Angew. Chem. Int. Ed. Engl. [JOURNAL]
Sun
200 papers
An Oxygen-Defect-Induced Unsaturated Coordination Strategy Boosts High-Selective PET Upcycling via Suppressing Oxygen Evolution.
Lu X, Song J, Guo Y … +8 more , Liang C, Liu Y, Wang Z, Cheng H, Zheng Z, Wu Y, Huang B, Wang P
Angew Chem Int Ed Engl · 2026 Jul · PMID 42397802 · Publisher ↗
Electrochemical upcycling of polyethylene terephthalate (PET) plastics coupled with hydrogen production offers a sustainable pathway for carbon reutilization and energy sustainability. However, PET-derived ethylene glyco...
Electrochemical upcycling of polyethylene terephthalate (PET) plastics coupled with hydrogen production offers a sustainable pathway for carbon reutilization and energy sustainability. However, PET-derived ethylene glycol electro-oxidation reaction (EGOR) in alkaline conditions inevitably competes with oxygen evolution reaction (OER) due to enhancing OH utilization for OER under industrially relevant high-current conditions, reducing electrolysis efficiency and degrading catalyst stability. In this study, we precisely regulate oxygen-defect concentration to construct an unsaturated CoFeO(OH)/CFP catalyst, achieving 93% ± 2% Faradaic efficiency (FE) for formic acid and over 700 h of stability. In situ characterizations and theoretical calculations show that oxygen defects tune the surface electronic structure and promote the timely consumption of electrochemically generated MO(OH) species by EG preventing the excessive accumulation of high-valence species and suppressing OH evolution into oxygenated OER intermediates. By balancing MO(OH) formation with its spontaneous reaction with EG, OH utilization toward EGOR is enhanced, enabling efficient OER suppression at high anodic potentials. Furthermore, a large-scale three-cell electrolyzer (300 cm per piece) achieves 17.4 A at 3 V with nearly 100% FE for hydrogen production, reducing energy consumption by > 21.05% compared with overall water splitting. This work provides mechanistic insights and a practical strategy for industrial PET upcycling integrated with low-energy hydrogen production.
Reprogramming Photosensitization Mechanisms for Hypoxic Tumor Therapy via Organic Photovoltaic-Inspired Heterojunctions.
Yan S, Qiao L, Guo WJ … +4 more , Xu S, Qi T, Tang BZ, Peng HQ
Angew Chem Int Ed Engl · 2026 Jul · PMID 42397801 · Publisher ↗
Conventional Type II photodynamic therapy (PDT) is severely compromised by tumor hypoxia. Drawing inspiration from the charge-separation principles of organic photovoltaics (OPV), we herein show that a molecularly predef...
Conventional Type II photodynamic therapy (PDT) is severely compromised by tumor hypoxia. Drawing inspiration from the charge-separation principles of organic photovoltaics (OPV), we herein show that a molecularly predefined donor-acceptor interface can re-route the excited-state fate of a classical Type II photosensitizer. Electrostatic co-assembly of cationic Y6-2Pr with anionic Rose Bengal (RB) furnishes a stoichiometrically defined 1:2 heterojunction, in which ultrafast intermolecular electron transfer gives rise to an interfacial charge-transfer-to-charge-separated (CT → CS) evolution. This process strongly attenuates triplet-mediated singlet-oxygen sensitization and redirects the photochemistry of RB toward a hypoxia-tolerant Type I pathway dominated by superoxide generation. The photogenerated holes concurrently oxidize NADH, establishing an interfacial photoredox cycle that weakens intracellular reductive defense. By translating a central concept of organic photovoltaic interfaces to photomedicine at the level of a stoichiometrically defined molecular complex, this work provides a route to retrofit classical Type II photosensitizers with Type I photoredox function.
Chemical Design Principles for Managing the Capacity-Stability Trade-Off in High-Voltage Sodium Layered Cathodes.
Zeng A, Qiu S, Cheng R … +4 more , Kang L, Liu P, Zhao E, Xiao X
Angew Chem Int Ed Engl · 2026 Jul · PMID 42397800 · Publisher ↗
High-voltage layered transition-metal (TM) oxides are attractive for sustainable sodium-ion battery (SIB) cathodes, yet their development is constrained by the persistent capacity-stability trade-off. Here, we establish...
