Multiscale-designed synthesis of amidoxime-based covalent organic polymers for uranyl extraction applications

Pd(II)-coordinated porous organic polymer anchoring Pd NPs: An efficient cooperative and sustainable catalyst for Suzuki-Miyaura cross-coupling reactions

π-π Interaction mediated energy storage in β-Ketoenamine covalent organic polymer electrode

Integrated experimental and theoretical engineering of an advanced triazole–amide functionalized porous organic polymer via click chemistry for sustainable removal of picric acid

Rationally designed bifunctional covalent organic polymers for broad-spectrum-driven photothermal catalytic Cr(VI) reduction and iodine capture

The development of dynamic organic phosphorescent polymers is often limited by the challenge of exerting precise and reversible control over their condensed matter structures. While external stimuli can modulate emission, a fundamental materials-level principle for governing hierarchical reorganization remains elusive. Here, we report that ion-driving entanglement of polymer chains serves as a powerful general strategy to direct reconfigurable hierarchical structures, thereby enabling highly tunable organic phosphorescence. Specifically, potassium ions programmatically bridge ether and sulfonic acid groups within κ-carrageenan (κCG), triggering polymer entanglement and chromophore aggregation to form a dynamically reversible architecture. This structural transformation, validated by atomic force microscopy (AFM) and rheology, grants control over triplet exciton behavior, yielding phosphorescence that is tunable from blue to green (CIEy: 0.037-0.382) with a lifetime of up to 199.50ms and an efficiency of 17.97%. The entanglement is thermally reversible, allowing on-demand emission switching. Furthermore, we demonstrate the translational potential of this mechanism by constructing a visual urinary potassium analyzer, where ion-concentration-dependent phosphorescence enables quantitative detection. This work establishes polymer entanglement as a central design principle for adaptive photonic materials, opening avenues for smart sensing and healthcare monitoring.

Organic electrodes hold promise for sustainable, cost-effective, grid-scale aluminum metal batteries (AMBs) that store aluminum complex ions. However, most conventional organic polymers reported to date suffer from sluggish redox kinetics and structural collapse, which severely restrict the rate performance and cycling stability. Herein, we report a thiophene-amine porous organic framework (TA-POF) cathode that integrates dual redox-active N and S sites, large 1D channels, and an extended π-conjugated backbone. These structural advantages enable efficient electronic delocalization and rapid AlCl4- ion diffusion. The resulting AMBs exhibit a high energy efficiency of 88.3% and outstanding long-term cycling stability, showing no degradation over 2000 cycles and offering an operational life that exceeds that of most AMB cathodes. Importantly, at a high areal loading of 6.9 mg cm-2, the AMB still delivers 91% of the capacity obtained at low loading. Ex situ studies verify a reversible dual-site anion storage process. This work establishes thiophene-amine POF as a robust platform for designing durable, efficient, and sustainable AMBs.

In this work, highly porous organic polymers with α,β-enone-linkage were synthesized via the Horner-Wadsworth-Emmons (H-W-E) polymerization in 10-20 g, and the catalytic amount of AlCl3 was found to increase the BET surface area of the as-prepared BIT-POP-120 and BIT-POP-121 dramatically (up to 716 m2 g-1), much higher than that of enone-liked porous organic polymers (POPs) reported. More importantly, this H-W-E polymerization of triphsophonate 4 with 2,5-hexanedione 6 provided a powerful way to offer 18% flexible moiety in BIT-POP-121 based on low-field NMR. Very high Pd/Pt selectivity of 3.54 and 28 was observed for BIT-POP-121 respectively, based on the adsorption capacity and Kd value using a binary solution of Pd2+ and Pt2+. This is very promising for the Pd recovery from the spent automotive catalytic converters in the future. The powerful strategy for making flexible POPs by H-W-E polymerization using easily available and stable aliphatic diketones will lead the development of high-performance flexible POPs for broad applications including recovery of precious metals in the near future.

