Ni-Ag or Ti-Ag co-doped crystalline/amorphous WO3 core/shell hybrid nanorod arrays (WWNA and WWTA) were rationally designed to address three key factors-crystallinity, surface morphology, and conductivity that critically influence the electrochromic (EC) performance of WO3. In this architecture, vertically aligned, selfsupporting single-crystalline hexagonal WO3 nanorods serve as the scaffold, overlaid by a layer of amorphous WO3 films co-doped with Ni-Ag or Ti-Ag. This hierarchical structure offers multiple advantages: (1) the 1D nanorods provide a high surface area for redox reactions; (2) the crystalline/amorphous interface promotes strong interfacial coupling; (3) Ni or Ti doping introduces lattice distortion and oxygen vacancies; (4) W-O-Ni or W-O-Ti bonds modulate the band structure, enhancing optical absorbance; and (5) embedded Ag subnanoparticles restructure the local electronic environment, boosting conductivity. As a result, the WWNA-10 and WWTA-10 structures exhibit excellent EC performance, with high optical modulation (60.92 % and 62.39 % at 630 nm), fast coloring/bleaching times (5.54/2.06 s and 5.06/1.71 s), and good cycling durability (WWTA10 retains 93.9 % of its initial redox activity after 1000 cycles). This co-doped core/shell design offers a synergistic strategy beyond conventional doping or morphology control, paving a promising pathway for nextgeneration high-performance EC materials.
The ternary strategy, which introduces a third component into the binary system, is a simple and effective method for boosting power conversion efficiency (PCE) of organic solar cells (OSCs). Herein, a novel non-fused-ring small molecule acceptor (NFR-SMA), namely DFTQA-2Cl, featuring a medium bandgap and high planarity, was designed and synthesized through a synergistic strategy combining terminal chlorination and an isomeric thiophene it-bridge. The introduction of DFTQA-2Cl into the D18:Y6 binary system creates a ternary blend with complementary absorptions and cascaded energy alignment, which accelerates exciton dissociation, enhances charge collection, and boosts current density for in high-performance OSCs. Simultaneously, doping modulation via DFTQA-2Cl optimizes the micromorphology and phase separation size of active layer. Based on this, the optimized ternary OSC based on D18:Y6:DFTQA-2Cl achieved a notable PCE of 18.04 %, a 6.68 % enhancement over the 16.91 % of its binary D18:Y6 system, along with simultaneous enhancements in other parameters. Additionally, the ternary OSCs achieved a T80 operational stability of over 1500 h. This work illustrates that incorporating a medium-bandgap NFR-SMA with good planarity as a third component in a binary system effectively enhance the basic parameters of ternary OSCs.
Reactive oxygen species (ROS)-based endoplasmic reticulum (ER) stress is a prerequisite for the induction of immunogenic cell death (ICD), and the development of metal-based ICD inducers has garnered significant attention. However, the drug-target mechanisms of ICD inducers still require further exploration. Herein, we reported an ER-targeting iron(II) complex (Fe-NBM) as an ICD inducer, which was obtained through a solvothermal domino reaction. Accordingly, pyridin-2-ylmethanamine and 1-methyl2-formylbenzimidazole underwent consecutive covalent transformations to form a novel N -heterocyclic ligand, which subsequently coordinated with ferrous chloride to directly yield the crystalline Fe-NBM in one pot. Confocal laser scanning microscope (CLSM), molecular docking and cellular thermal shift assay (CETSA) showed that Fe-NBM could specifically target the ER by binding to the IRE1 alpha (Inositol Requiring kinase Enzyme 1 alpha) and induce ICD by generating ROS-based ER stress. In an immunocompetent mouse model, Fe-NBM could significantly inhibit tumor growth and stimulate anti-tumor immunity, and exhibit an enhanced effect when combined with anti-PD1 therapy, leading to near-complete tumor elimination. To gain deeper understanding of how to synthesize such effective ICD inducers at the molecular level, a combination of electrospray ionization mass spectrometry (ESI-MS) and crystallography was employed for thoroughly tracking the step-economy synthetic process. To the best of our knowledge, Fe-NBM is the first iron-based ICD inducer that directly targets ER through binding to IRE1 alpha. We believe that the ICD-related target information presented in this work will enhance our understanding of the molecular mechanisms underlying ICD and facilitate the design of new ICD inducers. (c) 2026 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
In most Mn4+ aliovalent-doped A2BB’O6 phosphors, the generated defects acted as non-radiative quenching centers, which intensified the phonon-electron interaction and thereby enhance the non-radiative transition. In this study, Mn4+-based isovalent-doped double perovskite luminescent materials were targeted for investigation. Equimolar Zr4+ and W6+ cations were employed to fully replace the B’ (pentavalent cations) sites in Sr2GdB’O6, thereby providing isovalent doping sites for Mn4+ ions, which substantially improved the luminescent efficiency and thermal stability of the materials. The results demonstrate that the as-prepared red luminescent material Sr2GdZr0.5W0.5O6:Mn4+ (SGZW:Mn4+) exhibits an internal quantum efficiency (IQE) of 46.47%. At 423 K, the emission intensity retained more than 71% of its room-temperature emission intensity. In plant growth lighting tests, the high-efficiency SGZW:Mn4+ effectively provided red light supplementation for plants. Additionally, white light-emitting diode (WLED) packaging tests confirmed that its red emission plays a crucial role in regulating the color temperature of the WLED device. This work achieved the performance enhancement of Mn4+-activated double perovskite red luminescent materials through composition optimization, offering an effective modification strategy for the design of analogous material systems in the future.
A new type of B-embedded ultra-stable green emission TADF emitter t BuNO– t BuBO can stably emit at 516 ± 6 nm after doping 10–100% in OLED. Its interaction with DMAP induces optical changes, providing a new strategy for display and sensing fields.