High-voltage layered transition-metal (TM) oxides are attractive for sustainable sodium-ion battery (SIB) cathodes, yet their development is constrained by the persistent capacity-stability trade-off. Here, we establish a functional-unit-based design framework by decomposing the layered oxide lattice into active, buffer, and skeletal units that govern redox capacity, structural accommodation, and framework stability. Through systematic evaluation of TMO octahedra, NiO, MnO, and TiO are identified as representative functional units and integrated into a series of NaNi Mn Ti O (NMTxyz) oxides to validate functional cooperation. Binary and functionally mismatched ternary configurations exhibit poor or lopsided electrochemical behavior, whereas functionally matched architectures simultaneously deliver high capacity and durable stability, exemplified by NMT523 and NMT433 cathodes. To translate these insights into design guideline, two quantitative descriptors, active unit content and functional unit mismatch, are introduced to regulate the balance between capacity and cycling stability.
Tailoring the Electric Double Layer for Advanced Rechargeable Batteries: Mechanisms, Strategies, and Outlook.
Wu J, Zhang J, Zhang G … +4 more , Wang M, Wang X, Lin Q, Li B
Angew Chem Int Ed Engl · 2026 Jul · PMID 42397797 · Publisher ↗
The structure of the electric double layer (EDL) at the electrode/electrolyte interface functions not only as the physical arena for electrochemical reactions, but also as the fundamental determinant of battery kinetics,...
The structure of the electric double layer (EDL) at the electrode/electrolyte interface functions not only as the physical arena for electrochemical reactions, but also as the fundamental determinant of battery kinetics, interface stability, and cycle life. Although the solid electrolyte interphase (SEI)/cathode electrolyte interphase (CEI) film has been extensively studied, the microstructure and macroscopic performance of the EDL as precursor to interfacial film formation lacks systematical elucidation. This review aims to provide a comprehensive overview of the theoretical evolution of EDL models alongside their pivotal roles and regulation strategies in advanced batteries. We first retrace the development from classical Helmholtz models to modern microscopic theories. Subsequently, we delve into distinct regulation mechanisms and strategies tailoring EDL chemistry across various rechargeable battery systems such as Li-based, Zn-based and other metal-ion batteries. These approaches encompass electrolyte optimization, electrode engineering, interface modification, and external field regulation, intending to suppress side reactions, guide uniform metal deposition, and stabilize electrode interfaces. Furthermore, advanced techniques for simulating and characterizing the microstructure of the EDL are discussed. Finally, the review outlines current challenges and forward-looking perspectives on multidimensional rational design, data-driven screening, operando characterizations, and applications under extreme conditions, providing theoretical guidelines for interface engineering of next-generation batteries.
Interfacial Hydrogen Bonding for Efficient and Robust Flexible Tin Perovskite Solar Cells.
Wang Y, Tang G, Chen L … +11 more , Cao X, He D, Zheng K, Ha T, Yang L, Li K, Tang J, Yu L, Zeng L, Li J, Tai Q
Angew Chem Int Ed Engl · 2026 Jul · PMID 42397794 · Publisher ↗
Flexible tin perovskite solar cells (F-TPSCs) have attracted substantial attention owing to their high theoretical efficiency, eco-friendliness, and promising applications in wearable electronics and the internet of thin...
Flexible tin perovskite solar cells (F-TPSCs) have attracted substantial attention owing to their high theoretical efficiency, eco-friendliness, and promising applications in wearable electronics and the internet of things. However, the inferior quality of perovskite buried interfaces caused by low interfacial adhesion and large deformation of plastic substrates has seriously impaired the performance of F-TPSCs. Here, a biocompatible functional material, 1-chloro-1-deoxy-D-fructose (1-CDF), has been introduced into the poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) hole-transporting layer, which enables hydrogen-bonding interactions between PEDOT:PSS and both the underlying ITO and the top perovskite layer, thus significantly enhancing the interfacial adhesion. It can also regulate the crystallization dynamics of the perovskite, resulting in the growth of pinhole-free perovskite film with high crystallinity and homogeneous bottom contact. Besides, the incorperation of 1-CDF leads to conformation changes of the PEDOT:PSS, rendering higher conductivity and more matched energy level alignment with perovskites. The power conversion efficiencies (PCEs) of 15.56% (14.67% certified) and 11.06% are reached for F-TPSCs with active areas of 0.049 cm and 1 cm, respectively. In addition, the F-TPSC obtains an unprecedented PCE of 22.21% under 1000 lux indoor light illumination. The unencapsulated devices also exhibit excellent stability.
A Photocurable Covalent Polyoxometalates-Membrane With Hierarchical Proton Conduction Pathways for High-Performance Vanadium Flow Batteries.
