Shi LY, Ding YT, Liu XD
… +11 more, Wu SD, Sun WJ, Sun B, Wei YS, Zhang Z, Liu ST, Chen L, Xiang D, Zhang Y, Liu Z, Zhang HL
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42334018
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Neuromorphic computing, particularly memristor-based architectures, offers a promising route to overcome the von Neumann bottleneck. Single-molecule devices, with their high integration density and low energy consumption...Neuromorphic computing, particularly memristor-based architectures, offers a promising route to overcome the von Neumann bottleneck. Single-molecule devices, with their high integration density and low energy consumption, represent an emerging platform for next-generation computing. Here, we report the first optoelectronic volatile single-molecule memristor based on the organic photovoltaic material Y6. The device exhibits reproducible conductance switching driven by electric-field-induced structural relaxation, enabling gradual and linear conductance modulation that mimics synaptic behavior. Under red-light illumination, the Y6 junction shows a remarkable 457% increase in conductance and a significantly reduced switching threshold, demonstrating strong photoresponsivity and low-power operation. Furthermore, frequency-dependent pulse tests clearly reproduce short-term synaptic plasticity (STP), demonstrating the memristor's ability to emulate dynamic synaptic functions. When the experimentally measured current response of the Y6 single-molecule memristor is incorporated into an artificial neural network (ANN) model, the system achieves a speech-recognition accuracy of 71.50%, closely matching that of the benchmark ANN (74.90%). This work pioneers the realization of synaptic functionality in a single-molecule memristor and validates its application within an artificial neural network. It provides a new strategy for developing highly integrated molecular-scale neuromorphic computing devices.
Wang J, Li Z, Wang J
… +5 more, Gu K, Xu C, Yue L, Zhang Z, Rao B
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42334003
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Luminescent diradicals hold great promise for optomagnetic applications, yet those with a triplet ground state remain largely underexplored for the inherent high reactivity from two spin-parallel unpaired electrons, whic...Luminescent diradicals hold great promise for optomagnetic applications, yet those with a triplet ground state remain largely underexplored for the inherent high reactivity from two spin-parallel unpaired electrons, which hinders synthesis and enhances non-radiative quenching. Herein, we report the first luminescent Schlenk diradical 2 with a distinct triplet ground state, concisely assembled from a methoxybenzene core and four polychlorobenzene pendants and readily isolated under air by routine silica-gel chromatography. Good stability results from the steric hindrance of its propeller conformation, which effectively safeguards the two carbon radical centers. Comprehensive characterization elucidated the molecular structure and confirmed a triplet ground state with strong magnetic exchange interaction (J/k > 320 K). Notably, diradical 2 shows a red emission at 619 nm with a quantum yield of 9.6% in cyclohexane, facilitated by its rigid propeller conformation and the D-A electron distribution for the coexistence of electron-rich methoxybenzene and electron-deficient polychlorobenzenes. The luminescence predominantly originates from the T → T transition, as the large energy gaps (T → S and T → S) prohibit singlet-state luminescence. This work not only enlarges the Schlenk hydrocarbon family but also opens new avenues for the understanding and design of luminescent high-spin species.
Li L, Sun Z, Wang X
… +8 more, Zhang L, Chen Z, Gu Q, Yang J, Cui Y, Peng YK, Sun L, Zhang Q
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333935
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Molecular electron spins are compelling qubit candidates; however, mitigating their rapid relaxation and decoherence driven by structural disorder and phonon coupling remains a central challenge. Constructing molecular q...Molecular electron spins are compelling qubit candidates; however, mitigating their rapid relaxation and decoherence driven by structural disorder and phonon coupling remains a central challenge. Constructing molecular qubit frameworks (MQFs) represents a promising strategy to preserve quantum coherence by embedding spin centers in a rigid and ordered microenvironment. Here, we report a host-guest superlattice MQF by cocrystallizing tetrathiafulvalene (TTF) with a one-dimensional B←N coordination polymer (CityU-65). Encaging TTF radical spins within this highly ordered lattice establishes a rigid and magnetically dilute environment, effectively suppressing spin-lattice relaxation and partially mitigating spin decoherence. Consequently, CityU-65 preserves coherent spin addressability even under ambient conditions. At room temperature, the superlattice exhibits a prolonged spin-lattice relaxation time (T = 9.6 µs) and a modestly improved phase-memory time (T = 0.9 µs) compared to pristine crystalline TTF. Our work establishes B←N superlattice cocrystallization as a powerful strategy for engineering designer quantum materials, providing a general guideline for the development of high-performance organic qubits through structural and phononic modulation.
