We develop a single-molecule fluorescence imaging method based on DNA origami frameworks to quantify electric field effects on DNA conformation and hybridization properties at the single-molecule level. The regulation patterns of applied potential and scanning duration on the activity of DNA probes are determined and electric field-induced structural relaxation in DNA frameworks is revealed.

Self-assembled DNA nanostructures have been popularly used to develop DNA-based electrochemical sensors by exploiting the nanoscale positioning capability of DNA origami. However, the impact of the electric field on the structural stability of the DNA origami framework and the activity of carried DNA probes remains to be explored. Herein, we employ DNA origami as structural frameworks for reversible DNA hybridization, and develop a single-molecule fluorescence imaging method to quantify electric field effects on DNA conformation and hybridization properties at the single-molecule level. Through single-molecule temporal kinetic analysis of hybridization events occurring on individual DNA origami, we systematically determine the regulation patterns of applied potential and scanning duration on the activity of DNA probes. Optical super-resolution reconstruction of probe sites reveals electric field-induced structural relaxation in DNA frameworks. This approach not only provides insights into electrochemical DNA sensing devices, but also lays the foundation for developing hybrid electrical–optical analysis at the single-molecule level.

A novel inorganic lacunary-structure metal-oxo framework, BSiW9, serves as ETL of p-i-n OSCs, resulting in not only a remarkable PCE but also outstanding long-term stability.

Organic solar cells (OSCs) with p-i-n architecture usually exhibit decent efficiency due to the easily tunable energy levels of organic interfacial layers (ILs). However, their operational lifetime is limited by the morphological instability of organic ILs especially the electron-transporting layer (ETL) that shows strong self-aggregation tendency. Besides, organic ETLs are confronted with significant challenges including large batch-to-batch variations and high costs. Herein, we develop an inorganic lacunary-structure metal-oxo framework as ETL of p-i-n OSCs. The resultant molecule, BSiW9, not only shows ultralow cost but also leads to significantly enhanced electron extraction in OSCs. Moreover, the redox activity of BSiW9 allows reinforced electrical conductivity by using a hydroquinone-derivative dopant, HQ. The doping strategy finally results in a remarkable PCE of 20.5% in p-i-n OSC, largely outperforming that using organic ETLs. Meanwhile, an outstanding long-term stability is obtained in this champion device, with 92% of original efficiency maintained after a maximum-power-point tracking for 1250 h, among the longest lifetimes of p-i-n OSCs. This work demonstrates the effectiveness of utilizing rationally tailored low-cost metal-oxo framework as ILs for more industrially compatible OSCs.

A dual-stimulus programmed coacervate transformation system is developed. The sequential application of pH and salt concentration induces transition of membrane-less coacervates into nested multiphase coacervates and, ultimately, into vesicular-like multiphase coacervates. This transition endows selective client recruitment and exclusion by resultant coacervates, and facilitates the spatial orchestration of enzymatic reactions.

Stimuli-responsive (multiphase) coacervates deserve significant attention as cell-like entities that can adapt to their environment and undergo morphological reconfiguration. In this study, a tandem-triggered transition system is presented that enables the transformation of single-phase coacervates into multiphase structures through the sequential application of two external stimuli: pH and salt concentration. A polyanion containing acid-labile amide bond is incorporated into the membrane-less coacervates. Upon exposure to an acidic pH, hydrolysis of the amide bond induces charge reversal from polyanion to polycation, triggering the first transition from single-phase to nested multiphase coacervates. This transformation alters the spatial redistribution and viscosity of coacervate components and influences sequestration behavior toward various (macro) molecules. Subsequently, the introduction of hypertonic environment as secondary stimulus induces selective dissociation and structural reconfiguration of nested multiphase coacervates into vesicular-like multiphase coacervates, further altering the coacervate components' fluidity and partitioning properties. Notably, the diverse inherent properties of coacervates among this tandem-triggered transition enables the variation of spatial organization for enzymatic reactions. Overall, the findings demonstrate a strategy for the sequential control of coacervate structural reconfiguration through dual stimuli, providing a versatile platform for the development of programable and adaptive coacervate-based protocells.

This study identifies lithium naphthalene as a lithiation agent for the large-scale preparation of disordered rock-salt Li3V2O5, investigates the impact of chemical lithiation on electrochemical behavior, and decouples lattice distortion modes using DFT calculations. A one-step synthesis method produces materials with an elongated a-axis, enhancing rate capability and providing a solid theoretical basis for industrialization.