Mu X, Yu F, Liu T … +7 more , Qiu T, Li T, Sun Z, Lang Z, Li Y, Wang Y, Tan H
Angew Chem Int Ed Engl · 2026 Jul · PMID 42397793 · Publisher ↗
Developing proton exchange membranes (PEMs) that integrate high conductivity, selectivity, and processability is highly challenging. Although polyoxometalates (POMs) are promising proton conductors, their practical appli...
Developing proton exchange membranes (PEMs) that integrate high conductivity, selectivity, and processability is highly challenging. Although polyoxometalates (POMs) are promising proton conductors, their practical application is hindered by poor processability, susceptibility to leaching, and difficulty in forming continuous proton conduction pathways within polymers. Herein, a new photocurable polyoxometalate (POM)-organic membrane (PAPOM-AMPS) is synthesized via ultrafast UV-initiated copolymerization of an acrylamide-functionalized arsenomolybdate cluster (APOM), 2-acrylamido-2-methylpropanesulfonic acid (AMPS), and acrylic acid (AA). This molecular-level design ingeniously constructs hierarchical proton transport channels: the covalently immobilized APOM clusters serve as long-range highways, while sulfonic (-SOH) and carboxylic (-COOH) acid groups synergize with water molecules to facilitate efficient proton dissociation and dynamic short-range hopping. The membrane exhibits an exceptional proton conductivity of 0.417 S·cm at 80°C and 100% RH, surpassing Nafion 117. With confined ionic domains (∼2.27 nm), it achieves ultrahigh proton/vanadium selectivity (18.1 × 10 S·min·cm), 4.6 times that of Nafion 117. When configured into a sandwich-structured membrane for vanadium flow batteries (VFBs), it delivers outstanding performance, including 98.2% coulombic efficiency, 86.7% energy efficiency, and exceptional cycling stability (0.12% capacity decay per cycle at 120 mA·cm). This work provides a groundbreaking strategy for next-generation high-performance proton-conductive membranes.
Boosting Photocatalytic Overall Water Splitting Activity of Phosphorene Through Five-Coordinate Passivation Enabled by Carbene Addition.
Zhang H, Li Y, Xu J … +10 more , Liu S, Wang T, Gao C, Du P, Ji H, Jiang J, Wang GW, Xiong Y, Baek JB, Yang S
Angew Chem Int Ed Engl · 2026 Jul · PMID 42397789 · Publisher ↗
Phosphorene is a promising two-dimensional semiconductor for solar-driven redox reactions, yet its practical deployment is severely restricted by rapid degradation under ambient conditions. Conventional covalent function...
Phosphorene is a promising two-dimensional semiconductor for solar-driven redox reactions, yet its practical deployment is severely restricted by rapid degradation under ambient conditions. Conventional covalent functionalization typically forms phosphorus-carbon single bonds (P─C), leaving phosphorus atoms in a four-coordinate environment and thus failing to fully quench the intrinsic reactivity associated with one residual unpaired electron. Here, we develop a selective strategy to achieve five-coordinate passivation of phosphorene by constructing phosphorus-carbon double bonds (P═C) through a one-step photochemical carbene addition reaction. Using a carbene precursor, adamantane groups are grafted onto phosphorene to afford a robust P═C-bonded architecture. Comprehensive spectroscopic analyses, together with density functional theory (DFT) calculations, validate the preferential formation of the P═C bonds. The resulting P═C-passivated phosphorene exhibits markedly improved ambient stability compared to the pristine and four-coordinate-passivated phosphorene. When utilized as a metal-free photocatalyst, the P═C-passivated phosphorene enables highly efficient overall water splitting without sacrificial agents under visible light, delivering record-high evolution of H and HO with rates of up to 612 and 658 µmol h g, respectively, along with excellent cycling stability.
Fundamentals, Measurement and Regulation of the Conductance of Single Molecule Junctions.
Yasini P, Batzinger K, Smeu M … +1 more , Borguet E
Angew Chem Int Ed Engl · 2026 Jul · PMID 42391312 · Publisher ↗
The miniaturization of conventional silicon-based devices is one of the pinnacles of achievement of the 20 century which evolved according to Moore's prediction, demanding a higher number and smaller size of electronic c...