A green, sustainable, and ultrasound-assisted method for the synthesis of β-enaminone derivatives was developed. This study introduces a sulfur-enriched coal tar-based porous organic polymer (CTHP-SES) as a highly efficient, metal-free catalyst, providing an environmentally friendly alternative to conventional synthetic methods. The synthesis employed CTHP-SES, a metal-free catalyst characterized by a microporous framework and thiol-functionalized acidic sites. Optimization studies were conducted to determine the optimal reaction conditions, including solvent selection and catalyst loading. Propylene carbonate was identified as the most suitable solvent, while 20 mg of catalyst afforded efficient conversion under mild, ultrasound-assisted conditions. The optimized protocol enabled the synthesis of β-enaminones in yields of up to 93% within only 20 minutes. The CTHP-SES catalyst exhibited a broad substrate scope, efficiently converting a wide range of aromatic and aliphatic amines. Notably, it outperformed conventional catalysts such as ZnCl₂, AlCl₃·6H₂O, FeCl₃, and p-TSA in terms of catalytic activity and recyclability, retaining more than 71% of its initial efficiency after seven reuse cycles. The excellent catalytic performance of CTHP-SES is attributed to its acidic framework, which facilitates ketone activation. Its superior activity and reusability highlight its potential as a sustainable green catalyst. Molecular docking studies against the CTX-M-64 enzyme revealed strong antibacterial potential for the synthesized β-enaminones, with compound E-17 exhibiting the highest binding affinity (-8.22 kcal mol⁻¹), suggesting promising therapeutic applications. This study successfully established a sustainable and efficient ultrasound-assisted protocol for the synthesis of β-enaminones using the CTHP-SES catalyst. The synthesized β- enaminones demonstrated significant antibacterial potential, highlighting the dual applicability of this work in both catalysis and medicinal chemistry.

Integrating organic photovoltaics into anodes (IPV-anodes) represents a promising way to exploit the excellent optoelectronic properties of organic polymer: non-fullerene bulk-heterojunctions (BHJ) for solar-to-fuel applications. However, the high voltage losses, poor photochemical stability and high synthetic complexity of the most commonly used polymer: non-fullerene combinations have limited their full potential. Here, we address these limitations by introducing a BHJ comprising the low-synthetic-complexity polymer PTQ10 and the near-infrared absorbing acceptor L8-BO. By integrating this new BHJ with a graphite sheet functionalised with a NiFeOOH catalyst, we achieve a low onset potential of +0.64 VRHE, a photocurrent density of 21 mA cm-2 at +1.23 VRHE and a t 80 operational stability of 22 h under full AM1.5 G illumination (i.e., without using any UV filter) for water oxidation. These values represent a 40 mV increase in photovoltage and a sevenfold improvement in operational stability (t 80 extended from 3 h to 22 h) compared to reference IPV-anodes based on the ternary D18:PM6:L8-BO photoactive blend. Spectroscopic analyses reveal that these improvements stem from the reduced non-radiative voltage losses (from 0.24 V to 0.19 V) and superior photochemical and morphological stability of the PTQ10:L8-BO blend compared to the reference blend. Building on these advances, we demonstrate monolithic tandem IPV-anodes integrating PTQ10:IDIC and PTQ10:L8-BO organic blends to achieve a solar-to-hydrogen efficiency of 6.2%, offering critical insights for boosting the stability and efficiency of integrated solar-to-hydrogen systems working without any external bias.