Disordered rock-salt Li3V2O5 (DRX-LVO) anode exhibits distinctive 3D Li+ percolation transport networks, which offers the unique advantage for ultra-charging. However, the existing chemical lithiation preparation routes not only pose safety risks due to the use of highly reactive reagents but also inevitably result in products with poor crystallinity. Investigating the origin, impact, and strategies for crystallinity degradation is pivotal for advancing the industrialization of chemical lithiation. To address the safety issue, different lithiation reagents were evaluated from the perspective of lone electron activity, and lithium naphthalene was identified as an ideal reagent balancing safety and efficiency. Through DFT calculations, the mechanism underlying different types of distortions in the DRX system was decoupled while the distinct effects of a/b/c-axis variations on migration energy barriers were elucidated. Guided by theoretical insights, the a-axis was nominated as the critical parameter for enhancing electrochemical performance, leading to the development of Li3V2O5 with elongated a-axis dimensions that exhibit significantly improved rate capabilities (80 mAh g−1 at 20 A g−1). This study elucidates the distortion mechanisms via exploring the correlation among chemical lithiation feasibility, lattice tuning and kernel parameter confirmation, as well as fast-charging behavior, shedding light on precise crystallographic design on high-performance fast-charging anode.

Boron-introducing electronically reconfigures the inert Zn2+ 3d10 center into active Zn-NxB4₋x sites (Zn-NBC), endowing the catalyst with a 26-fold boost in Fenton-like pollutant degradation by strengthening PDS adsorption and promoting ·O2 − and 1O2 generation.

Despite growing interest in single-atom catalysts (SACs) for Fenton-like reactions, zinc (Zn)-based SACs remain unexplored due to the inherent inertness of Zn2+, whose fully occupied 3d10 electronic configuration limits redox activity. Here, we overcome this limitation by introducing boron (B) atoms to reconfigure the electronic structure of Zn-N4 coordination sites, yielding an activated catalyst denoted as Zn-NBC. This electronic modulation transforms inert Zn-N4 sites into catalytically active centers (Zn-N x B4- x ), enabling significantly enhanced Fenton-like activity. Compared to the unmodified Zn-N4 catalyst (Zn-N4C), Zn-NBC exhibits a 26-fold increase in the rate of organic pollutant degradation. Density functional theory (DFT) calculations and experimental results reveal that Zn-N4C and Zn-NBC exhibit distinct PDS adsorption behaviors, with B incorporation tuning both adsorption strength and electronic interactions at the Zn center. Crystal orbital Hamilton population (COHP) analysis further demonstrates that the Zn-NBC facilitates the activation of the S─O bonds in peroxydisulfate (PDS), promoting the generation of reactive oxygen species, including peroxide radicals and singlet oxygen. These findings establish a new paradigm for activating electronically inert metal centers and position Zn-NBC as a promising platform for efficient and sustainable environmental remediation.

STING agonists offer enormous prospects in cancer immunotherapy. Nonetheless, controllable delivery of STING agonists remains elusive. Here, we report sono-enzyme dual-triggered polymeric nanoplatform for precision delivery of STING agonist MSA-2 and sonosensitizers. This paradigm demonstrates superior competence in augmenting antigen-specific immunity, which combines with sonodynamic therapy, yielding remarkable therapeutic outcomes and well-tolerated safety in a murine preclinical tumor model.

The stimulator of interferon genes (STING) pathway is a central target in cancer immunotherapy, but current STING agonist therapies lack precision control, leading to suboptimal therapeutic outcomes and systematic adverse effects. Herein, we engineered a dual-locked immuno-polymeric nanoplatform (IPN) with precise spatiotemporal control over the release of STING agonists to enhance cancer immunotherapy. This platform, constructed from biocompatible poly(β-amino esters) (PBAE), incorporates the STING agonist (MSA-2) covalently linked via ester bonds, which is co-assembled with a sonosensitizer. Upon activation by ultrasound and natural esterase enzyme, IPN significantly enhances the localized release of MSA-2 within the tumor. Alongside, this platform augments the generation of toxic radicals, leading to the spread of tumor antigens and immunogenic biomolecules, subsequently initiating a high magnitude of antigen-specific T cells for tumor eradication. The multifaceted advantages of ultrasound and enzymes synergistically enhance the physical contact and spatial organization of immune-related reactants as well as chemical bioprocesses. This dual-locked IPN platform demonstrates an eight fold greater tumor inhibition compared to single-locked counterparts and a four fold enhancement over the summation effect, highlighting a safer and more effective paradigm for cancer immunotherapy.

