Stimuli-responsive materials hold great potential for the development of smart materials due to their specifically tailored characteristics. However, it is challenging to understand internal molecular dynamics when the macroscopic mechanics of materials change in response to specific applied stimuli. Herein, we present the biological composite fibers of which mechanical properties can be reversibly

Design and construction of suitable pore microenvironments for selective catalytic reactions of small guest molecules is a major goal for chemists. Herein, we report control of competitive E–Z photoisomerization and photodimerization within porous metal–organic frameworks (MOFs) by fine-tuning the pore microenvironments using different dicarboxylate linkers. MOFs with small pores ( ( E )-X⊂MOF1 and

One major remaining challenge in polymer chemistry is the development of efficient chemical recycling strategies to fully retrieve starting materials. Polytetrahydrofuran (PTHF) is widely used, but its stable ether bonds make it difficult to chemically reuse after disposal. Here, we propose a “polymer A → polymer B” strategy for one-step quantitative upcycling of PTHF to polyesters. The route undergoes

Covalent adaptable networks (CANs), which combine the benefits of traditional thermosets and thermoplastics, have attracted considerable attention. The dynamics of reversible covalent bonds and mobility of polymer chains in CANs determine the topological rearrangement of the polymeric network, which is critical to their superior features, such as self-healing and reprocessing. Herein, we introduce

Over the past 20 years, great efforts have been invested to develop site-specific approaches to protein modification in order to dissect protein functions directly and accurately. Here, we report a proximity-triggered group transfer strategy from a sulfonium warhead to a Cysteine (Cys) of the target protein. With a guiding ligand, cargoes can be selectively transferred form sulfonium center onto Cys

Controlling dynamic molecular self-assembly to finely tune macroscopic properties offers chemical solutions to rationalize material design. Here we report that combining disulfide-mediated ring-opening polymerization with β-sheet-like H-bonding self-assembly can drive a direct small-molecular assembly into a layered ionic network with precise architectural tunability and controllable functions as ion-transport

Myrtoidine and malagashanine, highly complex indole alkaloids, are effective adjuvant in developing cures for plasmodium malaria and also potent multi-drug resistant agents. Despite nearly 30 years of progress, myrtoidine and related a family of other Malagasy alkaloids still present formidable challenges for synthetic chemists. A diastereoselective [2+2+2] tandem cyclization reaction with alkyl substituted

Redox mediators (RMs), serving as intermediate electron carriers or reservoirs, play vital roles in developing new charge transfer energy storage systems with high voltage or capacity in aqueous batteries. However, the underlying mechanism and selection criteria of RMs remain unclear in aqueous batteries, which hinders the further exploitation of new RMs and aqueous battery chemistries. Herein, rather

Supported metal catalysts integrating advantages of catalytic hydrogenation and stoichiometric reduction are highly desirable for the green production of fine chemicals. Decoupling catalytic hydrogenation into H2 activation and selective reduction taking place at different locations is expected to provide an effective strategy to fabricate such catalyst systems. Herein, we report a decoupled hydrogenation

Enormous LiFePO4 (LFP)/graphite batteries retired from the market need urgent rational disposal and reutilization based on the degradation analysis of the evolutional mechanism for electrodes. Typically, Li inventory loss is one of the main reasons for the degradation of LFP-based batteries. The reduced portion of lithium in a cathode is inevitably consumed to form solid electrolyte interphase or trapped

The inevitable ion migration that occurs within ionic polycrystalline perovskite film results in inferior long-term stability of perovskite solar cells (PVSCs) that cannot meet the commercial requirements. Here, a novel poly(ionic liquid) named poly-1-vinyl-3-propyltrimethoxysilane imidazolium chloride (PImIL-SiO) is first introduced into perovskite to strengthen grain boundaries (GBs) and construct

Heterogeneous ice nucleation (HIN) on foreign surfaces plays a crucial role across a wide range of environmental and biological processes, and control of HIN is highly desirable. Functionalized surfaces to control HIN pose interesting scientific challenges, and hold great potential for technological impact. Here, we combine the ice nucleation tuning capability of polyelectrolytes with mussel-inspired

