carbon‐centered radical guides the design of the prototypical synthetic hydroxylation catalyst. We are exploring methods to evolve beyond the metal‐oxo oxidant and hydroxide rebound, to incorporate a wider array of functional group. We have demonstrated the application of CoII(OTf)2 (10 mol% catalyst; OTf = tri

The cleavage of carbon‐carbon bonds and their subsequent reassembly into highly functionalized and useful molecules in an atom‐efficient manner has always been a central focus in the realm of organic synthesis. In this report, we describe the construction of highly functionalized naphthol esters via a tandem reassembly process, driven by Ullmann‐type coupling of enaminones and 1,3‐dicarbonyl compounds

Currently, lack of ways to engineer specific and well‐defined active sites in zeolitic imidazolate frameworks (ZIFs) limits our fundamental knowledge with respect to the mechanistic details for (photo)electrocatalytic hydrogen evolution reaction (HER). Here, we introduce the open metal sites into ZIFs through the selective ligand removal (SeLiRe) strategy, comprehensively characterize the altered structural

Whereas molybdenum dinitrogen complexes have played a major role as catalytic model systems of nitrogenase, corresponding tungsten complexes were in most cases found to be catalytically inactive. Herein, we present a modified pentadentate tetrapodal (pentaPod) phosphine ligand in which two dimethylphosphine groups of the pentaPodMe (P5Me) ligand have been replaced with phospholanes (Pln). The derived

Vanadium flow battery (VFB) promises a route for achieving grid‐scale power storage by harnessing renewable energy sources. However, the sluggish reaction kinetics of vanadium redox couples and serious hydrogen evolution reaction (HER) still restrict the further development of VFB. Addressing these challenges requires not only effective solutions but also ones that are cost‐efficient and scalable to

Olefin triblock copolymers based on glassy polystyrene (PS), ethylene butadiene rubber (EBR) and highly crystalline polyethylene (PE) segments were prepared for the first time using a switch strategy from anionic polymerization to coordinative chain transfer (co)polymerization (CCT(co)P). PS chains obtained by anionic polymerization were transmetalated with mesitylmagnesium bromide (BrMgMes) to act

The directional assembly of porous organic molecules into long‐range ordered architectures, featuring controlled hierarchical porosity and oriented pore channels with defined spatial arrangements, is a fundamental challenge in chemistry and materials science. Herein, using porous organic cages as starting units, we present a cooperative multiscale‐assembly strategy enabling the simultaneous alignment

Skeletal editing represents an attractive strategy for adding complexity to a given molecular scaffold in chemical synthesis. Isodesmic reactions provide a complementary skeletal editing approach for the redistribution of chemical bonds in chemical synthesis. However, catalytic enantioselective isodesmic reaction is extremely scarce and enantioselective isodesmic reaction to synthesize atropisomeric

Herein, we introduce a series of ionic covalent organic frameworks (iCOFs) with a focus on addressing the challenge of water collection at low relative humidity levels below 25%. These iCOFs are characterized by numerous hydrophilic sites and high water stability, enabling efficient water vapor adsorption even at relatively low humidity levels. Through the use of various hygroscopic salt cations and

Electronic‐rich functional groups and flexible segments have long been perceived to be the decisive factors influencing lithium‐ion transfer in polymer electrolytes, while crystallinity is regarded as the great scourge. Actually, the research on the influence of crystalline phase and crystalline plane is still in scarcity. Herein, taking poly(vinylidene fluoride)‐hexafluoropropylene (PVDF‐HFP) as an

A golden fullerene with a composition of [Au42(Ph3P)10(5‐CF3‐Hpa)8] (CF3COO)2 (5‐CF3‐H2pa = 5‐trifluoropyridyl‐2‐amine) ( Au42 ) has been synthesized with pyridylamino and phosphine ligands as the protecting agents. Single crystal X‐ray structural analysis reveals that the cluster has a D3h Au4210+ core, which can be depicted as a centered core‐shell structure Au@Au15@Au26. The 41 Au atoms of the Au15@Au26

Single‐atom catalysts (SACs) inherit the merit of both homogeneous and heterogeneous systems with atomically dispersed mononuclear metal centers on the solid supports. Herein, we developed an Ir‐SAC catalyst via the polymerization of an active homogeneous 2‐picolinylhydrazone ligand‐based iridium (Ir) metal complex. Such catalysts provide great stabilization against migration and agglomeration due

A site‐selective functionalization of a C(sp3)–H bond was achieved in the presence of an intrinsically more reactive C(sp2)–H bond by controlling the orientation of a directing group via a photo‐induced E/Z isomerization of an oxime ether. By combining E/Z isomerization and an electron deficient Cp*CF3Ir(III) catalyst, the scope of oxime ethers in C(sp3)–H functionalization was successfully expanded