Catalyst-free C─N radical coupling reaction in a single-molecule junction is demonstrated. After the molecule is excited by ultraviolet irradiation, the oriented external electric field synergistically facilitates the transfer of hydrogen atoms and triggers the radical coupling reaction by lowering the energy barrier.

Radical coupling reactions have been widely used in the synthesis of complex organic molecules, materials science, and drug research. However, restricted conditions or special catalysts are required to overcome the energy barrier and trigger the coupling reaction efficiently. In this study, we provide experimental evidence that the C─N radical coupling reactions can be significantly accelerated by an oriented external electric field (OEEF) under synchronous UV irradiation without a catalyst. By repeatedly forming thousands of single-molecular junctions with reactant molecules in nonpolar solvents under a bias voltage, a new conductance plateau was observed upon UV irradiation, which was completely absent in polar solvents owing to the electrical shielding effect. This finding indicates that the radicals generated under light irradiation can timely participate in the coupling reaction under the in situ action of OEEF, leading to the high-efficiency generation of the C─N radical coupling product, which was confirmed by the measured electron paramagnetic spectrum and high-resolution mass spectrometry. With the assistance of theoretical calculations, the underlying mechanism was further revealed, i.e., OEEF can significantly decrease the reaction barrier and facilitate the intermolecular hydrogen atom transfer (HAT). This study provides a catalyst-free paradigm for high-efficiency radical reactions.

By engineering the ANF-mediated thermal reconstruction, we achieved the deep modification of MXene with synergistic noncovalent/covalent interaction toward an optimal reaction interface, which breaks the trade-off between the reactivity and stability for energetic pseudocapacitive storage chemistry. The unique synergistic interface effects trigger a high specific capacitance of 531.9 F g−1 and a capacity retention of 92.2% after 180, 000 cycles.

MXenes serve as pivotal candidates for pseudocapacitive energy storage owing to sound proton/electron-transport capability and tunable topology. However, the metastable surface terminal properties and the progressive oxidation leads to drastic capacity fading, posing significant challenges for sustainable energy applications. Here, with the aramid nanofiber as the interface mediator, we engineer the thermal reconstruction of MXenes to synergistically introduce interfacial covalent and noncovalent interactions, resulting in a high specific capacitance of 531.9 F g−1 and a capacity retention of 92.2% after 180, 000 cycles. In-situ heating transmission electron microscopy observations demonstrate the formation of ultrafine mesopores with interfacial reconstitution for mass transport intensification. Theoretical calculations indicate electronic accumulation adjacent to the covalent bonds, endowing the heterogeneous interface with fast electronic conduction capability and favorable adsorption of H+. In addition, the dual modification improves the oxidation energy barrier of MXenes to TiO2, resulting in a thermodynamically promoted and sustainable storage microenvironment. Our research emphasizes the synergistic mechanism of noncovalent interactions and covalent bonding toward an optimal reaction interface, which breaks the trade-off of MXenes between the reactivity and stability for energetic energy storage.

What makes aromatic ligands selective for CO2 over CH4? Broadband rotational spectroscopy reveals how 1,2,3-trifluorobenzene forms stronger F⋯C tetrel and π–π interactions with CO2, versus weaker CH⋯F hydrogen bonds with CH4, along with intriguing tunneling motions. These molecular-level insights could benefit the design of ligands for selective gas adsorption in MOFs and related materials.

The cluster growth behavior of CO2 and CH4 on an aromatic ligand has been studied through the unambiguous identification of complex structures of 1,2,3-trifluorobenzene-(CO2)1–4 and -ß(CH4)1–2 using broadband rotational spectroscopy in conjunction with extensive theoretical calculations. The results reveal a contrast in the thermodynamically favorable ligand-gas binding sites and noncovalent interactions of the two gaseous molecules on the ligand. The observation of a tunneling splitting and large centrifugal distortions indicates that CH4 molecules bind to the fluorinated π system via three weak hydrogen bonds without CH4 self-interactions, resulting in an effective structure displaced toward the dissociation limit. Conversely, CO2 shows diverse and stronger intermolecular interactions with the fluorinated benzene, including F─C tetrel bonding, lone pair to π-hole interactions, π–π stacking, and a significant contribution from CO2 self-interactions. The thorough examination of ligand–gas interactions and aggregation patterns highlights the significant capacity and selectivity of the fluorinated aromatic ligand for accepting CO2 over CH4.