Hypercrosslinked polymers, a class of porous organic polymers (POPs), are constructed by crosslinking linear polymers or knitting small aromatic molecules with a molecular crosslinker, typically via Friedel-Crafts alkylation. In this study, we report a new approach for the synthesis of POPs via the crosslinking of linear polyimines with m‑phenylenediamine through nucleophilic addition of amines to imines, forming aminal linkages. The resulting aminal-linked POPs, with an estimated low cost of 16USD/kg, exhibited high surface areas up to 650m2/g and abundant microporosity, in contrast to the ∼100m2/g observed for the linear polyimine. This method demonstrated good generality: four linear polyimines with different structures were successfully crosslinked into POPs with high porosity. Both experimental results and theoretical calculations indicate that the use of diamines at the meta-position is critical for efficient crosslinking, whereas para-diamines did not initiate crosslinking. With their high surface area and rich microporosity, these POPs displayed high adsorption capacities for C2 hydrocarbons and CO2, but significantly lower capacity for CH4. Dynamic breakthrough experiments confirmed excellent separation performance for C2 hydrocarbons/CH4 mixtures, highlighting their potential for hydrocarbon separation. This study provides a new strategy for the synthesis of cost-effective POPs and demonstrates their promising applications in gas separation.

Porous organic polymers (POPs) are promising photocatalyst substrates due to their high surface area, tunable pore size, and functionalization versatility. However, these materials face challenges in structural stability suffering from reversible covalent bonds, rapid electron-hole recombination, and limited scalability in synthesis for photocatalytic water purification. Herein, we demonstrate a cost-effective strategy by depositing nonprecious metal hydroxides (Fe(OH)2, Ni(OH)2, and Zn(OH)2) onto a simple triazine-based POP (PT) to enhance interfacial charge transfer and photocatalytic activity. Remarkably, the Zn(OH)2-modified PT composite (PT-Zn(OH)2) achieves 98% degradation of 10 ppm methylene blue within 40 min─a 2.3-fold improvement over pristine PT (42%). Systematic characterization (UV-vis, XPS-VB, electrochemical impedance spectroscopy, and PL) reveals that Zn(OH)2 deposition optimizes the semiconductor's band structure, reduces charge recombination, and improves interfacial electron-hole separation kinetics. This work highlights the pivotal role of metal hydroxide-POP interfacial engineering in enhancing photocatalysis and provides a scalable, precious-metal-free design for efficient pollutant degradation.

Perovskite quantum dots (PQDs) are promising candidates for next-generation displays but suffer from poor stability during manufacturing and application. Owing to their intrinsic soft lattice and weak surface ligand-lattice bonding, PQDs degrade easily under light, heat, humidity, and oxygen. Herein, we propose an inorganic-organic covalently bonded dual-shell encapsulation strategy for PQDs. An inorganic inner shell locks the crystal surface to ensure structural stability, while the inorganic shell links to an organic acrylate polymer shell via Si-O-Si bonds to improve dispersion and chemical cross-linking, thereby enhancing the encapsulation of individual PQDs. Benefiting from this strategy, PQDs retain more than 90% of their pristine fluorescence lifetime and maintain stable colloidal dispersion even after 30 days of storage in polar solvents. Under 75% relative humidity, ambient air, and 10,000 cd/m2 blue light irradiation for 100 h, the fluorescence intensity of the prepared PQD film remained at 96.081 ± 0.019%, compared to 40.037 ± 0.024% for the pristine sample group, indicating enhanced blue light resistance. Carboxylic acid groups in the organic shell precisely passivate surface defects, boosting the photoluminescence quantum yield (PLQY) from 59.1% to 98.3%. Utilizing alkenyl double bonds in surface ligands and their photoinitiated cross-linking, 5 μm high-resolution pixel patterning is achieved. The PQD-based color conversion layer exhibits excellent stability, delivering a brightness of 1,468,161.5 cd/m2 under excitation from a 445 nm blue-light chip and a 67.7-year operational lifetime at 100 cd/cm2, which is 100-fold longer than that of unencapsulated PQDs. This strategy enables the practical application of PQDs in high-resolution backlight displays.