Khosravi A, Yuen HM, Fremin S
… +5 more, Pannilawithana NA, Supasueb N, Zhang Y, Liu P, Ngai MY
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333929
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Amino alcohols are prevalent in pharmaceuticals, agrochemicals, and functional materials, yet regioselective remote C─N bond formation from simple alkenes remains limited. We report a remote-Markovnikov formal 1,3-hydroa...Amino alcohols are prevalent in pharmaceuticals, agrochemicals, and functional materials, yet regioselective remote C─N bond formation from simple alkenes remains limited. We report a remote-Markovnikov formal 1,3-hydroamination of allyl carboxylates enabled by cooperative photoredox, cobalt, and Brønsted acid catalysis. The reaction proceeds via metal-hydride hydrogen atom transfer (MHAT) followed by 1,2-radical acyloxy migration (1,2-RAM) to generate a tertiary carbon-centered radical at a site remote from the original alkene, affording protected tertiary alkyl amino alcohols across a broad substrate scope, with secondary variants also accessible. Experimental and computational studies support a C─N bond-forming step best described as radical ligand transfer (RLT) at a Co(III)─N intermediate, rather than Co(IV)/S2 or carbocationic pathways. This rare nitrogen-transfer manifold accounts for the observed regioselectivity and catalyst-influenced stereochemical outcomes. By enabling migration-controlled 1,3-hydroamination, this strategy complements conventional 1,2-hydroamination and expands accessible amino alcohol chemical space.
Ma X, Zhang T, Sun C
… +3 more, Kuai Y, Li XX, Zheng ST
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333926
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This work investigates the first one-dimensional (1D) silver cluster-mediated polyoxotantalate molecular heterostructures of -[Ag-Ta]- (1g, 1y, and 1r), combining silver clusters as versatile emitting units and polyoxota...This work investigates the first one-dimensional (1D) silver cluster-mediated polyoxotantalate molecular heterostructures of -[Ag-Ta]- (1g, 1y, and 1r), combining silver clusters as versatile emitting units and polyoxotantalate as light propagation units. Its ultra-low waveguiding loss coefficient of (1.03 ∼ 1.63 × 10 dB/µm) demonstrates this assembly of silver clusters and polyoxotantalate as an efficient platform in designing active optical waveguides. The solvent-affected luminescent emission of silver clusters within this heterostructure enables the construction of emission-tunable (green, yellow, and red) waveguides. Furthermore, the local photoluminescent (PL) behaviors of a single crystal could be changed via local thermal treatment, leading to the formation of an optical heterojunction. Spatially PL resolved spectra also confirm heterojunction microrods exhibit an obvious optical waveguide effect with a low waveguide loss coefficient (2.22 ∼ 2.93 × 10 dB/µm) during propagation. This study not only represents the first example following the function decomposition discipline but also establishes new types of silver cluster-mediated polyoxotantalate-based low-dimensional ultralow-loss optical waveguides for advanced optical communication and information coding.
Liu M, Guo A, Wang F
… +6 more, Gu X, Wang X, Du Y, Liu X, Li L, Dong A
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333914
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Effective SF capture and recovery are essential for reducing greenhouse gas emissions and promoting resource recycling, yet many porous materials exhibit reduced separation performance for SF/N mixtures in humid environm...Effective SF capture and recovery are essential for reducing greenhouse gas emissions and promoting resource recycling, yet many porous materials exhibit reduced separation performance for SF/N mixtures in humid environments due to water adsorption competition or structural instability. To address this challenge, we propose a "superhydrophobic nanotrap" strategy by designing a nitrogen-rich superhydrophobic porous organic cage (POC) named IMUPOC-DA. This material incorporates a moisture-blocking shield of superhydrophobic isobutyl chains and an inner cavity with a π-system and Lewis base sites that synergistically enhance SF trapping. At 298 K and 1 bar, IMUPOC-DA achieves an SF adsorption capacity of 53.6 cm g and an SF/N uptake ratio of 20.02, a record-high reported thus far for POC-based adsorbents. More importantly, the superhydrophobic surface endows the material with an extremely low water uptake (72.1 mg g), a high water contact angle (150.11), and excellent water stability. Dynamic column breakthrough experiments under 80% relative humidity show nearly unchanged SF breakthrough time compared with dry conditions, demonstrating outstanding SF/N separation performance even in a moist environment. Therefore, this work not only provides a high-performance candidate for industrial SF recovery but also presents a general design strategy for developing moisture-resistant adsorbents for gas separation.