Developing smart materials with tunable high‐temperature afterglow (HTA) luminescence remains a formidable challenge. This study presents a metal‐free doping system using boric acid as matrix and polycyclic aromatic hydrocarbons as dopants. This composition achieves dynamically tunable afterglow combining a bright blue HTA lasting for over ten seconds even at 150°C and an ultra‐long yellow room‐temperature

Lithium‐sulfur batteries (LSBs) are among the most promising next‐generation energy storage technologies. However, a slow Li‐S reaction kinetics at the LSB cathode limit their energy and power densities. To address these challenges, this study introduces an anionic‐doped transition metal chalcogenide as an effective catalyst to accelerate the Li‐S reaction. Specifically, a tellurium‐doped, carbon‐supported

Catalytic regio‐ and enantioselective hydroamination of less activated internal alkenes presents a challenge to synthetic chemists due to their low reactivity and the difficulty in simultaneously controlling regio‐ and enantioselectivities. Here, we report an iridium‐catalyzed enantioselective hydroamination of internal alkenes directed by an amide. The amide group on the alkene effectively directs

Huge annual consumption of thermoplastics results in the generation of large amounts of waste after their service life. Currently, the most popular recycling method based on mechanically melt‐reprocessing deteriorates the material performance and is economically unattractive, which makes it unviable to be implemented in large scale. Herein, we present a chemical upcycling strategy that can transform

To enhance the alkaline hydrogen evolution reaction (HER), it is crucial, yet challenging, to fundamentally understand and rationally modulate potential catalytic sites. In this study, we confirm that despite calculating a low water dissociation energy barrier and an appropriate H adsorption free energy (ΔG*H) at Ru‐top sites, metallic Ru exhibits a relatively inferior activity for the alkaline HER

Radical S‐adenosyl methionine enzymes catalyze a diverse repertoire of post‐translational modifications in protein and peptide substrates. Among these, an exceptional and mechanistically obscure example is the installation of α‐keto‐β‐amino acid residues by formal excision of a tyrosine‐derived tyramine unit. The responsible spliceases are key maturases in a widespread family of natural products termed

: Furan‐functionalized peptides are of significant pharmacological interest due to their pronounced bioactivities and unique potential for orthogonal bioconjugation and derivatization. However, naturally occurring peptides with furyl side chains are exceedingly rare. This study presents a streamlined method to predict and assess the microbial production of peptides incorporating 3‐furylalanine (Fua)

Electrochemiluminescence (ECL) of the conventional system of [Ru(bpy)3]2+ luminophore and amine‐based coreactants is particularly inefficient on noble metal electrodes. This is due to the formation of a passivating oxide layer on the metal surface inhibiting the electro‐oxidation of amines like tri‐n‐propylamine (TPrA) coreactant, Herein, we demonstrated the enhancement of ECL emission on gold surface

The very first representative of trithia‐bridged N‐heterotriangulene, a triphenylamine with sulfur atoms bridging the ortho‐positions, was synthesized by a sequence of regioselective sulfenylation with phthalimidesulfenyl chloride followed by Lewis acid‐catalyzed electrophilic cyclization. X‐ray crystallography revealed a saddle‐shaped geometry of the polycyclic scaffold. UV/Vis absorption spectroscopy

Aqueous zinc‐ion batteries (ZIBs) are playing an increasingly important role in the field of energy storage. However, their practical applications are handicapped by severe dendrite formation and side reactions on zinc anodes. Herein, a low‐concentration high‐entropy (HE) electrolyte strategy is proposed to achieve high reversibility and ultra‐durable zinc metal anode. Specifically, this HE electrolyte

Next‐generation battery technologies need to consider their environmental impact throughout the whole cycle life, which has brought new chemistries based on earth‐abundant elements to the spotlight. Rechargeable calcium batteries are such an emerging technology, which shows the potential to provide high cell voltage and high energy density close to lithium‐ion batteries. Additionally, the use of Ca2+

Chiral rhenium(I) emitters showing circularly polarized phosphorescence (CPP) are an attractive mainstay for CP organic light‐emitting diodes (CP‐OLEDs). However, the efficiency of such emitters is not ideal, and they have never been explored for circularly polarized electroluminescence (CPEL) applications. Here, we have tailored robust chiral Re(I) complexes with improved CPP properties, and firstly

Genetically encodable photosensitizers allows for the design of artificial photoenzymes to expand the scope of abiological reactions. Here, we report the genetic incorporation of a thioxanthone‐containing amino acid into a protein scaffold using an engineered pyrrolysyl‐tRNA/pyrrolysyl‐tRNA synthetase pair. The designer enzyme was engineered to catalyze a dearomative [2 + 2] cycloaddition reaction