Air-fed electrochemical H2O2 production via the two-electron oxygen reduction reaction (2e- ORR) offers a sustainable alternative to conventional processes, yet its efficiency is fundamentally constrained by low O2 availability and intrinsically coupled electron-proton transfer. Here, we construct a bifunctional covalent organic polymer interface integrating carbonyl electron-relay units and quaternary ammonium cationic motifs on commercial carbon black (QSPIP-TMC@CB), enabling efficient H2O2 electrosynthesis directly from air. The QSPIP-TMC@CB delivers a H2O2 production rate of 3410.1 mmol·h-1·g-1 with 91.4% H2O2 Faradaic efficiency (FEH2O2) under air, and sustains stable operation at 100.0 mA·cm-2 for 35.0 h. Mechanistically, carbonyl motifs function as reversible redox mediators that facilitate electron injection into O2, while quaternary ammonium cations enrich interfacial O2 and regulate proton accessibility via Donnan repulsion, suppressing excessive protonation of the *OOH intermediate and preventing O─O bond cleavage. This cooperative regulation decouples electron transfer from proton supply, thereby stabilizing the 2e- pathway under O2-lean conditions. The strategy is readily extendable to representative ORR catalysts (Co─N─C and ZnO) and enables gram-scale H2O2 production (4.8g h-1 at 5.0 A, 1.0 wt% within 5min), establishing functionalized-interface electron-proton decoupling as a general and scalable design paradigm for air-fed H2O2 electrosynthesis.

Mononitrogen-containing aromatic compounds, exemplified by carbazole (CZ) and triphenylamine, are emerging as promising high-potential candidates (3.6-4.3V vs. Li+/Li) for p-type anion-storage electrode materials. However, the inherent reactivity of their para positions at elevated potentials (>4V) induces undesirable electropolymerization, leading to severe low initial coulombic efficiency (ICE). Herein, we propose an active-site blocking strategy to fundamentally address this critical challenge through molecular engineering. Specifically, we develop a CZ-based organic polymer, poly[5-(9-ethyl-9H-carbazol-3-yl)-5,10-dihydrophenazine] (p-ECZDPZ), tailored as the model system to validate the efficacy of our proposed strategy. By strategically incorporating 5,10-dihydrophenazine and ethyl group into its structure, the active para positions of the CZ moieties are effectively blocked. This enables a superior ICE of 86% without requiring any pretreatment, surpassing other known CZ-based organic electrode materials to date. The constructed Li-based dual-ion full batteries (LDIBs) achieve a peak discharge capacity of 204 mAh g-1, an ICE of 84%, and a stable operation over 20 000 cycles. At high cathode mass loading, the LDIBs demonstrate an energy density of 445Wh kg-1 while retaining no capacity decay for 8000 cycles. Pouch-type full cells achieve direct activation during the first charge process, realizing an energy density of 305Wh kg-1 cathode.

Developing an efficient and robust photocatalyst for optimal C2+ product generation from carbon dioxide (CO2) is a pressing need in advancing solar fuel production. In this study, we designed an ionic vinylene-bridged conjugated porous organic polymer (Py-POP) enriched with charged pyridine groups via a quaternization-promoted Knoevenagel condensation reaction. The resulting positively charged polymeric framework with shape-persistent nanochannels enabled the uniform assembly of SnS2 units through ionic interactions mediated by amino and sulfhydryl groups. The hybrid porous photopolymer (SnS2@Py-POP) converts CO2 into ethylene with a rate of 34.7 μmol g-1 h-1 with a selectivity of ethylene around 78.7% under visible light photoirradiation, which outperforms all the C2 selective Sn-based photocatalysts. Our findings principally sheds light on the mechanism of selectivity reversal (from C1 to C2 product) by hybrid catalyst framework engineering. In-depth investigations by synchrotron-based X-ray absorption spectroscopy (XAS) and morphological analysis via high-resolution transmission electron microscopy (HRTEM) reveal the nature of interaction for hybrid heterostructure formation within the porous network. Electron transfer pathways were mapped using time-resolved photoluminescence (TRPL) and transient absorption spectroscopy (TAS), which revealed a Z-scheme electron transfer mechanism. This mechanism facilitates enhanced electron accumulation on the SnS2 layer, promoting efficient CO2 activation and subsequent C-C coupling, ultimately leading to ethylene formation. Furthermore, the ethylene formation mechanism has been investigated in detail by time-resolved diffuse reflectance infrared spectroscopy (TR-DRIFTS), corroborated with density functional theory (DFT). This study opens a new avenue for achieving selectivity reversal in a C1 selective photocatalyst through electronic modulation enabled by the formation of an inorganic-organic hybrid heterostructure.