Shirai S, Makino T, Kajitani T
… +1 more, Tanaka M
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333913
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This study reports the first observation that a short self-complementary DNA oligonucleotide can self-assemble into two distinct liquid-crystalline architectures-long fibers and double-layered molecular tubes-upon therma...This study reports the first observation that a short self-complementary DNA oligonucleotide can self-assemble into two distinct liquid-crystalline architectures-long fibers and double-layered molecular tubes-upon thermal annealing. These two morphologies are determined by depletion forces tuned by the concentration of poly(ethylene glycol) (PEG) in solution. At lower PEG concentrations (25-30%), the depletion forces between duplexes are relatively weak. Under these conditions, nucleation occurs only at lower temperatures after sufficient duplex DNA has formed, leading to predominantly longitudinal growth and the formation of elongated DNA fibers. Small-angle X-ray scattering (SAXS) revealed a single columnar hexagonal packing structure within these fibers. At higher PEG concentrations (35-40%), the depletion forces become stronger. Under these conditions, nucleation occurs even at elevated temperatures, where the amount of duplex is still limited, leading to the formation of tubular assemblies. SAXS measurements conducted on the tubular DNA assemblies revealed two separate hexagonal lattice constants, suggesting differences in packing density between the inner core and the outer framework. This work establishes a new direction in DNA-based materials design, demonstrating that hierarchical liquid-crystalline architectures can emerge from a single short DNA oligonucleotide simply by tuning molecular crowding conditions.
Liu H, Guo W, Chang J
… +5 more, Liu J, He X, Niu S, Feng G, Bao F
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333912
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Aqueous ammonium-ion batteries (AAIBs) are promising energy storage devices, yet their development is hindered by the lack of high-performance electrode materials. While small-organic molecules possess structural tunabil...Aqueous ammonium-ion batteries (AAIBs) are promising energy storage devices, yet their development is hindered by the lack of high-performance electrode materials. While small-organic molecules possess structural tunability and diverse redox activity, their application is often limited by tedious synthesis, insufficient active-sites, and dissolution in electrolytes. Herein, we synthesize a small-organic molecule, DNQP, featuring multiple C═O/C═N redox-active centers, via a rapid microwave route. This method completes the condensation between -NH and C═O in 40 min (vs. 72 h for solvothermal), simultaneously introducing additional redox-active C═N bonds and extending the π-conjugated framework. Electronic structure analyses reveal that DNQP possesses an ultranarrow bandgap (1.053 eV), a highly delocalized π-conjugated framework, and favorable π-π stacking channels for charge transport. These features, combined with a chelation-coordination storage mechanism, enhance electron transfer, structural stability, and multi-electron reactivity. As a result, DNQP achieves 79% redox-site utilization, delivering a four-electron capacity of 155.9 mAh g at 0.1 A g, and exhibits remarkable cycling performance over 12 000 cycles at 5 A g. A DNQP//α-MnO full-cell retains 99% capacity after 2000 cycles. Mechanism studies elucidate a reversible two-step, four-electron NH storage process governed by N─H⋯O/N─H⋯N H─bonding. This work offers a rational molecular design and rapid synthesis for high-performance AAIBs organic materials.