Mild and direct conversion of methane into high value-added products is a desired goal for chemistry, energy, and environment. The active species generated in the photocatalytic reaction system under mild conditions activate the inert C–H bond in methane and promote methane conversion. This review focuses on the developed mechanisms for C(sp3)–H bond activation in photocatalytic methane conversion

Stimulator of interferon genes, namely STING, an adaptor protein located in the endoplasmic reticulum, has been recognized as a shining target for cancer and infection research. However, STING agonists cyclic dinucleotides (CDNs) have shown almost zero efficacy in phase I clinical trials as a monotherapy, likely due to poor cellular permeability and rapid diffusion despite intratumoral injection. These

Single-atom catalysts (SACs) are gaining increasing recognition because of their superior catalytic properties for various reactions. However, the performance of SACs is often limited by the lack of neighboring metal centers to cooperate in catalysis. Herein, a synergetic interaction between neighboring Cu atoms of a few-atom catalyst (FAC) on graphdiyne (GDY) is found to greatly enhance the production

Polymers were widely proposed as carriers for cytosolic protein delivery, but always less effective due to the existence of multiple barriers such as protein binding, cell internalization and endosome escape during cytosolic delivery. Inspired by the strong binding affinity of natural polyphenols with proteins and cell membranes, herein we propose polyphenol modification to improve the protein delivery

Ortho-sulfur substituted arylphosphine oxides and arylphosphonates are the precursors of ortho-sulfurative arylphosphanes which are widely utilized as ligands in transition metal-catalyzed reactions. However, efficient synthetic methods to access such compounds are sparce. Herein, highly valuable ortho-sulfur substituted arylphosphine oxides and arylphosphonates were constructed via difunctionalization

The development of new catalytic enantioselective access to CF3-containing stereogenicity is of great interest for the expediting discovery of lead compounds yet remains challenging. Specifically, enantioselective synthesis of valuable ketones featuring α-CF3 stereogenicity has rarely been reported. We devise a general and modular approach to facilely access enantioenriched α-CF3 ketones via nickel-catalyzed

Electronic and bonding situations at reaction centers are often detected by the remote substituent effect. For nonorganometallic reactions, this effect is conventionally described by the well-known Hammett-type substituent constants. However, for most transition metal (TM)-involved systems, no analogous numeral descriptors reflecting the intrinsic differences between metallic and nonmetallic bonding

CO2 is the main greenhouse gas and a renewable carbon resource. Electrochemical transformation of CO2 (CO2ET) to value-added chemicals and fuels is one of the promising routes to reduce CO2 emission and contributes to sustainability and carbon neutrality. In this review, we discuss recent developments on apparatuses used in CO2ET, electrocatalytic reactions of CO2 with water, organics, nitrogen, and

Herein, we report the synthesis and structures of two novel mixed-metal clusters denoted as Th9Ag6 and Th9Ag12. Both clusters feature unprecedented Th9 cores. The cores are tricapped trigonal prism moieties that are novel among actinides. Attempted alternative synthesis routes indicate that the Th9 clusters are accessible only through slow introduction of Ag+ into a solution containing a Th6 cluster

Atomically precise gold and/or silver nanoclusters play a key role in crystallography and coordination chemistry. Compared with gold nanoclusters, silver nanoclusters become unstable and difficult to crystallize due to the high reactivity of metal silver. Herein, we report a silver nanocluster Ag213(Adm-S)44Cl33 ( Ag213) coprotected by bulky thiolates and chlorides. The low surface thiolate coverage

Chemically fueled dissipative self-assembly paves the way for innovative materials with lifelike properties and functions. Achievement of nonequilibrium systems with biocompatibility and biofunctions remains an important and challenging task. Here, we present biocompatible chemically fueled transient polymer nanoparticles and their applications in temporally programmable in vivo imaging. The lifetime

Development of high-efficiency electrode materials for the electrochemical CO2 reduction reaction (CO2RR) with high current density and selectivity compatible with industry is an important but significant challenge. Herein, we describe a facile strategy to enhance the selectivity and current density by regulating the local electron density of the cobalt site in a series of stable, conjugated, bimetallic

CCS Chemistry, Volume 4, Issue 6, Page 1824-1828, June 2022.

