Xu Z, Yang Q, Fang W
… +3 more, Yuan W, Sui K, Shen Z
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42402185
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Supramolecular assemblies exhibiting circularly polarized luminescence (CPL) are attractive candidates for advanced photonic and optoelectronic materials. However, precise regulation of CPL output across distinct wavelen...Supramolecular assemblies exhibiting circularly polarized luminescence (CPL) are attractive candidates for advanced photonic and optoelectronic materials. However, precise regulation of CPL output across distinct wavelength regions remains challenging, particularly in systems that require the programmable integration of molecular structure, supramolecular chirality, energy transfer, and external-stimulus responsiveness. Herein, we report two chiral coumarin-based cholesterol amide derivatives that exhibit striking regioisomer-dependent assembly behavior and CPL properties. Notably, CHC-1 selectively forms long-range ordered chiral nanofibers in both polar and nonpolar solvents, giving rise to pronounced supramolecular chirality together with strong blue CPL activity. Single-crystal analysis and theoretical calculations jointly demonstrate that subtle structural isomerism has a pronounced impact on assembly activity. Moreover, co-assembly of CHC-1 with thioflavin T affords strong green CPL emission through efficient energy transfer. Furthermore, incorporation of the photoisomerizable spiropyran allows photoresponsive modulation of wavelength-dependent CPL behavior. Benefiting from the photoisomerization of spiropyran, the co-assembled gels show distinct near-infrared CPL emission. This work establishes a versatile strategy for constructing wavelength-dependent, multi-mode CPL supramolecular systems and highlights how structurally programmed assembly can be leveraged to regulate chiroptical properties in multi-component materials.
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42402184
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We report a general and modular chiral surrogate rotaxane (CSR) strategy for the synthesis of mechanically planar chiral rotaxanes (MPCRs) of high optical purity (ca. 99.6% ee). A diastereomeric CSR, readily separable by...We report a general and modular chiral surrogate rotaxane (CSR) strategy for the synthesis of mechanically planar chiral rotaxanes (MPCRs) of high optical purity (ca. 99.6% ee). A diastereomeric CSR, readily separable by column chromatography, is first generated through an S2 interlocking process in which a Na-templated directional macrocycle encircling a chiral nucleophilic auxiliary is captured by a semidumbbell-shaped electrophile. Subsequent displacement of the auxiliary with a semidumbbell-shaped nucleophile furnishes the target MPCR with complete stereochemical fidelity and quantitative recovery of the auxiliary. This scalable approach avoids reliance on preparative chiral stationary phase HPLC and supports stereochemical assignment by correlation, reducing the need for product-by-product x-ray crystallographic analysis. Moreover, the strategy provided access to all three stereoisomers of a co-conformationally mechanically planar chiral [3]rotaxane, each in 99.8% stereoisomeric purity. These results establish a practical platform for accessing stereochemically well defined mechanically chiral rotaxanes for systematic study and future functional applications.
Tian N, Ju H, Liu Y
… +7 more, Huang J, Luan Z, Hou Q, Chen Q, Zhang B, Huang J, Zeng MH
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397940
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Novel synthetic methods offer significant potential to accelerate drug development, yet there remains a largely unexplored area for efficiently synthesizing metal-based anticancer agents. Herein, we report a novel solvot...Novel synthetic methods offer significant potential to accelerate drug development, yet there remains a largely unexplored area for efficiently synthesizing metal-based anticancer agents. Herein, we report a novel solvothermal domino reaction of pyridine-2-methylamine (and its 4-OCH-substituted derivative), benzaldehyde, and CuCl∙2HO, which simultaneously achieves ligand synthesis and coordination assembly in one pot and facilely affords innovative dinuclear dicoordinate copper(I) complexes (Cu1 and Cu2) with the in situ-formed bulky steric-hindering tetraarylethane ligands featuring the bis-imidazo[1,5-a]pyridine scaffold. The unique geometry of Cu1 and Cu2 confers physiological stability and vacant coordination sites for efficiently catalyzing Fenton-like reactions. Further studies reveal that Cu2 effectively elevates intracellular copper ion levels to induce cuproptosis, concurrently disrupting cellular redox homeostasis to trigger ferroptosis. The concurrent cuproptosis-ferroptosis activation finally elicits significantly enhanced immunogenic cell death (ICD), which facilitates the antitumor activity of Cu2. Moreover, in combination with immune checkpoint inhibitor αPD-1, Cu2 exhibits improved immunotherapy effects. This work introduces the first small-molecule copper complex that achieves immunotherapy potentiation through cuproptosis-ferroptosis-ICD induction and provides a new pathway for accessing innovative metal-based antitumor agents through such a rationally designed domino reaction.