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333907
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Developing quasi-solid-state composite electrolytes (QSCEs) that combine high interfacial stability with rapid ion transport remains a key challenge for constructing long-life, ultrahigh-rate lithium metal batteries (LMB...Developing quasi-solid-state composite electrolytes (QSCEs) that combine high interfacial stability with rapid ion transport remains a key challenge for constructing long-life, ultrahigh-rate lithium metal batteries (LMBs). Herein, a highly interface-stable and ion-conductive QSCE (denoted as PSI) is developed by utilizing poly(ionic liquid)-grafted porous silica hybrid molecular brush (SiO-g-PILDFOB) as a multifunctional filler. The synergistic effect of boron and fluorine in poly(ionic liquid) side chains promotes the formation of a highly stable solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI), significantly enhancing interfacial compatibility with highly active electrodes. Meanwhile, porous silica provides continuous transport channels for lithium ions, substantially improving lithium-ion transport efficiency. As a result, the Li|PSI|NCM9055 full cell achieves a long cycle life of 1000 cycles at an ultrahigh rate of 8 C. Moreover, under a high cut-off voltage of 4.4 V, the Li|PSI|NCM9055 pouch cell with a high cathode loading (6.9 mg cm) exhibits a specific discharge capacity of 200.9 mAh g at 0.7 C and demonstrates a long lifespan of 500 cycles. A 1.54 Ah pouch cell with an energy density of 413 Wh kg can also be achieved by using high-loading cathodes (21 mg cm). This work provides a feasible design strategy for developing ultrahigh-rate and high-voltage LMBs.
Dong W, Tian H, Hu Y
… +6 more, Xia Y, Bian Z, Feng W, Wen K, Qi X, Zhao W
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333901
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Metathesis reactions are fundamental transformations in organic synthesis, enabling efficient reorganization of unsaturated bonds and underpinning broad applications in pharmaceuticals, functional materials, and polymer...Metathesis reactions are fundamental transformations in organic synthesis, enabling efficient reorganization of unsaturated bonds and underpinning broad applications in pharmaceuticals, functional materials, and polymer science. To date, the conceptual and methodological development of metathesis transformations has been focused predominantly on carbon-carbon unsaturated bonds, and strategies that combine unsaturated bond reorganization with the direct incorporation of heteroatoms remain rare. Additionally, the established metathesis methodologies have been developed typically within the framework of transition metal catalysis, and transition metal-free alternatives are scarcely explored. Here, we demonstrate that borata-alkenes can serve as non-metal alkylidene surrogates to enable a transition metal-free hetero-enyne metathesis to access cyclopentene derivatives. This process accommodates diverse electrophiles and can be integrated into cascade sequences, allowing three- and four-component couplings from readily accessible 1,1,1-triborylalkanes. The resulting chemodivergent products include cyclopentenyl boronic esters, geminal borylsilylalkanes, conjugated dienes, and, in a sequential four-component variant, highly substituted ketones and enol ethers. Mechanistic studies and density functional theory (DFT) calculations support a borata-alkene-mediated metathesis pathway, establishing a transition metal-free approach for cyclopentene synthesis via carbon-carbon bond reorganization.
Yan Y, Fan Y, Wang R
… +9 more, He J, Lu Z, Yang Y, Xia Z, Pan Y, Leng S, Zhu Z, Wang S, Zou Y
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333896
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N, N-Dimethylformamide (DMF) is a widely used chemical reagent often described as a "universal solvent" due to its exceptional solvating capabilities. A sustainable synthesis route involves the green electrochemical coup...N, N-Dimethylformamide (DMF) is a widely used chemical reagent often described as a "universal solvent" due to its exceptional solvating capabilities. A sustainable synthesis route involves the green electrochemical coupling of CO with dimethylamine (DMA). However, the rational design of highly efficient catalysts for this transformation remains constrained by a limited mechanistic understanding of the key reactive intermediates governing the process. In this study, *COO is identified as the pivotal intermediate facilitating C─N coupling, a finding substantiated by in situ Fourier transform infrared spectroscopy (FT-IR) and online differential mass spectrometry (DEMS). Complementary Raman spectroscopy analyses further revealed that the intermediate adopts a stable chair-like configuration, characterized by dual-coordinated adsorption through both C and O atoms. Based on these mechanistic insights, a ZnCu catalyst was engineered that facilitates efficient CO activation while simultaneously stabilizing this adsorption configuration, thereby enhancing the C─N coupling pathway. As a result, a DMF Faradaic efficiency (FE) of 51% and a production rate of 575 mmol·g·h are achieved, outperforming all previously reported catalytic systems under comparable conditions. This study establishes a robust framework for understanding and optimizing C─N coupling via precise intermediate stabilization.