The design and manufacture of bifunctional electrocatalysts are of great significance in the electrolysis of water. Herein, porous organic polymers (POPs) of metal-N-heterocyclic carbene were synthesized from imidazolium borate ionic POPs and supported on a nickel foam surface (Pd-NHC/NF, Ag-NHC/NF, and Cu-NHC/NF). Among them, Pd-NHC/NF exhibited high activity for both hydrogen evolution reaction and oxygen evolution reaction. The oxygen evolution overpotential of Pd-NHC/NF was 245 mV with a Tafel slope of 83 mV dec-1; the hydrogen evolution overpotential was 139 mV with a Tafel slope of 94 mV dec-1 at 10 mA cm-2 in alkaline media. Additionally, the assembled Pd-NHC/NF||Pd-NHC/NF electrolyzer demonstrated excellent performance in electrocatalytic water-splitting, achieving a voltage of 1.55 V at 10 mA cm-2 and showing outstanding stability for over 90 h in the long-term test. The results highlighted the substantial capability of Pd-NHC as a bifunctional catalyst for electrocatalytic water-splitting.

The in situ BINOL formation strategy afforded, for the first time, core-engineered BINOL-based porous organic polymers (POPs) containing tetraphenylethylene and pyrene. These POPs exhibited volatile iodine vapor uptake of up to 371 wt% and photocatalytic degradation of methyl orange within 50 min, showcasing the potential of BINOL-based POPs for all-around decontamination.

Indirect transmission of viruses via contaminated surfaces highlights the need for effective antiviral coatings. Recent advances have led to the development of diverse surface engineering strategies, including organic (polymer- and peptide-based) and inorganic (metal-based) coatings. While polymer and peptide-based systems have been extensively explored in the antibacterial field, their application in antiviral coatings remains underexplored despite their demonstrated ability to reduce viral titers. This minireview provides a mechanistically informed overview of polymer- and peptide-based antiviral surface coatings. We summarize recent studies with a focus on coating materials, methods, physicochemical characterization techniques, target viruses, and antiviral performance. In addition, we critically evaluate key limitations in the field, including the lack of standardized testing protocols, restricted diversity of surfaces and viruses, and insufficient assessment of coating durability and cytotoxicity. Finally, we discuss future directions focused on standardized and rationally designed evaluation frameworks to support the practical translation of antiviral coatings.

Developing high-performance supercapacitors requires an optimal balance of capacitance, energy, and power density together with long-term cycling stability. Here, we report a family of heteroatom-doped, spin-active, and redox-active hexaazatriphenylene-quinone covalent organic polymers (COPs) prepared through complementary mechanochemical and solution-phase syntheses. These materials exhibit chemical robustness under acidic conditions and strong pseudocapacitive activity arising from delocalized spin centers and quinone redox sites. Among them, COP-2 displays the most favorable electrochemical characteristics, achieving an areal capacitance of up to 6214 mF/cm2 (863 F/g) and an unprecedented energy density of 1.91 mWh/cm2 (266 Wh/kg) at 1 mA/cm2 in symmetric two-electrode devices. The material also demonstrates high-rate capability with a maximum power density of 51.4 mW/cm2 (7139 W/kg) and stable cycling performance, retaining 82.1% capacitance after 50,000 cycles. Mechanistic studies combining spectroscopy, electrochemical analysis, and electronic structure simulations highlight the interplay of redox activity and spin delocalization in governing charge storage. These results establish a molecular-to-device design framework for developing spin-active porous polymers as advanced energy storage materials.