Li WH, Ma YX, Ye YP
… +3 more, Zhu YN, Lv Q, Wang XD
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397893
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Two-dimensional (2D) organic crystals have attracted significant attention due to their highly ordered structures and exceptional optoelectronic properties. However, the conventional forms are often limited to simple geo...Two-dimensional (2D) organic crystals have attracted significant attention due to their highly ordered structures and exceptional optoelectronic properties. However, the conventional forms are often limited to simple geometries, restricting functional diversity. Therefore, developing structural designs to overcome the limitation is of critical importance. Herein, we report a preparation route for mirror-symmetric V-shaped 2D organic crystals by utilizing differential attachment energies across crystal facets, combined with temperature, solution concentration, and viscosity to promote crystal growth, resulting in the synthesis of V-shaped crystals and the transition from 1D to 2D architectures. The two arms of the V-shaped crystal exhibit mirror symmetry, and half of the angle between the two arms is approximately 67°. According to the optical waveguide tests, 2D crystal exhibits an optical loss coefficient as low as 0.075 dB/µm. In the V-shaped 2D homostructure, photons propagate uniformly within each arm but exhibit an abrupt intensity change at the interface, revealing asymmetric waveguide behavior and altering photon transport pathways, forming an angle of about 134° with the original path. This work provides new insights into the precise fabrication and functional integration of unconventional organic crystals.
Wang Y, Luo Y, Wu L
… +5 more, Chen J, Duan M, Rasool A, Wang Y, Zhu S
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397890
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Transition-metal-catalyzed migratory cross-coupling offers an attractive strategy for converting readily available precursors into complex molecular architectures. However, current methods are typically restricted to a s...Transition-metal-catalyzed migratory cross-coupling offers an attractive strategy for converting readily available precursors into complex molecular architectures. However, current methods are typically restricted to a single migratory mode (e.g., chain-walking, through-space shift, or E/Z isomerization). Integrating multiple mechanistically distinct migratory events within a selective cross-coupling manifold to unlock new chemical space and diverse isomeric products remains a formidable challenge. Herein, we report a cobalt-catalyzed, migratory E-selective asymmetric aza-NHK (Nozaki-Hiyama-Kishi) coupling of ortho-iodophenylethylenes with imines. The key to this process is a synergistic sequence that combines a through-space 1,4-Co/H shift with alkenylcobalt E/Z isomerization. Notably, mixtures of E/Z-alkenyl bromides are also viable substrates, undergoing an unprecedented alkenylcobalt E/Z isomerization prior to E-selective asymmetric coupling. This method provides efficient access to high-value α-chiral (E)-allylic amines with exceptional control over regio-, E/Z-, and enantioselectivity.
Shi HN, Wang YX, Zhang KJ
… +8 more, Han XW, Zhou YY, Gao Y, Sun XL, Wang K, Zhao Y, Fu Q, Tang Y
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397887
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AA-type α,ω-dihydroxy telechelic polyolefins (tPOs) are key macromonomers for the step-growth construction of circular polyolefin(-like) materials and, in particular, block-level sequence-controlled olefin block copolyme...AA-type α,ω-dihydroxy telechelic polyolefins (tPOs) are key macromonomers for the step-growth construction of circular polyolefin(-like) materials and, in particular, block-level sequence-controlled olefin block copolymers (OBCs), yet a general route to α,ω-dihydroxy tPOs directly from commodity ethylene/α-olefins has remained inaccessible. Here, a catalyst-free tandem Zn-B exchange/oxidation enables near-quantitative conversion of CCTP-derived poly(ethylene-co-α-olefin) polymeryl-Zn intermediates into AA-type α,ω-dihydroxy tPOs with >95% difunctional ratios while preserving industrially relevant microstructures and allowing scale-up to ∼60 g per batch. These tPOs and their corresponding diester tPOs undergo polycondensation to afford alternating OBCs with controlled block lengths and tunable compositions. An architecture-controlled comparison with corresponding random analogs further shows that, although the overall composition primarily determines the total crystallinity, the alternating sequence leads to a more homogeneous nanoscale physical network, lower viscoelastic dissipation, more effective strain hardening, and improved cyclic stability with reduced stress relaxation. These results demonstrate that the AA-type telechelic platform not only expands telechelic polyolefin chemistry but also enables sequence-programmable polyolefin architectures with distinct and practically meaningful performance advantages, establishing sequence control as a powerful design lever for recyclable multiblock polyolefin materials.