Jiang L, Ma J, Liu Y
… +3 more, Peng L, Tian Y, Zhou S
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333893
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The clinical utility of classical metallodrugs is limited by insufficient tumor selectivity and systemic toxicity. Platinum-based chemotherapeutics, while foundational in oncology, exemplify this challenge because of the...The clinical utility of classical metallodrugs is limited by insufficient tumor selectivity and systemic toxicity. Platinum-based chemotherapeutics, while foundational in oncology, exemplify this challenge because of their indiscriminate action on both cancerous and healthy cells, leading to detrimental side effects. Inspired by the versatile coordination chemistry in metalloproteins, we developed a platinum(IV)-based metallo-stapling strategy to construct tumor-specific metalloprodrugs. This approach leverages the Pt(IV) complex dually as a chemotherapeutic agent and a structural staple that conformationally rigidifies an epidermal growth factor receptor (EGFR)-targeting ligand. The resultant macrocyclic metalloprodrug exhibits precise targeting of EGFR-overexpressing malignancies, achieving in vivo tumor platinum accumulation 7-fold higher than the parent Pt(II) complex and 5-fold greater than its linear counterpart due to superior metabolic stability and efficient receptor-mediated uptake conferred by the macrocyclic architecture. Upon reaching the tumor microenvironment, the construct undergoes dual-payload release to liberate platinum drug and the IDO-1 inhibitor NLG919, eliciting a robust immunogenic cell death cascade while simultaneously reversing immunosuppression. Furthermore, a combination with an aPD-L1 immune checkpoint blockade produces a marked synergistic antitumor response. This work establishes Pt(IV)-directed metallo-stapling as a versatile platform for precision cancer therapy, offering a generalizable strategy to chemically engineer a broad range of metalloprodrugs with enhanced tumor selectivity and biosafety.
Li X, Wang X, Deng L
… +8 more, Ji X, Tu Y, Liu C, Wang Z, Wang L, Ye X, Yang Y, Zhang Q
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333892
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Escherichia coli (E. coli), Shigella dysenteriae (S. dysenteriae), and Proteus vulgaris (P. vulgaris) are the leading bacterial causes of death and diseases in many countries. Vaccines are economical and effective tools...Escherichia coli (E. coli), Shigella dysenteriae (S. dysenteriae), and Proteus vulgaris (P. vulgaris) are the leading bacterial causes of death and diseases in many countries. Vaccines are economical and effective tools against bacterial infection. Herein, we present the first total synthesis and immunological evaluation of the E. coli O29, S. dysenteriae serotype 11, and P. vulgaris O12 O-antigen decasaccharides, pentasaccharides, and related oligosaccharide fragments. We found that the hexasaccharide, including two repeating units of the core trisaccharide, was the optimal epitope, which was conjugated with the carrier protein CRM197 to furnish a semisynthetic glycoconjugate vaccine. The glycoconjugate vaccine induced a robust antigen-specific immune response, and the antibody sera could recognize the surface O-antigens of E. coli O29. This glycoconjugate vaccine, including a common trisaccharide fragment, existed in many bacterial O-antigens, which can be further used as a potential broad-spectrum vaccine against E. coli, S. dysenteriae, P. vulgaris, and Cronobacter malonaticus (C. malonaticus).