Self-assembled thiol-rich polypseudorotaxanes with high modularity were developed via a “one-pot” preparation through the threading of thiolated α-cyclodextrins on polymers and subsequent oxidation of thiols into disulfide bonds. This dynamic motif was used as a functionalization platform for thiophilic metal nanoparticles, either tethering them to a photothermal hydrogel or for their surface functionalization with nanoscopic “wrapping”.

As supramolecular assemblies, polypseudorotaxanes (PPR) exhibit inherent advantages in modular adaptability and structural programmability, with the potential to build tuneable platforms integrating various functionalities. Here we report the “one-pot” preparation of a self-assembled thiol-rich PPR (SPPR), where thiolated-α-cyclodextrins (SHαCD) spontaneously thread onto polymers, and are then crosslinked into a three-dimensional network by the thermally-triggered oxidation of thiols into disulfide bonds. The dynamic thiol groups along the SPPR provide remarkable modularity for the functionalization of thiophilic metal nanoparticles (NPs), exemplified by two application vectors. First, SPPR were used as building blocks of a thermo-responsive hydrogel to incorporate thiophilic NPs, where NPs are tethered to the networks and, in turn, reinforce its mechanical properties. The resulting gels, characterized by small-angle neutron-scattering and rheology, display photo-responsive gelation and thixotropy. In the second application, the affinity of metal NPs to the dynamic thiol groups on SPPR was exploited to “wrap” the polymers around the NPs, through simple tuning of concentration and chain length. The flexible polydisulfides layer endows NPs with enhanced cancer cytotoxicity, possibly via the thiol-mediated uptake pathway. These results establish SPPR as a powerful functionalization platform, offering a promising route toward customized supramolecular materials.

LL-37 and its truncates modulate Aβ40 primary nucleation by forming hetero-oligomers, nanoclusters, and microclusters, which act as off-pathway aggregates inhibiting fibrillation. These transient assemblies influence fibril progression and cytotoxicity, highlighting the dynamic interplay between aggregation and toxicity. Integrating nanoscale and microscale perspectives provides mechanistic insight into Aβ40–LL-37 interactions and informs therapeutic strategies for Alzheimer's disease.

LL-37 and its variants with amphiphilic structure can modulate amyloid-β (Aβ) fibril formation, but the detailed mechanism behind it is still unclear. By using four different peptides (LL-37, LL-379–32, LL-3718–29, LL-3719–28), we found these peptides affect Aβ40 aggregation differently. Nanoscale analysis showed that all LL-37 peptides form hetero-oligomers and nanoclusters with Aβ40, but LL-37 and LL-3719–28, which exhibit the strongest inhibition of Aβ fibrillation, form more hetero-oligomers and smaller nanoclusters. This suggests that hetero-oligomers and small nanoclusters may represent an off-pathway, preventing the formation of productive aggregates. At the microscale, all LL-37 peptides were found to promote Aβ cluster formation, but LL-37 and LL-3719–28 can form larger clusters with Aβ rapidly, emphasizing that smaller nanoclusters can assemble to macroscale clusters easier, inducing more toxic aggregates. Both nanoscopic and microscopic mechanisms revealed inhibition of Aβ fibrillation by all LL-37 peptides, impacting Aβ primary and secondary nucleation, while only LL-37 and LL-3719–28 affected Aβ elongation. Our findings highlight the role of LL-37 and its synthetic fragments in Aβ40 aggregation across different scales, particularly focusing on cluster formation at the nanoscale and microscale to fill the knowledge gap between oligomerization and fibrillation.

A novel lithium-mediated electrodeposition process (Pd0→Li2Pd→Li2PdO2) overcomes the challenge of palladium dissolution in dilute hydrochloric acid and enables efficient recovery. High-purity palladium deposits with a low lattice strain were obtained by regulating the voltage and concentration.