Song Y, Zhang J, Zhang R
… +4 more, Li M, Han B, Zhang J, Ma J
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397886
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The atomically dispersed catalysts have received much attention due to maximum atom utilization and enhanced catalytic performance. Compared with the widely studied single-atom catalysts and dual-atom catalysts, the mult...The atomically dispersed catalysts have received much attention due to maximum atom utilization and enhanced catalytic performance. Compared with the widely studied single-atom catalysts and dual-atom catalysts, the multi-atom catalysts (MACs) have unique features of collective effect of multiple metal atoms and more designable and tunable coordination environments that are desirable for catalytic reactions. Up to now, the research on MACs remains quite scarce, mainly restricted by the synthetic difficulty in precisely controlling the composition and arrangement of multiple metal atoms in MACs. Herein, we report a versatile soft-hard dual template route for the synthesis of both mononuclear MACs and heteronuclear MACs, which are stabilized on interpenetrating multi-chambered N/C nanospheres. The as-synthesized Ni/Cu-MAC exhibits high performance for electrocatalytic CO reduction reaction, delivering a CO Faraday efficiency of >99% at low required potentials (-0.26 V to -0.56 V). A cathode energy efficiency >75% is achieved at an industrial current density of 0.60 A cm, representing highly competitive performance among the reported CO-to-CO electrocatalysts. The experimental and computational results demonstrate the synergistic effect between the atomically dispersed Ni and Cu for promoting the catalytic conversion of CO to CO.
Bi X, Li Q, Zhao N
… +14 more, Zhang Z, Wang Y, Huo K, Yu X, Li S, Bian Z, Han Y, Liu X, Yan Y, Wang W, Xu W, Liu Q, Tsubaki N, Wu M
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397884
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The rational design of highly efficient catalysts and the development of novel reaction pathways are eternal themes and central challenges in the field of chemical synthesis. Here, we design a dual-engine catalytic syste...The rational design of highly efficient catalysts and the development of novel reaction pathways are eternal themes and central challenges in the field of chemical synthesis. Here, we design a dual-engine catalytic system for CO hydrogenation to aromatics via a synergistic C alcohols/olefins pathway. The dual-engine catalytic system initiated by FeCo active sites and CuZnAl promoters guarantees the continuous C alcohols/olefins supply, delivering a record-breaking aromatics yield (31.1%) with the aid of aromatization component H-ZSM-5. Multiple characterization and theoretical simulations reveal that C alcohols trigger carbon-chain growth through oxonium-mediated rapid carbocation generation via a low-barrier "protonation-dehydration" sequence, whereas olefins serve as π-substrates to propagate carbon-chain. This synergy accelerates both oligomerization and subsequent aromatization, effectively circumventing both the sluggish initial C─C coupling of methanol-mediated pathways and the high-barrier direct protonation step in olefins-mediated pathways. Techno-economic analysis (TEA) further demonstrates the superior industrial viability of this novel process. This work establishes a new paradigm for designing efficient catalytic systems and engineering process toward sustainable CO valorization.