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333889
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Fluorination strategies for electrolyte solvents are widely used to improve the electrochemical performance and cycling stability of Li-metal batteries. Recently, β-fluorinated 1-ethoxy-2-methoxyethane (FxEME) has been d...Fluorination strategies for electrolyte solvents are widely used to improve the electrochemical performance and cycling stability of Li-metal batteries. Recently, β-fluorinated 1-ethoxy-2-methoxyethane (FxEME) has been designed and shown to exhibit excellent oxidative stability. However, solvent design remains largely empirical, and its atomistic-level effects are not fully understood. Here, we investigated how fluorination affects the oxidative stability of asymmetric ethers, (Fx)EME, using multiscale modeling with density functional theory (DFT), ab initio molecular dynamics (AIMD), and machine-learning force field (MLFF)-MD. DFT and AIMD capture fluorination-induced electronic-structure changes with high accuracy, while MLFF-MD enables exploration of interfacial reactions at larger time and length scales. Our results indicate that β-fluorination stabilizes ethoxy C-H bonds via inductive effects and weakens solvent-cathode (LiNiO) interactions through electron redistribution, mitigating oxidation and C-C activation. Furthermore, the increased dipole moment of F3EME drives a preferential orientation that shields the methoxy group. Overall, these three fluorination-induced effects confer FxEME significantly higher oxidative stability than EME. This work provides atomistic insights into fluorination-driven electronic and interfacial effects, supporting rational electrolyte design.
Li H, Qian L, Zhang C
… +4 more, Cheng K, Mu W, Zuilhof H, Wang X
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333880
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Artificial synthesis of compounds to mimic the catalytic functions of natural enzymes and investigate their underlying mechanisms is challenging work. The development of glycoside hydrolase mimics encounters significant...Artificial synthesis of compounds to mimic the catalytic functions of natural enzymes and investigate their underlying mechanisms is challenging work. The development of glycoside hydrolase mimics encounters significant obstacles due to the complex stereochemistry and reaction mechanisms involved. Metal-organic frameworks (MOFs) have become promising candidates for artificial enzymes due to their ordered structure and ability to precisely control the active sites. Herein, a bimetallic MOF (CZPDC) containing bimetallic nodes is synthesized as an enzyme mimic to hydrolyze glycosidic molecules. X-ray absorption near-edge structure confirms the coexistence of Ce and Zr in the metal cluster nodes. DFT calculations reveal the unique adsorption behavior of CZPDC toward the negatively charged functional group connected to the C atom at the C2 position on the Ce site, thereby avoiding the stereoisomerism-induced selectivity between glycoside atoms and heteroatom carbons, making it suitable for the degradation of more complex polysaccharide systems. The catalytic behavior enables efficient hydrolysis of complex biological tissues containing multiple chemical bonds, disrupts bacterial biofilms, and kills internal bacteria. These characteristics endow CZPDC with strong potential for application in areas such as glycoside-catalyzed hydrolysis and bacterial biofilm removal.
Li X, Liu Z, Wen X
… +6 more, Jiang J, Qiu S, Wang Y, Liu J, Jiang W, Wang Z
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333877
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Improving the emission efficiency of chiral π-systems is of significance for their practical applications in materials science. Herein, we report a family of highly emissive double π-helical molecular carbons featuring a...Improving the emission efficiency of chiral π-systems is of significance for their practical applications in materials science. Herein, we report a family of highly emissive double π-helical molecular carbons featuring a cyclooctatetraphenylene (COTt) or cyclooctahexaphenylene (COTh) core. In contrast to previously reported non-emissive tetrabenzo-COTt derivatives, the introduction of nitrogen via diarylamine/carbazole fusion leads to fluorescence quantum yields as high as 98%. The high configurational stability of these double π-helices enabled successful chiral resolution of their enantiomers using high-performance liquid chromatography. Notably, structural evolution from the COTt to the COTh core results in an approximately three-fold increase in the luminescence dissymmetry factor (g), while the circularly polarized luminescence (CPL) brightness reached 110 M cm, among the highest values reported for cyclooctatetraene (COT)-based chiral molecular carbons. Theoretical calculations further support these results, revealing large electric transition dipole moments (|μ|) and perfect parallel/antiparallel alignment between the μ and magnetic transition dipole moments (m). Our work provides valuable insight into the molecular design of high luminescent chiral emitters.