To address palladium supply–demand challenges and conventional recovery inefficiencies, this study develops a lithium-mediated electrodeposition process for efficient palladium recycling from spent catalysts. Density functional theory calculations identified a controlled Pd0→Li2Pd (Pd δ− )→Li2PdO2 (Pd2+) transformation pathway, and experimental verification confirmed that Li2Pd precursors underwent oxidative transformation into Li2PdO2 with structural inheritance. Li2PdO2 exhibited Pd2+–O2− coordination and underwent rapid dissolution in dilute hydrochloric acid. Pd2+ exhibits a quasi-reversible redox process, thereby eliminating multivalent-state-induced efficiency losses. Field simulations demonstrated that the anisotropic current distribution in the 2D electrode plane drove the edge effects, which directly controlled the annular palladium deposition at the base. Electrodeposition produced a phase-pure palladium deposit with high (111)-textured crystallinity and ultralow lattice strain. Elevated voltages enhanced the nucleation density, inducing a morphological transition from dendritic to compact clusters, while the amplified edge effects promoted the formation of mossy structures. Elevated Pd2+ concentrations triggered mass-transfer-driven competitive growth, resulting in the transition of palladium deposits from uniform grains to particles with graded size distributions. This work addresses the critical challenge of inefficient palladium dissolution using a phase-engineering strategy and establishes an integrated dissolution-electrodeposition framework that enables the high-efficiency recovery of secondary palladium resources.

A nucleophilic ubiquitin-based probe, Biotin-Ub74-DYn-2, was developed to selectively label sulfenylated deubiquitinases (DUB-SOH). The probe demonstrated high specificity in vitro and enabled the identification of 13 oxidized DUBs in H2O2-treated 293T cell lysates via label-free proteomics, offering a new approach to study redox-regulated DUB activity.

Activity-based ubiquitin probes (Ub-ABPs) are powerful tools for studying the functional landscape of deubiquitinases (DUBs). While most existing Ub probes have focused on examining the native state of DUBs, oxidative stress, especially in cancer and inflammatory contexts, can oxidize the catalytic cysteine of DUBs, significantly altering their activity. Here, we developed three novel ubiquitin-based activity probes (Ub-ABPs) to selectively trap the sulfenylated form of deubiquitinases (DUB-SOH). These probes employ ubiquitin as the recognition element and incorporate distinct warheads: an electrophilic norbornene moiety (Biotin-Ub-NMA) or dimedone-derived cyclic C-nucleophiles (Biotin-Ub-PRD and Biotin-Ub75-DYn-2), enabling covalent capture of oxidized cysteine residues. Of these, Biotin-Ub-PRD and Biotin-Ub75-DYn-2 successfully labeled DUB-SOH, highlighting the importance of proper probe-substrate interaction for effective trapping. Optimization of the ubiquitin length showed that the Ub74 variant displayed enhanced affinity toward DUB-SOH. Biotin-Ub74-DYn-2 enabled enrichment and identification of DUB-SOH targets via immunocapture and label-free quantitative proteomics. Collectively, these sulfenic acid-targeting Ub-ABPs represent versatile tools for elucidating redox-dependent DUB regulation, with potential applications in understanding redox dysregulation in disease contexts.

A rigid tetrazine-based porous organic cage with record SF6 uptake is post-synthetically tuned via iEDDA chemistry to enhance stability, and further polymerized into networked materials with tunable porosity for selective CO2/N2 separation.

Porous organic cages (POCs) have emerged as promising porous materials for a wide range of applications. However, their development is often limited by insufficient chemical stability and challenges in systematically functionalization. Herein, we reported the design and synthesis of a tetrazine-based POC (TC1) featuring rigid tetrahedral structure, prepared via a one-pot nucleophilic aromatic substitution reaction. TC1 exhibits high porosity, with a BET surface area at 1157 m2 g−1, and good chemically stability, surpassing most POCs formed through dynamic covalent chemistry. Its well-defined, electron-deficient cage cavity enable efficient SF6/N2 separation, showing the highest SF6 adsorption capacity and selectivity among all reported porous molecular materials to data, as confirmed by dynamic breakthrough experiments. Post-synthetic modification of TC1 via inverse electron-demand Diels-Alder (iEDDA) reactions yielded two functionalized cages (TC2 and TC3), which maintain good porosity and display further enhanced chemical stability over a broad pH range (-1 to 15). Furthermore, cage-based networked materials (TC1-P1 and TC1-P2) were successfully constructed through the iEDDA polymerization using TC1 as building unit, resulting in tunable porous frameworks with improved CO2/N2 selectivity.