Li J, Yu X, Lu X
… +5 more, Zhang H, Gao X, Wang L, Zhu L, Wang Z
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397881
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Zeolite membranes hold significant promise for industrially relevant gas separations; however, balancing high permeance and selectivity remains a persistent challenge. Although thinning the selective layer improves perme...Zeolite membranes hold significant promise for industrially relevant gas separations; however, balancing high permeance and selectivity remains a persistent challenge. Although thinning the selective layer improves permeance, achieving precise fabrication remains a major bottleneck. Herein, we demonstrate a sacrificial seed layer strategy enabling the fabrication of hierarchical MFI zeolite membranes (HMFI) on commercial α-AlO tubes. Through precise modulation of synergistic ionic interactions within the synthetic gel and the nutrient supply rate during crystallization, the seed layer functions as both a porogen to generate a macroporous sublayer and a "fertilizer" to promote surface gel crystallization, forming a dense top layer. The resulting HMFI membrane delivers more than a fourfold enhancement in the ideal selectivity of n-butane and isobutane (n-/i-butane), accompanied by a 37% rise in n-butane permeance compared with conventional MFI membranes. Moreover, with a 10/90 n-/i-butane mixture, it exhibits an excellent separation factor of 158, along with a high n-butane permeance (188 × 10 mol m s Pa), representing the highest performance for reported membranes on tubular supports. The strategy not only enables a novel route to high-performance membranes, but also enriches the conceptual framework of the conventional secondary growth protocol, offering new avenues for microstructural engineering.
Qi S, Li N, Zhang L
… +7 more, Chen J, Guo X, Ma J, Chen Y, Ye Z, Yin X, Yang C
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397880
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Incorporating chirality into multi-resonance (MR) frameworks offers an attractive route to narrowband circularly polarized luminophores, yet chiroptical amplification is constrained by decoupling between chiral perturbat...Incorporating chirality into multi-resonance (MR) frameworks offers an attractive route to narrowband circularly polarized luminophores, yet chiroptical amplification is constrained by decoupling between chiral perturbation and MR-confined radiative transitions. Self-assembly amplifies chirality through helically coupled emissive dipoles, but its morphology-dependent order conflicts with efficient electroluminescence. Here, we establish a self-assembly-independent intramolecular amplification strategy based on a C-symmetric figure-eight macrocyclic MR architecture. Theoretical calculations reveal that transition-symmetry control and through-space interchromophoric coupling strengthen intramolecular chiral exciton interactions while preserving intrinsic MR emission. TmCz-[10]AD integrates narrowband emission, fast reverse intersystem crossing of 2.31 × 10 s, high photoluminescence quantum yield and a dissymmetry factor (|g|) approaching 10, enabling solution-processed organic electroluminescent (EL) device with a maximum external quantum efficiency exceeding 20.5% and an |g| value of 6.2 × 10.
Yang D, Wang C, Zhou X
… +6 more, Zhao X, Tan H, Gao H, Yu F, Wang Y, Li Y
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397875
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Smart covalent organic frameworks capable of modulating photocatalytic properties responsive to external stimuli represent next generation of emerging catalysts sought by researchers, yet studies on these dynamic materia...Smart covalent organic frameworks capable of modulating photocatalytic properties responsive to external stimuli represent next generation of emerging catalysts sought by researchers, yet studies on these dynamic materials and structure-activity relationships remain scarce. Herein, we report a smart metal covalent organic framework (Cu-MCOF) incorporating copper cyclic trinuclear clusters (Cu) as redox-active and structurally adaptive nodes, which exhibits dual responsiveness to hydrogen bromide (HBr) stimulation, undergoing reversible imine protonation and Br-mediated reconstruction of copper nodes. These transformations induce pronounced narrowing of optical gap from 2.50 eV to 2.02 eV, a redshift in absorption onset from 500 nm to 613 nm, and enhanced charge separation efficiency. Consequently, Cu-MCOF-HBr achieves 40-fold increase in photocatalytic activity for α-terpinene oxidation, with superoxide radical selectivity exceeding 99%, compared to 41% for Cu-MCOF. The same stimulus-triggered enhancement is demonstrated in the photocatalytic 1,2,4-trimethoxybenzene bromination. Spectroscopic studies and density functional theory (DFT) calculations reveal that synergistic imine protonation and cluster restructuring promote electron localization within Cu units, facilitate spatial charge separation, and shift oxygen adsorption to imine sites, thereby selectively promoting superoxide radical generation. This work provides the smart MCOF photocatalyst based on dynamic metal-cluster nodes and offers fundamental insights into stimulus-driven regulation of photocatalytic pathways and selectivity.