Liu J, Wang B, Wang Z
… +5 more, Sun Y, Zhang Z, Yang Y, Qiao Z, He B
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333872
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Membrane-based direct air capture (m-DAC) offers an energy- efficient route to mitigate rising atmospheric CO, but its practical deployment is hindered by low CO concentration and high humidity. Herein, we propose a "Sai...Membrane-based direct air capture (m-DAC) offers an energy- efficient route to mitigate rising atmospheric CO, but its practical deployment is hindered by low CO concentration and high humidity. Herein, we propose a "Sailing-with-Water" strategy that turns humidity from an obstacle into a mass-transfer driving force. The bifluorinated motifs are engineered by integrating fluorinated ionic liquid@UiO66 (IL@UiO) as porous fillers and a novel polymer, PIM-1DFBP, as the second fluorine source. The abundant fluorine sites within the membrane facilitate CO capture and enrichment from dilute streams via Lewis acid-base interactions. Notably, under high humidity conditions, the fluorine sites in the membrane form a hydrogen-bond network with water molecules, creating a polar microenvironment that further enhances CO affinity and builds ultrafast channels for CO permeation. The optimized membrane achieves a CO permeability of 12697.08 Barrer and CO/N selectivity of 44.06 under 65% relative humidity, surpassing the 2019 Robeson upper bound. The membrane also exhibits 180-days stability, large-area defect-free fabrication, and process simulation shows that only 612.37 m is needed to reach 40% CO outlet concentration. This work provides a humidity-resistant paradigm for high-performance m-DAC.
Li JX, Zhuo WZ, Jiang MY
… +3 more, Lin Y, Zhu YS, Su B
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333871
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The enantioselective construction of acyclic quaternary carbon stereocenters and vicinal quaternary/tertiary stereocenters represents two persistent challenges in organic synthesis. Herein, we report a unified transient...The enantioselective construction of acyclic quaternary carbon stereocenters and vicinal quaternary/tertiary stereocenters represents two persistent challenges in organic synthesis. Herein, we report a unified transient boryl-assisted, catalytic enantioselective strategy that enables the synthesis of both isolated quaternary carbon stereocenters and vicinal quaternary/tertiary stereocenters. Central to this strategy are the boryl-organized stereodefined acyclic tetrasubstituted enolates and their subsequent stereoselective alkylation, achieved through highly enantioselective copper-catalyzed conjugate borylation of α-substituted α,β-unsaturated esters. The resulting borylative alkylation products are obtained with high enantio- and diastereoselectivity (up to 98% ee and > 20:1 d.r.) and undergo diverse downstream transformations of the boryl unit, providing versatile access to acyclic quaternary/tertiary stereocenters. Following its stereodirecting role, the boron unit can be removed in a one-pot protodeboronation to furnish esters bearing isolated α-quaternary stereocenters with high ee values (up to 94% ee). This catalytic strategy provides a general solution to the stereocontrolled alkylation of acyclic tetrasubstituted enolates and enables modular access to complex quaternary carbon architectures.
Cano-Blanco DC, Bellomi S, Bonavia D
… +5 more, Alxneit I, Lomachenko KA, Föttinger K, Kröcher O, Ferri D
Angew Chem Int Ed Engl
· 2026 Jun · PMID 42333868
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Hybrid materials based upon mixed metal oxides provide an effective strategy to boost catalytic performance through redox-induced interfacial engineering. Herein, we present an efficient catalyst toward NO decomposition...Hybrid materials based upon mixed metal oxides provide an effective strategy to boost catalytic performance through redox-induced interfacial engineering. Herein, we present an efficient catalyst toward NO decomposition containing short-range ordered RhO and CeO species anchored to the CoO spinel. The activity enhancement relative to CoO is non-additive with respect to the RhO/CoO and CeO/CoO interfaces and is uniquely linked to the modulation of the Co and Rh oxidation states at a synergistic Rh-O-Co-O-Ce interface. This ensemble provides increased redox flexibility and facilitated lattice oxygen activation, resulting in markedly enhanced NO decomposition. Kinetic analysis and operando modulated excitation x-ray absorption spectroscopy (ME-XAS) provide direct mechanistic evidence that NO decomposition proceeds via a multi-site, cooperative Mars-van Krevelen pathway, in which CoO-CeO acts as an oxygen reservoir enabling the redox cycling of RhO species. This study highlights the ability of mixed metal oxide catalysts to exploit interfacial effects to achieve improved activity in redox-mediated reactions and offers a rationale for the engineering of metal oxide-metal oxide catalysts guided by operando spectroscopy.