CCS Chemistry, Volume 4, Issue 6, Page 1818-1823, June 2022.

CCS Chemistry, Volume 4, Issue 6, Page 2165-2166, June 2022.

Optical imaging with molecular probes is becoming an essential tool for advancing biological research and clinical applications. However, most currently available molecular probes show limited sensitivity, specificity and accuracy due to their typical responsiveness to a single stimulation for biomarker-based imaging. In this study, we develop a novel molecular probe that shows alkaline phosphatase-instructed

It is still a formidable challenge to simultaneously switch single-chain magnet (SCM) behavior via ligand modification and light irradiation in the field of molecular spintronics. Herein, we present a ligand-bridged layer {[pzTpFe(CN)3]4Co2(Bib)4}·3H2O ( 1; pzTp, tetra-kis(1-pyrazolyl)borate; Bib, 1,4-bis-(1H-imidazol-1-yl)benzene) and a well-isolated double chain {[pzTpFe(CN)3]2Co(Bpi)2}·CH3CN·4H2O

Fundamental knowledge of structure-activity correlations for heterogeneous single-atom catalysts (SACs) is essential in guiding catalytic design. While linear scaling relations are powerful for predicting the performance of traditional metal catalysts, they appear to fail with the involvement of SACs. Comparing the catalytic CO oxidation activity of different atomically dispersed metals (3d, 4d, and

The constantly mutating SARS-CoV-2 poses great risk of efficacy loss to the present neutralizing therapeutics. Thus, it is of urgent need to develop versatile strategies that enable rapid design and engineering of potent neutralizing therapeutics for newly emerging variants. Herein, we present an unprecedented DNA nanocrown that can topologically match and multivalently bind the S-trimer of SARS-CoV-2

We herein presented the efficient syntheses, crystal structures and physical properties of a series of novel benzene triimide (BTI) radical anions, emphasizing the relation between molecular structure with spin-spin intermolecular interactions and physical properties in crystalline state. BTI radical crystals were prepared by reduction of the variously substituted BTIs 1 with cobaltocene (CoCp2) followed

The development of A-DA′D-A type small molecule acceptors (SMAs) has promoted the rapid progress of polymer solar cells (PSCs) in recent years. The outer side chains on the terminal thiophene ring and inner side chains on nitrogen atoms of the pyrrole ring of the DA′D fused ring play important roles in the photovoltaic performance of the SMAs. Here, we synthesized two new SMAs, 2,2′-((2Z,2′Z)-((12

Since polymer-based light-emitting diodes (PLEDs) are well-suited building blocks for large-area and low-cost flexible display equipment, state-of-the-art thermally activated delayed fluorescence (TADF) PLEDs are in high demand. To respond to this demand, light-emitting TADF units have initially been modified with electron-transporting units to balance the carrier transport of regiorandom TADF polymers

Photocatalytic reduction of CO2 to carbon fuels is an important target but highly challenging to achieve. Here, we report the efficient photoconversion of CO2 into formic acid over a Ga(III)-based metal–organic framework (MOF) material using triethanolamine as the sacrificial agent. Under light irradiation and at room temperature, photoreduction of CO2 over MFM-300(Ga) yields formic acid with a selectivity

Poly(β-peptoid) is a class of polypeptide mimics that possesses excellent biocompatibility and resistance to proteolysis. However, the synthesis of poly(β-peptoid)s with functionalities is a long-standing challenge that greatly hinders the functional study and application of poly(β-peptoid)s. We report a controllable and easy synthesis of poly(β-peptoid)s bearing diverse functionalities via the ring-opening