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397857
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Herein, we report isolable donor-acceptor-stabilized Si-E-Si trimetallylenes (E = Ge (2), Sn (3), Pb (4); Si = Mes(cAAC)Si; Mes = 2,4,6-MeCH; cAAC = C(CH)(CMe)N-2,6-PrCH), stabilized by a cyclic alkylaminocarbene attache...Herein, we report isolable donor-acceptor-stabilized Si-E-Si trimetallylenes (E = Ge (2), Sn (3), Pb (4); Si = Mes(cAAC)Si; Mes = 2,4,6-MeCH; cAAC = C(CH)(CMe)N-2,6-PrCH), stabilized by a cyclic alkylaminocarbene attached to the divalent Si atoms. They were synthesized through salt-metathesis reactions of the dimeric silanylidene anion (SiK) 1a and EX precursors (X = Cl, N(SiMe)). Computational analyses reveal that 2-4 adopt bent donor-acceptor-stabilized Si-E-Si frameworks featuring polarized Si-C(cAAC) π interactions together with delocalized Si-E π interactions involving the Lewis-acidic E center. This donor-acceptor electronic structure results in small HOMO-LUMO gaps, giving rise to pronounced near-infrared (NIR) absorption. Remarkably, the one-electron reduction of 2 and 3 leads to the Ge- and Sn- radical anions 2 and 3, respectively, thereby highlighting that this donor-acceptor motif can even stabilize heavy Group 14 elements in lower oxidation states.
Zhang H, He T, Liu C
… +10 more, He L, Ye Z, Yan K, Zhang Y, Wang Z, Xu S, Zhang H, Cao XM, Zhang Y, Tang Y
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397853
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The direct synthesis of ultrathin MWW zeolites with precisely controllable aluminum location represents a significant challenge. Herein, we report a sustainable approach using cycloketones as secondary nitrogen-free orga...The direct synthesis of ultrathin MWW zeolites with precisely controllable aluminum location represents a significant challenge. Herein, we report a sustainable approach using cycloketones as secondary nitrogen-free organic structure-directing agents (NF-OSDAs) to fabricate two-dimensional (2D) MWW zeolites. Cyclobutanone (Cy4) directs the formation of ultrathin nanosheets featuring expanded interlayer spacing and tunable aluminum distribution. We demonstrate that Na-cycloketone complexes selectively occupy specific pore environments, effectively reducing the population of T-T framework aluminum (Al) sites and migrating to T Al sites, promoting external Brønsted acidity. The resulting Cy4-MWW catalyst exhibits outstanding performance in bulky-molecule transformations. Mechanistic studies reveal that cycloketones undergo in situ self-condensation to generate dimeric species that function as pivotal structural directors. Their steric presence affects layer thickness and nanosheet packing, whereas their Na-coordinated forms strongly interact with T Al sites, thereby driving aluminum migration from the confined T-T Al positions to accessible T Al sites. This strategy exhibits broad versatility across a range of cycloketones (Cy4-Cy10), enabling the concurrent tuning of both the MWW architecture and its aluminum distribution.
Yang B, Liu Y, Zhang S
… +8 more, Jiang B, Tian D, Wang F, Zhang C, Han S, Yang Z, Liu L, Fu N
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397851
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Covalent organic frameworks (COFs) hold great promise for advancing lithium-ion battery (LIB) cathode performance and overcoming resource bottlenecks due to their abundant elemental synthesis, tunable functionality, and...Covalent organic frameworks (COFs) hold great promise for advancing lithium-ion battery (LIB) cathode performance and overcoming resource bottlenecks due to their abundant elemental synthesis, tunable functionality, and stability. However, most COF cathodes commonly suffer from relatively low redox potential and/or poor charge-storage capability, which limits their energy densities. Here, we report the rational design of a p-type high-redox-potential COF by polymerizing 10,15-dihydro-5,10,15-triethyl-5H-diindolo[3,2-a:3',2'-c]carbazole-3,8,13-triamine (TAT-NH) and 9-methyl-9H-carbazole-3,6-dicarboxaldehyde (Cz-CHO) building blocks (namely, TAT-Cz COF). The COF features an extended π-conjugated framework and a moderate pore size (∼2.3 nm), enabling efficient anion transport and insertion/de-insertions. More importantly, by engineering high-redox-potential nitrogen sites into the COF, a high operating working voltage (3.0-4.5 V vs. Li/Li) is achieved. As an LIB cathode, it delivers a high reversible capacity of 131 mAh g at 0.1 C, along with excellent rate performance (65 mAh g at 20 C). Additionally, it demonstrates exceptional cycling stability, retaining 76 mAh g after 3000 cycles at 1.0 C with only 0.0114% capacity decay per cycle. In situ spectra and theoretical calculations reveal a highly reversible charge-storage mechanism involving N radical cations coordinated with PF anions. This work provides insights for developing high-redox-potential COFs with tailored structures and enhanced performance for high-energy-density organic cathodes.