Red-light-driven, oxygen-tolerant reversible addition–fragmentation chain transfer (RAFT) polymerization using methylene (MB+) and triethanolamine (TEOA) enables the synthesis of degradable α-lipoic acid–vinyl copolymers with high molar mass (600 000 g mol−1), low dispersity, and high LA incorporation. The method tolerates diverse vinyl comonomers and yields poly(disulfide)s degradable by reducing agents, UV light, or ambient sunlight.

α-Lipoic acid (LA) has recently emerged as an attractive, inexpensive monomer for synthesizing degradable polymers via ring-opening of its 1,2-dithiolane, introducing easily cleavable disulfide linkages into polymer backbones. Reversible addition–fragmentation chain transfer (RAFT) copolymerization with vinyl monomers enables access to degradable poly(disulfide)s with controlled molecular weights. However, conventional thermal RAFT methods suffer from oxygen sensitivity, limited LA incorporation (<40 mol%), and modest degrees of polymerization (DP < 300). Here, we report an oxygen-tolerant, red-light-driven RAFT approach using methylene blue (MB⁺) as a photosensitizer, and triethanolamine (TEOA) as a sacrificial electron donor. This photoRAFT strategy affords well-defined LA–vinyl copolymers with DPs exceeding 6000, relatively low dispersities (Đ = 1.1–1.6), and LA incorporations up to 68 mol%. The method is compatible with a broad range of functional comonomers, including hydrophilic, charged, and zwitterionic acrylates and acrylamides, yielding water-soluble degradable polymers. The resulting copolymers are readily degradable by disulfide-reducing agents, UV light, and ambient sunlight. Overall, this mild and efficient platform overcomes the limitations of thermal RAFT, providing improved access to functional, high-molecular-weight degradable LA copolymers, suggesting potential applications as biocompatible plastics and biomedical materials.

The high-voltage structure degradation in O3-type layered oxides arises from co-deteriorating coupling between σ-type oxygen redox and cationic migrations. An anchoring ligand electron (ALE) strategy is proposed to confine oxygen redox in stable π-type configurations, reinforcing metal-oxygen coordination. Calcium ions, identified via multi-level screening as the optimal anchor agent, impart robust structural stability at 4.5 V during cycling.

High-voltage operation enables sodium-sufficient O3-type layered oxides to approach the maximum achievable energy densities for practical sodium-ion batteries (SIBs). This high-voltage regime, however, induces structural degradation strongly correlated with oxygen redox activity, a mechanism still incompletely resolved. Using prototypical O3-type NaNi1/3Fe1/3Mn1/3O2 (NFM) as a model system, we identify the origin of this instability as a detrimental feedback loop between σ-type oxygen redox and cation migration. We thus propose an “anchoring ligand electron (ALE)” strategy, employing a multi-level screening protocol to identify optimal anchor agents that confine oxygen redox to stable π-type configurations with robust metal-oxygen coordination. The ALE-engineered NFM cathode mitigates excessive oxygen ligand electron transfer, achieving record capacity retention at an ultrahigh voltage of 4.5 V after 300 cycles. The superior cyclic stability is demonstrated to be closely associated with the stable π-type oxygen redox and suppressed metal-oxygen decoordination. This ALE strategy expands the optimization pathway toward ultrahigh-voltage and high-energy-density cathodes.

Using a newly developed ReaxFF force field, we uncover the temperature-dependent molecular composition of liquid sulfur above its polymerization threshold, revealing the existence of sulfur macrocycles that were previously disregarded. This discovery reconciles long-standing discrepancies between experimental observations and theoretical models.

A detailed understanding of the composition and polymerization mechanism of elemental sulfur remains a decades long unresolved question for modern chemistry. However, the dynamic nature of molten sulfur significantly complicates its accurate characterization. To overcome this challenge, we performed the first comprehensive molecular dynamics (MD) simulations using a ReaxFF reactive force field specifically parameterized to capture the complex ring-opening polymerization dynamics of elemental sulfur. Rigorous development of the force field parameters, trained against extensive quantum mechanical datasets, was key to enabling these large-scale (>10 000 atoms) reactive MD simulations at polymerization-relevant temperatures. This study provides the first detailed atomic-level description of liquid sulfur, elucidating temperature-dependent molecular composition and offering unprecedented insights into sulfur polymerization mechanisms. These are the first simulations to reveal the formation of remarkably large macrocyclic sulfur rings at the onset of polymerization—a discovery that challenges longstanding mechanistic misconceptions, thus reshaping our understanding of sulfur polymerization. Our findings highlight the power of molecular dynamics in exploring complex polymerization processes, with broad impact in dynamic covalent chemistry and covalent adaptable polymers.