Exosomes secreted by tumor cells carry abundant molecular biomarkers that reflect the status of their originating cells. These tumor-derived exosomes (TDEs) have emerged as attractive diagnostic targets. However, the identification and characterization of highly heterogeneous TDEs remain practically challenging. Here, we report a dual rolling circle amplification (DRCA)-assisted approach for the selective

Hydrogen-bonded capsules have been widely employed as supramolecular hosts for organic molecular guests. Encapsulation of fullerenes by capsules is relatively scarce, especially those that utilize sulfur atoms as hydrogen-bond acceptors. Herein, we describe, in both solution and solid state, a bowl-shaped nanobelt [8]cyclophenoxathiin 1a and its tetra-methylated derivative 1b that can form C–H⋯S hydrogen-bonded

Here we report an in situ assembly growth method that controls the growth of NiTCNQ on the surface of graphdiyne (GDY). The catalytic system of donor–acceptor–donor (GDY/TCNQ/Ni) structure with multiple charge transfer (CT) was achieved by controlling the growth of NiTCNQ on the surface of GDY. Significantly, a controlled double layer interface of GDY/TCNQ/Ni was formed. This system implemented simultaneously

Revealing the molecular packing, intermolecular interactions, and aggregation behaviors in the nanocrystalline bulk heterojunction (BHJ) domains undertake the tasks for future materials design for efficient solar cells, especially in understanding the structure–property relationship of isomeric non-fullerene acceptors (NFAs). Theoretical calculations reveal that 2ClIC-βδ, with β- and δ-chlorine-substituted

The intricate correlation between charge degrees of freedom and physical properties is a fascinating area of research in solid state chemistry and condensed matter physics. Herein, we report on the pressure-induced successive charge transfer and accompanied resistive evolution in honeycomb layered ruthenate AgRuO3. Structural revisiting and spectroscopic analyses affirm the ilmenite type R-3 structure

Doping heteroatoms into polycyclic aromatic hydrocarbons (PAHs) is an efficient strategy to achieve fascinating electronic structures and materials. However, nanoscale B-doped PAHs remain very challenging because of the intrinsic instability of the boron atom and the lack of suitable precursors. In this study, we report a C54B2 polycyclic π-system with one embedded 1,4-diboron-substituted benzene subunit

The development of synthetic methods for the introduction of the fluorine atom and fluoroalklyl groups into organic molecules has gained increased attention. Synthetic organic chemists have recently jumped into the field of organofluorine chemistry and have thus made significant contributions. Furthermore, these newly developed methods are typically safer and more effective than the traditional methods

Higher alcohol synthesis (HAS) from syngas could efficiently alleviate the dependence on the traditional fossil resources. However, it is still challenging to construct high-performance HAS catalysts with satisfying selectivity, space–time yield (STY), and stability. Herein, we designed a diatomic catalyst by anchoring Co and Cu sites onto a hierarchical porous N-doped carbon matrix (Co/Cu–N–C). The

Inherently chiral 6,7-diphenyldibenzo[e,g][1,4]diazocine (DDD) has been synthesized enantioselectively for the first time via chiral phosphoric acid (CPA)-catalyzed cyclocondensation of readily available [1,1′-biphenyl]-2,2′-diamine ( 1a) and benzil ( 2a) in 82% yield, with 98% ee under mild reaction conditions. The strategy could also be applied to racemic biaryl diamines through kinetic resolution

Unlike biological materials that can sense mechanical force and actively remodel locally, synthetic polymers typically break down under stress. Molecular-level responses to damage with both stress-reporting and self-strengthening functions are significant yet difficult to realize for synthetic polymers. To overcome this challenge, chemo-mechanical coupling into polymers that can simultaneously ameliorate

The utilization of spin crossover (SCO) to modulate the luminescence properties in smart multifunctional materials and multichannel sensors is promising. However, it is challenging to build a strong coupling between SCO and luminescence in one system. Herein, we present a mononuclear compound [Fe(tpe-abpt)2(SeCN)2]·4DMF ( 1·4DMF, tpe-abpt: (4-(1,1,2,2-tetraphenylethene))-N-(3,5-bis(pyridin-2-yl)-4H-1

Nanoporous membranes and vesicles are interesting systems with potential in applications offering channels for material exchange. Herein, nanoporous membranes and polymersomes are developed by self-assembly of trans- and cis-stereoisomers of amphiphilic polymers. Two polymers, PEG550-TPE-Chol and PEG550-SS-TPE-SS-Chol, containing a central tetraphenylethene (TPE), a cholesterol (Chol), and a poly(ethylene

CCS Chemistry, Ahead of Print.