The miniaturization of conventional silicon-based devices is one of the pinnacles of achievement of the 20 century which evolved according to Moore's prediction, demanding a higher number and smaller size of electronic components each year. One path forward is the incorporation of atoms and molecules as small, low-cost, and stable structures in electronic circuits and their integration into complex architectures which have been a desire of the nanoscale community for many decades. At the quantum physics scale, the unique physical and chemical properties of single molecules could lead to numerous new and interesting phenomena that are not accessible using conventional approaches, resulting in the emergence of a wide variety of device functionalities and applications, for example, nano-switches, single-molecule sensors, and spin filters. Although single-molecule electronics is still at an early phase, the investigation of charge transport through molecules and their dynamics at the nanoscale is fundamentally important to understand the relevant scientific concepts and technological applications. We briefly review the history of molecular electronics as well as the fundamentals and theories required to understand charge transport through molecules. We provide an overview of methods to fabricate single-molecule junctions with a focus on STM-based approaches, their advantages, and limitations. The review highlights new insights and the latest progress on the structure-property relationship of single-molecule junctions that includes the effect of anchoring groups, molecular orientation in the junction (anisotropy of conductance), molecule-electrode binding (denticity), and the role of solvent on charge transport at the nanoscale. We also highlight how advances in machine learning and molecular dynamics techniques have impacted theoretical and computation-based approaches to studying molecular electronics. We then summarize the contribution of advanced statistical analysis and machine-based approaches to the analysis of single-molecule conductance data. We wrap up the review with a discussion on new materials for molecular electronics, as well as current challenges and the outlook in the development of practical molecular electronics.
Quantitative Photoswitching of Spin States in o-Fluoroazobenzene-Loaded Metal-Organic Frameworks.
Chen KP, Li D, Miao Q … +3 more , Ye S, Ni ZP, Tong ML
Angew Chem Int Ed Engl · 2026 Jul · PMID 42391274 · Publisher ↗
The integration of photochromic guest molecules into spin-crossover (SCO) metal-organic frameworks (MOFs) offers a promising approach for optically regulating magnetic properties. Herein, we report a crystalline material...
The integration of photochromic guest molecules into spin-crossover (SCO) metal-organic frameworks (MOFs) offers a promising approach for optically regulating magnetic properties. Herein, we report a crystalline material, [Fe(bpn){Ag(CN)}]·E-FAB (1-E) (bpn = 1,4-bis(4-pyridyl)naphthalene and E-FAB = E-o-tetrafluoroazobenzene), which displays an asymmetric three-/four-step SCO behavior. At room temperature, the material undergoes efficient (90%) and reversible E/Z photoisomerization of guest molecules upon alternating irradiation with green (530 nm) and blue (410 nm) light. Following green-light irradiation, the crystal of 1-Z, containing 90% FAB in the Z configuration, was obtained via a light-induced single-crystal-to-single-crystal transformation. The E-to-Z isomerization of FAB introduces steric constraints within the pores, effectively locking the host framework into the high-spin (HS) state. Furthermore, by controlling the proportion of the Z isomer through variation of irradiation time, we achieve continuous and quantitative modulation of the HS fraction. This work provides the first direct structural evidence of guest-driven light-induced spin change (GD-LISC), establishing a robust strategy for designing photoswitchable materials.
Cobalt Nanoparticles Confined in Defective Carbon Matrices for Robust Intermittent CO Methanation.
Qin J, Yin S, Yu C … +12 more , Tao Y, Mu J, Wang M, Luo J, Zhang L, Zhou Y, Yan Z, Zhang L, Dai Y, Wu W, Li H, Zeng J
Angew Chem Int Ed Engl · 2026 Jul · PMID 42391212 · Publisher ↗
The development of robust catalysts for CO methanation under intermittent operating conditions is key to harnessing renewable energy sources such as wind and solar. However, this pursuit faces two major obstacles. The he...
The development of robust catalysts for CO methanation under intermittent operating conditions is key to harnessing renewable energy sources such as wind and solar. However, this pursuit faces two major obstacles. The heating-cooling cycles induce prolonged thermal stress, resulting in catalyst deactivation. Moreover, the temperature-sensitive selectivity hampers the ability to maintain high methane yield, leading to undesired by-products. Herein, we report cobalt nanoparticles confined within carbon matrices, which achieved 82.3% CO conversion and > 99% CH selectivity over multiple heating-cooling cycles toward intermittent CO methanation. The catalyst robustness arises from the low coefficient of thermal expansion and high thermal conductivity of the carbon matrix, which effectively mitigates thermal stress during temperature fluctuations. Mechanistic studies confirm that the reaction proceeds via a formate pathway, which contributes to the high CH selectivity across a wide temperature range. These insights provide a design framework for developing robust catalysts, advancing CO methanation performance, and the efficient use of fluctuating renewable energy sources.