A Ru-functionalized carbonized TS-1 zeolite (Ru@TS@C) enhances charge transfer and photogenerated carrier separation, enabling photo-assisted near-neutral Zinc–air batteries with exceptional 4e− selectivity (74% lower overpotential, 218 versus 844 mV at 0.2 mA cm−2 under light) and reversibility. Extended to Li–O2 systems, it delivers superior rate capability and cycling stability, establishing zeolite-based photoactive cathodes for advanced metal–air batteries.

Neutral aqueous Zn−air batteries (ZABs), while promising for extended lifespans and recyclability compared to alkaline systems, are hindered by sluggish kinetics that limit energy efficiency and power output. Here, we report an effective approach to construct a photo-assisted near-neutral ZAB based on a photo-responsive titanium silicalite-1 zeolite (TS-1). The incorporation of Ru active centers into the 3D porous architecture of TS@C (Ru@TS@C), which exhibits remarkably enhanced electronic conduction, creates interconnected conductive pathways. This unique design facilitates rapid charge transfer across the 3D network, enabling exceptional reaction kinetics, and improved separation efficiency of photogenerated electron–hole pairs. Synergistic experimental and theoretical analyses reveal a photoinduced charge transfer mechanism in the conductive zeolite, where light-driven Ru-mediated electron exchange with oxygen adsorbates accelerates 4e−-dominant oxygen reduction reaction (ORR) kinetics. Consequently, the Ru@TS@C-based photo-assisted ZAB exhibits exceptional 4e− selectivity and reversibility, achieving a low overpotential of 218 mV at 0.2 mA cm−2 under illumination (74% reduction compared to dark conditions). Extended to Li–O2 batteries, this multifunctional architecture demonstrates superior rate capability and cycling stability (>150 cycles). This work pioneers the use of photoactive zeolites in metal–air batteries and establishes a universal framework for engineering photo-responsive interfaces to overcome intrinsic kinetic limitations in sustainable energy systems.

Amphiphilic linear block copolymers self-assemble into inverse photonic glass beads with ull visible-range coloration. The porous morphology and reactive design enable post-synthetic control over pore size and wall thickness, paving the way toward scalable, chemically programmable pigmentss for next-generation optical systems.

Structurally colored colloids, or photonic pigments, offer a sustainable alternative to conventional dyes, yet existing systems are constrained by limited morphologies and complex synthesis. In particular, achieving angle-independent color typically relies on disordered inverse architectures formed from synthetically demanding bottlebrush block copolymers (BCPs), hindering scalability and functional diversity. Here, we report a conceptually distinct strategy to assemble three-dimensional inverse photonic glass microparticles using amphiphilic linear BCPs (poly(styrene-block-4-vinylpyridine), PS-b-P4VP) via an emulsion-templated process. By employing trans-1,2-dichloroethylene to promote interfacial water infiltration, nanoscale aqueous domains form within the organic phase and direct short-range-ordered pore structures. Evaporative solidification arrests these structures into porous photonic beads with angle-independent color. Systematic control of surfactant alkyl chain length and BCP molecular weight enables precise tuning of pore size, shell thickness, and visible-range optical output. Furthermore, post-chemical modification via quaternization of P4VP provides an orthogonal chemical handle to modulate interfacial instability and photonic behavior. This work expands the self-assembly capabilities of linear BCPs and establishes a modular, scalable platform for producing structurally and chemically programmable photonic pigments.

The translation of new dynamic covalent thioorthoester chemistry into crosslinked metal scavengers and porous sulfur-rich lithium battery cathodes is highlighted as an example how the integration of new principles in supramolecular chemistry can open new directions to approach questions of significance in science and society.

Supramolecular chemistry promises that insights into contact between molecules will open up new directions to approach significant questions in science and society. In this spirit, Kraus et al. report the translation of fundamentally new dynamic covalent thioorthoester chemistry into metal-scavenging porous network materials and sulfur-rich, leakage-free cathode composites in lithium batteries (https://doi.org/10.1002/anov.70000).