Reversible deactivation radical polymerization (RDRP) provides unprecedented control over polymer composition, size, functionality, and topology. Various materials, such as linear polymers, star polymers, branched polymers, graft polymers, polymer networks, and hybrid materials, have been prepared by RDRP. The ability to control polymer topology also enabled precision synthesis of well-defined polymer

Recent years have witnessed breakthroughs in the study of zigzag hydrocarbon belts. However, the synthesis of heterocycle-containing zigzag molecular belts remains very rare and challenging despite their interesting structures and potential applications in chemistry and materials science. Here, we report the expeditious construction of a highly strained belt[4]arene[4](1,4-dihydropyridine) structure

Integrating catalytic reactions with molecular assembly is a promising means of achieving controllable supramolecular polymerization. We report herein a novel and controllable method for in situ supramolecular polymerization via organometallic-catalyzed macromolecular metamorphosis. To this end, covalent polymers with polypentenamer backbones and pendant supramolecular motifs are designed and synthesized

CCS Chemistry, Ahead of Print.

Aggregation-induced emission luminogens (AIEgens) exhibit excellent luminescence properties in the aggregated state. For chiral AIEgens, a combination of right- and left-handed objects can be packed more tightly than homochiral objects due to Wallach’s rule. However, the manner in which Wallach’s rule can affect the luminescence properties of chiral AIEgens remains unclear. We report that, in contrast

The novel triplet–triplet annihilation (TTA) upconversion (UC) field of rubrene (Rub) and dibenzotetraphenylperiflanthene (DBP) sensitized by bulk metal halide perovskite, integrated with copper-2,3,9,10,16,17,23,24-octafluorophthalocyanine (F8CuPc) as cosensitizer, have been investigated in perovskite solar cells (PVSCs) to minimize sub-bandgap photon transmission loss. The firm hydrogen bonding interaction

Efficiently modifying glycals by directly introducing functional groups into their double bonds is a long-standing challenge. Here, the strategy of introducing two different functional groups into 1-iodoglycals to obtain modified glycals in one step through palladium catalysis was reported for the first time, and the modified glycals contained stereodefined tetrasubstituted olefins. Using this method

Hard materials typically lack the mechanism of energy dissipation and cannot self-heal. Nature addresses this challenge by creating multiscale interfaces between high-contrast materials, namely minerals and biopolymers. Inspired by the enamel-dentin junction, an enamel-like crown consisting of β-FeOOH nanocolumns is interdigitated with a flexible self-healing layer. The iron oxide top layer has exceptionally

Identification and visualization of phase structures inside polymer blends are of critical importance in the understanding of their intrinsic structure and dynamics. However, the direct optical observation of the individual component phase in a dense bulk material poses a significant challenge. Herein, three-dimensional fluorescence imaging of phase separation and real-time visualization of phase transformation

Living organisms, from plants to animals, have inspired and guided the design and fabrication of polymeric hydrogels with biomimetic morphology, shape deformation, and actuation behavior. However, the existing polymeric hydrogels are fragile and vulnerable, which seriously hinders further application. Therefore, endowing hydrogels with a biomimetic self-growth property and regenerating the macroscopic

Structurally well-defined arenes with higher numbers of linearly-fused six-member rings (n ≥ 10) are important and highly desirable not only because of their experimental challenges but also due to their fundamental interests and the curiosity of their structure–property relationships. In this research, we successfully synthesized a novel large N-heteroarene ( N20) with 20 linearly-fused six-membered