Copper(II/III) Redox Couple Enables C─H Methylation via a Radical Mechanism Analogous to SAM Enzymes.
Doss EN, Moore CE, Zhang S
Angew Chem Int Ed Engl · 2026 Jul · PMID 42391196 · Publisher ↗
Biological methylation is a fundamental regulatory process in gene expression, biomolecule modification, and cell repair. Many enzymatic C-H methylation reactions proceed through sequential one-electron steps mediated by...
Biological methylation is a fundamental regulatory process in gene expression, biomolecule modification, and cell repair. Many enzymatic C-H methylation reactions proceed through sequential one-electron steps mediated by distinct redox cofactors, such as FeS clusters and methylcobalamin. However, structurally faithful model complexes of these cofactors have thus far been unable to replicate the characteristic C-H methylation reactivity. Herein, we report the first isolable copper(II/III)-methyl complexes that undergo C─H methylation via a radical mechanism analogous to SAM enzymes. The copper(II)-methyl complex undergoes reversible one-electron oxidation to a formal copper(III)-methyl species, which serves as a methyl radical reservoir capable of both generating and capturing carbon radicals. The Cu-CH complex mediates C-H methylation through hydrogen atom transfer (HAT) and methyl radical transfer, affording methylated products from substrates similar to those targeted by radical SAM methyltransferases. By merging the characteristic HAT and radical rebound reactivity within a single organometallic center, this copper(II/III)-methyl species provides a synthetic platform that mirrors key mechanistic features of enzymatic C-H methylation.
Ring Strain Engineering of Cyclic Ethers for High-Performance Sodium Metal Batteries.
Niu Y, Meng F, Li S … +10 more , Lu D, Zhu Y, Fu C, Wang H, Wang L, Long Y, Zhang G, Sun Z, Wu G, Chen W
Angew Chem Int Ed Engl · 2026 Jul · PMID 42391191 · Publisher ↗
1,3-dioxolane is a promising solvent for low-temperature batteries owing to its low freezing point and low viscosity. However, its tendency toward ring-opening polymerization leads to reduced ionic conductivity and deter...
1,3-dioxolane is a promising solvent for low-temperature batteries owing to its low freezing point and low viscosity. However, its tendency toward ring-opening polymerization leads to reduced ionic conductivity and deteriorated electrochemical stability. Here, we establish an electronic-geometric coupling design principle to regulate solvent stability in weak-weak electrolyte systems for sodium metal batteries. A dual-descriptor framework combining ring strain energy (RSE) and a sterically corrected electrostatic descriptor, defined by the lowest negative electrostatic potential normalized by molecular volume (ESP/Volume), is introduced to guide cyclic ether solvent design. Following this principle, 2,4-dimethyl-1,3-dioxolane is identified with reduced RSE and moderate ESP/Volume, enabling enhanced resistance to polymerization and improved Na-compatibility/ion transport. Molecular dynamics simulations and density functional theory calculations reveal that, the electrolyte forms an aggregate-dominated solvation structure with a high lowest unoccupied molecular orbital level, promoting the formation of a thin, uniform, and inorganic-rich solid electrolyte interphase. Consequently, the electrolyte delivers accelerated interfacial kinetics and stable operation across a wide temperature range. Na||Na symmetric cells cycle stably for 1800 h at room temperature, while Na||NaV(PO) full cells with high cathode loading (20 mg cm) operate for over 200 cycles at 25 °C and more than 900 cycles at -40° C.
Bond Length as a Unified Descriptor for Stable Iodine Battery.
Geng M, Wang Y, Zeng F … +7 more , Liu Y, Ni H, Hong B, Xia W, Han S, Zhao Y, Zhang B
Angew Chem Int Ed Engl · 2026 Jul · PMID 42391189 · Publisher ↗
Dissolution of active materials in the electrolyte and their subsequent shuttling are common challenges for realizing stable electrodes in rechargeable batteries. These issues become particularly pronounced in cathodes w...