Hao Y, Chen J, Hu N
… +4 more, Lan Y, Jia L, Li SJ, Jia S
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397847
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We report a synergistic photoredox/copper-catalyzed radical cascade cyclization for the enantioselective synthesis of axially chiral medium-sized lactones. Compared with conventional ionic pathways that require stringent...We report a synergistic photoredox/copper-catalyzed radical cascade cyclization for the enantioselective synthesis of axially chiral medium-sized lactones. Compared with conventional ionic pathways that require stringent polarity matching and substrate prefunctionalization, the present strategy employs alkyl halides as radical precursors, wherein photoredox mediated single electron transfer (SET) generates radicals that undergo radical addition to non-polarized alkenes followed by C-O bond formation. High stereocontrol and efficiency are achieved through a carboxylate-coordinated chiral copper complex (up to 83% yield, up to 96% e.e., >20:1 d.r.). The synthetic utility is demonstrated by the late-stage diversification of bioactive molecules. Theoretical calculations reveal that the stereodetermining step occurs during C-O bond formation, and that thermodynamic stability facilitates a central-to-axial chirality relay, thereby governing axial stability in the flexible seven-membered scaffolds.
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397845
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"The most exciting thing about my research is the moment of being the first in the world to discover and witness the mysteries of nature… If I were a piece of lab equipment, I would be a micropipette because I am precise..."The most exciting thing about my research is the moment of being the first in the world to discover and witness the mysteries of nature… If I were a piece of lab equipment, I would be a micropipette because I am precise, reliable, and always ready to deliver the right amount of effort…" Find out more about Huasong Ai in his Introducing… Profile.
Zhang F, Dong Y, Liu K
… +8 more, Hu H, Chang H, Zuo J, Ma X, Xu J, Dang Y, Wang X, Liang H
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397842
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Immune checkpoint blockades have shown great potential in cancer therapy. However, achieving efficient recruitment and activation of T cells while blocking immune suppression remains a critical challenge. Current strateg...Immune checkpoint blockades have shown great potential in cancer therapy. However, achieving efficient recruitment and activation of T cells while blocking immune suppression remains a critical challenge. Current strategies mainly focus on the blockade of the PD-1/PD-L1 axis, with limited attention to reprogramming immune functions on the tumor cell surface. Here, we report a "localized oxidation-covalent assembly" strategy that achieves precise modification of PD-L1 on the cell surface through glycan oxidation, thereby harnessing bioorthogonal reactions to induce the in situ construction of artificial topological nanostructures (ATNs), which subsequently augment T cell-mediated antitumor immunity. ATNs not only block the PD-1/PD-L1 axis to relieve immune suppression but also recruit and activate T cells through transmembrane bridging interactions, mimicking bispecific T cell engagers (BiTEs) and markedly enhancing antitumor immune responses. Mechanistic studies revealed that N-glycosylation sites are critical for probe-mediated aldehyde modification of PD-L1. We further demonstrated that the ATNs achieve spatially precise T cell recruitment and activation via PD-L1-dependent localization, enabling programmable immune regulation. Overall, this approach not only underscores the potential of glycan oxidation-driven self-assembly in immune modulation but also provides a versatile chemical biology tool for the precise reprogramming of immune checkpoint functions.