With antimicrobial resistance (AMR) reaching alarming levels, new anti‐infectives with unpreceded mechanisms of action are urgently needed. The 2‐C‐methylerythritol‐D‐erythritol‐4‐phosphate (MEP) pathway represents an attractive source of drug targets due to its essential role in numerous pathogenic Gram‐negative bacteria and Mycobacterium tuberculosis (Mt), whilst being absent in human cells. Here

P‐block metal carbon‐supported single‐atom catalysts (C‐SACs) have emerged as a promising candidate for high‐performance room‐temperature sodium‐sulfur (RT Na‐S) batteries, due to their high atom utilization and unique electronic structure. However, the ambiguous electronic‐level understanding of Na‐dominant s‐p hybridization between sodium polysulfides (NaPSs) and p‐block C‐SACs limits the precise

Globo H, a specific carbohydrate antigen overexpressed on various human malignancies, has attracted considerable interest as an antigenic target for anticancer vaccine development. Despite several Globo H‐based carbohydrate vaccines that have been designed, efficient access to Globo H hexasaccharide antigen and development of powerful adjuvants for enhancing antitumor immunity remain challenging. Herein

H2 and O2 evolutions occur simultaneously for conventional particulate photocatalytic overall water splitting (PPOWS), leading to a significant backward reaction and the formation of an explosive H2/O2 gas mixture. This is an issue that must be addressed prior to industrialization of PPOWS. Here, a convenient, cost‐effective, and scalable concept is introduced to uncouple hydrogen and oxygen production

Developing highly efficient, cost‐effective, and robust electrocatalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is paramount for the large‐scale commercialization of renewable fuel cells and rechargeable metal‐air batteries. Herein, a new ternary‐atom catalyst that is composed of paired Fe sites and single Ni sites (as Fe2‐N6 and Ni‐N4) coordinated onto hollow

Developing thermally activated delayed fluorescence (TADF)‐active silver clusters with near‐unity quantum efficiency is of practical importance in cutting‐edge optoelectronic devices, but remains a tremendous challenge due to the difficulty of de novo synthesis and uncertainty of properties. Herein, we demonstrate a lattice modulation on parent TADF‐activate silver cluster, acheving TADF‐driven photoluminescence

The photo‐Fenton process faces significant limitations in treating high‐turbidity, colored wastewater due to light attenuation and impurity interference (blocked mass transfer). To address these issues, we developed a suspended photothermal Fenton membrane by loading a photothermal catalyst on a hydrophobically modified cotton filter paper, enabling precise suspension 1 mm below the water surface.

Integrating Fenton chemistry and nanomedicine into cancer therapy has significantly promoted the development of chemodynamic therapy (CDT). Nanoscale polyoxometalates (POMs), with their reversible redox properties, exhibit promising potential in developing outstanding CDT drugs by exploring their Fenton‐like catalytic reactivity in tumor environments. However, such research is still in its infancy

Nature produces ATP, the energy currency, by converting solar energy (photophosphorylation) and chemical energy (substrate‐level phosphorylation and oxidative phosphorylation). Green electricity, as a significant and sustainable energy carrier, plays a crucial role in achieving a carbon‐neutral society. In this work, we established and verified a novel electrodriven phosphorylation method. Spinach

ZIF‐8 membranes have shown great promise in industrial‐scale C3H6/C3H8 separation. Nonetheless, sustainable preparation of pressure‐resistant ZIF‐8 membranes remains a grand challenge. In this study, we pioneered the use of supercritical ethane (scC2H6) as reaction medium for preparing pressure‐resistant ZIF‐8 membranes. Membrane growth in neutral organic environment was proven to have less disturbance

Producing crystalline covalent organic framework (COF) films is intimately related to the elusive nucleation and growth processes, which is desirable for efficient molecular transport. Rational control over these processes and insights into the mechanisms are crucial to improve synthetic methodology and achieve COF films with regular channels. Here, we report the controllable synthesis of COF films

Spiro skeletons have emerged as a privileged class of chiral carriers across various research fields, including asymmetric catalysis and functional materials, due to their remarkable configurational rigidity. However, limited structural diversity of spiro frameworks significantly restricts the expansion of their applications. Here we present a new class of axially chiral spiro‐bisindole frameworks

Drug resistance is a major cause of cancer recurrence and poor prognosis. The innovative design and synthesis of inhibitors to target drug‐resistance‐specific proteins is highly desirable. However, challenges remain in precisely adjusting their conformation and stereochemistry to adapt the chiral regions of target proteins. Herein, using a stepwise programmable modular assembly approach, we precisely

Selective electrocatalytic hydrogenation (ECH) of phenol is a sustainable route to produce cyclohexanone, an industrially important feedstock for polymer synthesis. However, attaining high selectivity and faradaic efficiency (FE) of cyclohexanone remain challenging, owning to over‐hydrogenation of phenol to cyclohexanol and competition of hydrogen evolution reaction (HER). Herein, by employing hydrogen