Dissolution of active materials in the electrolyte and their subsequent shuttling are common challenges for realizing stable electrodes in rechargeable batteries. These issues become particularly pronounced in cathodes with high solubility, including high-energy iodine electrodes. The interaction strength of iodine with the host electrode and electrolyte is critical for determining electrochemical stability, yet there is a lack of an appropriate parameter to quantify it. Our findings reveal that, as a weak Lewis acid, iodine's interaction strength is highly influenced by the nucleophilicity of surrounding ligands. We propose the I-I bond length, which can be conveniently probed through Raman tests, as a unified descriptor to predict the iodine electrode stability. The asset of this descriptor is demonstrated in (i) rational design of complex electrodes to enhance the binding strength between iodine and host and (ii) efficient screening of electrolyte solvents to minimize the shuttle. The collective effects enable stable cycling of Li-I batteries under the challenging current rate of 0.1 C for over 4000 h. Overall, the unified descriptor provides a powerful means to expedite electrode and electrolyte design for overcoming active material dissolution challenges.
Electron-Switching Astaxanthin Enables Programmable Triple-Phase Interface Chemistry for High-Loading All-Solid-State Lithium-Sulfur Batteries.
Chen Z, Liu H, Yan Y … +7 more , Mei Y, Zhang B, Xiao K, Cai D, Chen C, Yang S, Yang Z
Angew Chem Int Ed Engl · 2026 Jul · PMID 42391116 · Publisher ↗
All-solid-state lithium-sulfur batteries (ASSLSBs) promise high energy density and intrinsic safety, yet their performance is fundamentally constrained by unstable triple-phase interfaces among sulfur, conductive carbon,...
All-solid-state lithium-sulfur batteries (ASSLSBs) promise high energy density and intrinsic safety, yet their performance is fundamentally constrained by unstable triple-phase interfaces among sulfur, conductive carbon, and solid electrolytes. Such instability leads to sluggish solid-solid sulfur redox kinetics, hindered charge transport, and severe chemo-mechanical degradation. Herein, we demonstrate a biomolecular strategy using astaxanthin (AXT) as an electron-switching interfacial regulator to simultaneously address these coupled challenges. Combined experimental and theoretical analysis reveal that AXT modulates electrolyte decomposition pathways in a coverage-dependent manner via a localized "electron pocket" effect, favoring the formation of electrochemically active LiS over insulating LiCl. Meanwhile, polar oxygen functional groups in AXT establish low-potential corridors that facilitate Li transport and stabilize key intermediates, thereby accelerating sulfur redox kinetics. In addition, the chain-like molecular architecture of AXT acts as a flexible scaffold to buffer volume fluctuations and preserve interfacial contact integrity during cycling. Consequently, AXT-modified ASSLSBs achieve exceptional electrochemical performance under high sulfur loading conditions, delivering an areal capacity of 16.56 mAh cm at 9.49 mg cm sulfur loading. This work establishes a biomolecule-driven electronic engineering paradigm for programmable interface chemistry, offering a general strategy toward high-energy-density and durable solid-state batteries.
Highly Dissymmetric and Multicolor Circularly Polarized Organic Hyperafterglow.
Li H, Xu F, Song Z … +11 more , Zhao F, Guo S, Tan C, Liu J, Li J, Zhang H, Li H, Xie G, Tao Y, Li B, Huang W
Angew Chem Int Ed Engl · 2026 Jul · PMID 42391035 · Publisher ↗
Circularly polarized organic afterglow (CPOA) materials have garnered considerable interest for their potential in information encryption, 3D displays, and sensing technologies. However, realizing CPOA materials that sim...
Circularly polarized organic afterglow (CPOA) materials have garnered considerable interest for their potential in information encryption, 3D displays, and sensing technologies. However, realizing CPOA materials that simultaneously offer high efficiency, long lifetime, high color purity, and large dissymmetry factor (g) remains a significant challenge. Herein, an effective CP-hyperafterglow design strategy that rationally integrates narrowband hyperafterglow polymers with cholesteric liquid crystal matrices is proposed. The resulting polymeric films deliver multicolor narrowband CP-hyperafterglow emission with high photoluminescence quantum yields of up to 81%, emission bandwidths as narrow as ∼40 nm, ultralong lifetimes reaching 957 s, and maximum |g| values of up to 1.3. Benefiting from these photophysical merits, various applications, including information encoding, multilevel encryption, and chiral display, are demonstrated. These findings offer a simple and reliable route toward high-performance CP-hyperafterglow, advancing the development of chiral optoelectronic materials and applications.
Proton Transfer Shuttle Mediated Dormant-Active Balance for Accelerated and Controlled Polymerization of N-Carboxyanhydrides.