Zhao Y, Zhao Z, Chen HC
… +12 more, Sun X, Li Q, Li D, Hua Y, Zhao H, Chen S, Su Y, Gao Z, Xi K, Xiao C, Ding S, Zeng L
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397837
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Publisher ↗
Ru atomic clusters (AC) are promising cost-effective platinum-group-metal anode catalysts for the alkaline hydrogen oxidation reaction (HOR) in anion-exchange-membrane fuel cells (AEMFCs), yet their practical application...Ru atomic clusters (AC) are promising cost-effective platinum-group-metal anode catalysts for the alkaline hydrogen oxidation reaction (HOR) in anion-exchange-membrane fuel cells (AEMFCs), yet their practical application remains limited by insufficient structural robustness and sluggish proton transport across the electrolyte/electrode interface. Herein, we report a design concept that leverages p-block indium single atoms with In-NO coordination as electronic bridges to stabilize Ru AC and reconstruct a proton-conductive interfacial hydrogen-bond network for efficient and durable HOR catalysis in practical AEMFCs. We find that the bridged In-NO sites establish strong covalent Ru-In anchoring interactions through pronounced d-p orbital hybridization, stabilizing Ru AC against coalescence and detachment for markedly improved operational durability. Meanwhile, electronic coupling between Ru AC and bridged In-NO sites tunes surface oxophilicity of Ru to promote higher coverage of hydroxyl adsorbate species and drive dynamic reorientation of interfacial water from cation-bound states toward free water in the gap region, thereby reinforcing hydrogen-bond connectivity and enabling more efficient interfacial proton transport. The resulting Ru AC/In@CNO delivers a mass activity of 7.17 A mg , surpassing Pt/C by 9.0-fold. Particularly, Ru AC/In@CNO-based AEMFCs achieve a high peak power density of 1.33 W cm and maintain stable operation for over 50 h at 500 mA cm.
Ma GT, Ren BH, Yue TJ
… +4 more, Peng WX, Ren WM, Liu Y, Lu XB
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397836
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Efficient and selective chemical recycling of commercial plastics back to monomers is a pivotal strategy for achieving a circular plastics economy. However, rare catalysts can deliver versatility in both polymerization a...Efficient and selective chemical recycling of commercial plastics back to monomers is a pivotal strategy for achieving a circular plastics economy. However, rare catalysts can deliver versatility in both polymerization and depolymerization processes. Herein, we report an efficient and tolerant dinuclear zinc catalyst for the bulk depolymerization of various polyesters and polycarbonates to the corresponding cyclic monomers with >99% selectivity, and for repolymerization to virgin materials, through an intramolecular bimetallic synergistic dual-activation mechanism. A record-breaking activity of up to 43 kg of polymer/g of catalyst per hour was observed in the catalytic bulk poly(-lactic acid) depolymerization with microwave assistance. The catalyst could be recycled several times without obvious loss in activity and selectivity. This work provides an effective guideline for catalyst design that closes the loop for commercial plastics, offering a direct route to transform plastic waste into renewable feedstocks and advancing a truly sustainable materials economy.
Han D, Liu H, Li D
… +5 more, Lv M, Liu N, Cheng X, Chen Z, Yu WW
Angew Chem Int Ed Engl
· 2026 Jul · PMID 42397811
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Back-contacted architectures offer cost and stability advantages for perovskite solar cells (PSCs), yet their efficiencies have plateaued at ∼12% due to defect-induced recombination and limited carrier diffusion in thin...Back-contacted architectures offer cost and stability advantages for perovskite solar cells (PSCs), yet their efficiencies have plateaued at ∼12% due to defect-induced recombination and limited carrier diffusion in thin single crystals. Herein, a multi-dimensional defect suppression strategy is reported to overcome this bottleneck by incorporating N-methylformamidinium (MFA) into CsFAPbI (FA = CH(NH) ) crystals. MFA strengthens interaction between A-site cations with iodide ions, thereby suppressing iodide vacancies (point defects), relieving tensile microstrain, and eliminating dislocations and surface wrinkles (line and plane defects). This approach yields high-quality crystals with extended electron diffusion lengths (∼400 µm). As a result, an impressive efficiency of 17.35% is obtained, representing a substantial advance over reported back-contacted PSCs. Moreover, the devices exhibit excellent operational stability with no performance degradation after 1350 h of continuous light illumination. This work highlights the importance of suppressing multi-dimensional defects for enhancing carrier transport, which is instructive for developing efficient back-contacted PSCs.