Huang J, Sheng H, Cheng J … +1 more , Liu X
Angew Chem Int Ed Engl · 2026 Jul · PMID 42390905 · Publisher ↗
Since its inception in 2003, the concept of "reversible deactivation" to control chain propagation has emerged as a promising, though still evolving, strategy for precise polypeptide synthesis. Beyond a simple polymeriza...
Since its inception in 2003, the concept of "reversible deactivation" to control chain propagation has emerged as a promising, though still evolving, strategy for precise polypeptide synthesis. Beyond a simple polymerization method, this concept is expected to promote unique reaction pathways. Nevertheless, achieving both rapid and well-controlled ring-opening polymerization of N-carboxyanhydrides through the equilibrium between dormant and active species is rare and challenging. In this study, we report a proton transfer shuttle-assisted strategy that accelerates chain growth via trifluoroacetic acid (TFA) /tetrabutylammonium acetate (TBAA) cooperative system. Central to this strategy is reversible acceptance and donation of proton, thereby shifting the dormant-active equilibrium without disrupting it. This modulation increases the proportion of active chain ends while maintaining control over rapid polymerization process. Moreover, cooperative TFA/TBAA catalysis has streamlined the synthesis of well-defined polypeptides, which are amenable to further chemical modifications. Control experiments and density functional theory calculations provide insights into the origin of controllability and critical role of TFA/TBAA in regulating the reversible deactivation equilibrium. Consequently, this work establishes a robust and efficient approach for accelerated yet controlled preparation of polypeptides and generates fundamental insights that advance understanding and application of the "reversible deactivation" concept for precision polypeptide synthesis.
Chloride-Regulated Depolymerization of Aluminosilicate Networks for Fast Ion Transport Compliant Interfaces in Sustainable All-Solid-State Sodium Batteries.
Zhou L, Wang X, Yang R … +19 more , Xu Y, Zhang S, Li M, Wu H, Wang X, Yue J, Wang Y, Jin H, Zhu X, Zhang M, Li C, Yang X, Yuan X, Yin W, Xia W, Zhao C, Liang J, Sun X, Li X
Angew Chem Int Ed Engl · 2026 Jul · PMID 42390888 · Publisher ↗
All-solid-state sodium-ion batteries (ASSSIBs) provide a sustainable and cost-effective solution for large-scale energy storage. Sodium aluminosilicate (NASO) represents a resource-sustainable electrolyte option owing to...
All-solid-state sodium-ion batteries (ASSSIBs) provide a sustainable and cost-effective solution for large-scale energy storage. Sodium aluminosilicate (NASO) represents a resource-sustainable electrolyte option owing to their low cost, natural abundance, and electrochemical stability. However, their strong covalent network leads to intrinsic low ionic conductivity, and poor interfacial compatibility. This work employs Cl incorporation to depolymerize the hyperconnected covalent network of NASO, forming a modified NaAlSiOCl (NASOC) structure with discrete short-chain segments, which turns stress-induced large-scale cooperative rearrangement into localized deformation. Replacing a strong O─bridge with a weaker Cl─bridge further reduces the Young's modulus. Additionally, chloride doping effectively reduces the Na migration barrier by decreasing both the elastic deformation energy and the chemical binding energy. Consequently, this Cl-mediated depolymerization approach simultaneously reduces stiffness and improves ionic conductivity. The optimized NASOC electrolyte exhibits a low Young's modulus of ∼5 GPa and a high Na conductivity of 0.45 mS cm, which together facilitate superior ion transport and intimate electrode contact. The ASSSIBs employing NASOC retain 80.9% of their capacity after 500 cycles at 0.1 C. This work demonstrates a Cl-mediated depolymerization strategy that concurrently enhances ionic conductivity and mechanical compliance in solid electrolytes, providing key insights for designing high-performance and sustainable energy storage materials.
Asymmetric Zn─NO-Coordinated Hydrogen-Bonded Organic Frameworks for Electrochemical Hydrogen Peroxide Production and Wastewater Purification.
Liu Y, Yang W, Meng S … +4 more , Zhao S, Zhan S, Sun Y, Li Y
Angew Chem Int Ed Engl · 2026 Jul · PMID 42390881 · Publisher ↗
Hydrogen-bonded organic frameworks (HOF) demonstrate significant potential in the electrocatalytic synthesis of hydrogen peroxide. However, their practical application is severely hindered by the uncontrollable structura...
Hydrogen-bonded organic frameworks (HOF) demonstrate significant potential in the electrocatalytic synthesis of hydrogen peroxide. However, their practical application is severely hindered by the uncontrollable structural evolution of their skeletons during material synthesis which poses a challenge for constructing well-defined active sites. In this study, Zn was incorporated into the HOF to fabricate Zn-functionalized HOF (Zn-HOF) with asymmetric Zn─NO coordination configuration. Theoretical calculations and screening reveal that compared with common transition metal (Mn, Fe, Co, Ni, and Cu) systems, this asymmetric Zn─NO coordination effectively regulates the electronic structure, achieving optimal adsorption on the *OOH intermediate for the 2-electron oxygen reduction reaction. Experiments confirm the Zn-HOF catalyst achieves 96% maximum HO selectivity, enabling efficient HO production in unpurified tap or natural lake water with 89% Faradaic efficiency. Moreover, Zn-HOF can degrade various antibiotic pollutants, the Zn-HOF-loaded sandwich reactor exhibits only 0.87 kWh·m energy consumption, with its single-electrode cost merely 1/32 that of platinum-coated electrodes. Our work provides a viable pathway for the application of HOF-based materials in environmental remediation.
Photocatalytic Cascade Nitrogen Fixation for Selective Purification of Methane-Rich Coal-Bed Gas Over a Bimetallic MOF.
Li J, Zhang W, Wu Z … +5 more , Xue W, Guo X, Huang H, Pang J, Zhong C
Angew Chem Int Ed Engl · 2026 Jul · PMID 42390844 · Publisher ↗
CH-rich coal-bed methane (CBM) is often contaminated with N, but their similar properties make conventional separation energy-intensive and inefficient. Herein, we report a photocatalytic strategy for selective N convers...
CH-rich coal-bed methane (CBM) is often contaminated with N, but their similar properties make conventional separation energy-intensive and inefficient. Herein, we report a photocatalytic strategy for selective N conversion over CH, achieving simultaneous CBM purification and nitrogen valorization. A Co-Ni metal-organic framework (CoNi-PYZ) features isolated bimetallic sites, where ligand/Co units donate electrons to Ni, establishing spatially separated reduction and oxidation centers. This structural motif drives a photocatalytic cascade nitrogen fixation that N is first reduced to NH at the Ni sites; subsequently, the generated NH outcompetes CH for the Co sites, leading to its oxidation to NO . This remarkable selectivity is governed by the high polarity and lone-pair electron donation of NH, favoring its adsorption over nonpolar CH. Notably, the optimal catalyst achieves high activity under mild conditions without sacrificial agents, delivering NH and NO production rates of 599.8 and 199.8 µmol g h , respectively. Mechanism analysis reveals that ligand engineering optimizes the d-band center to balance adsorption and desorption, thereby minimizing the rate-determining step barriers for both half-reactions, consistent with the Sabatier principle. This work provides a reaction-driven alternative to traditional phase-separation, establishing a novel paradigm for CBM upgrading coupled with selective N transformation.
Scalable Art-Inspired Tessellated Covalent Organic Framework Membranes Enable Highly Selective Ion Separation.
Zhao Z, Guo R, Yang T … +4 more , Wang Z, Tong T, Du Y, Zhao S
Angew Chem Int Ed Engl · 2026 Jul · PMID 42390840 · Publisher ↗
Covalent organic frameworks (COFs), distinguished by their periodic and tunable network structures, exhibit great potential for molecular and ionic separation. Nevertheless, fabricating COF membranes with angstrom-scale...
Covalent organic frameworks (COFs), distinguished by their periodic and tunable network structures, exhibit great potential for molecular and ionic separation. Nevertheless, fabricating COF membranes with angstrom-scale pores faces challenges in precisely controlling channel dimensions and achieving seamless integration of frameworks. Here, we report the synthesis of a substoichiometric aminal-linked COF with a pore size of ∼5 Å and develop a covalent tessellation strategy inspired by Escher's art and derived from interfacial polymerization, that successfully fabricates defect-free tessellated COF (tCOF) membranes. The resulting tCOF membrane exhibits ultra-microporous structures, achieving high water permeance of 10.2 L m h bar, nearly perfect NaSO rejection of 99.4%, and exceptional Cl/SO selectivity of 1,090. The tCOF membranes can be continuously scaled up to roll-to-roll format with a width of 30 cm and an unlimited length. The potential applications in resource recovery are proved with a two-stage nanofiltration process, which produces NaCl with a high purity of >99% from NaCl/NaSO mixtures. Therefore, the innovative covalent tessellation methodology reported in this work provides a new avenue for the development of scalable COF membranes with angstrom-scale pores for highly selective separation.
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