With the rapid development of ternary organic photovoltaics (OPVs), exploring highly efficient matching ternary components has become a key issue. Herein, a ternary OPV was fabricated using J71 and PBDTTS-2FQx as donors and IT-4F as the acceptor. Binary devices based on J71:IT-4F and PBDTTS-2FQx:IT-4F achieved power conversion efficiencies (PCEs) of 9.52% and 6.44%, respectively. By leveraging the advantages of the two systems, a ternary OPV incorporating both donors was successfully prepared. With a weight ratio of J71:PBDTTS-2FQx:IT-4F of 0.85 : 0.15 : 1, the ternary OPV achieved an optimum PCE of 11.23%, along with improved short-circuit current density (JSC) and fill factor (FF). Moreover, the ternary OPVs exhibited substantially enhanced stability relative to the binary ones. The unencapsulated J71:IT-4F OPV retained 80% of its initial PCE after 530 h, while the unencapsulated ternary OPV retained 80% efficiency after 1000 h. This enhanced stability arises from the good compatibility between J71 and PBDTTS-2FQx, which facilitates the formation of an alloy-like donor phase.
ABSTRACT Novel synthetic methods offer significant potential to accelerate drug development, yet there remains a largely unexplored area for efficiently synthesizing metal‐based anticancer agents. Herein, we report a novel solvothermal domino reaction of pyridine‐2‐methylamine (and its 4‐OCH 3 ‐substituted derivative), benzaldehyde, and CuCl 2 ∙2H 2 O, which simultaneously achieves ligand synthesis and coordination assembly in one pot and facilely affords innovative dinuclear dicoordinate copper(I) complexes ( Cu1 and Cu2 ) with the in situ‐formed bulky steric‐hindering tetraarylethane ligands featuring the bis‐imidazo[1,5‐ a ]pyridine scaffold. The unique geometry of Cu1 and Cu2 confers physiological stability and vacant coordination sites for efficiently catalyzing Fenton‐like reactions. Further studies reveal that Cu2 effectively elevates intracellular copper ion levels to induce cuproptosis, concurrently disrupting cellular redox homeostasis to trigger ferroptosis. The concurrent cuproptosis‐ferroptosis activation finally elicits significantly enhanced immunogenic cell death (ICD), which facilitates the antitumor activity of Cu2 . Moreover, in combination with immune checkpoint inhibitor α PD‐1, Cu2 exhibits improved immunotherapy effects. This work introduces the first small‐molecule copper complex that achieves immunotherapy potentiation through cuproptosis‐ferroptosis‐ICD induction and provides a new pathway for accessing innovative metal‐based antitumor agents through such a rationally designed domino reaction.
Pure-green organic emitters compliant with the Broadcast Television 2020 (BT.2020) green standard are critical for ultra-high-definition (UHD) organic light-emitting diodes (OLEDs). Herein, we propose a simple yet effective spiro-fluorene locking strategy to develop two pure-green multi-resonance thermally activated delayed fluorescence (MR-TADF) emitters, namely DBN-MS and DBN-TMS. The introduction of the spiro-fluorene units not only extend π-conjugation to redshift emission to 512-513 nm but also enhance molecular planarity and rigidity, suppressing vibrational relaxation and enabling ultra-narrow full-width at half-maximum (FWHM = 16 nm) in toluene. Notably, DBN-MS maintains stable emission profile (λem = 518-520 nm, FWHM = 19-20 nm) across a broad doping concentration range (1-10 wt%), effectively mitigating spectral broadening and aggregation-caused quenching. Non-sensitized OLEDs exhibit a maximum external quantum efficiency (EQE) of 35.5%, low efficiency roll-off with an EQE value of 26.9% at 1000 cd m-2, and remarkable operational stability with lifetime (LT90) of 167 h in a stable device structure. More importantly, the state-of-the-art CIEy coordinates of 0.76-0.77 are demonstrated over 1-10 wt% broad doping range, representing the first bottom-emitting green OLED with a CIEy value reaching 0.77, and the closest to the BT.2020 green standard reported to date.
Polytetrafluoroethylene (PTFE) is widely used owing to its exceptional chemical and thermal stability; however, these same properties render it highly persistent in the environment, contributing to long-term fluorinated waste. Conventional degradation methods, such as pyrolysis above 500 °C or treatment with alkali metals, are energy-intensive and operationally demanding, highlighting the need for mild and practical defluorination strategies for sustainable fluoropolymer recycling. Here we report a visible-light-driven photocatalytic protocol for PTFE defluorination under mild conditions. The method uses carbazole-based photocatalysts (CBZ6 and KQGZ), readily prepared in two to three steps from commercial precursors, and proceeds in standard glassware under purple light-emitting diode irradiation. Finely divided PTFE powder (~1-μm particle size, 20-mg scale) is treated with a photocatalyst, base and sacrificial reductant, with dispersion maintained by intermittent sonication. Critical parameters influencing reactivity include photocatalyst identity and loading, dispersion efficiency, base purity and physical form, light source configuration, temperature control and irradiation time. The reaction yields soluble fluoride salts and a defluorinated amorphous carbon, along with carbon-derived oxyanions. Fluoride ions are quantified by 19F NMR spectroscopy or ion chromatography and can be recovered as potassium fluoride by recrystallization. The amorphous carbon is characterized primarily by Raman spectroscopy, supported by X-ray photoelectron spectroscopy, solid-state NMR and IR spectroscopy. The protocol is straightforward and accessible to researchers with standard training in organic synthesis, including graduate students and experienced laboratory technicians. The full protocol, encompassing photocatalyst preparation, PTFE defluorination and product characterization, can be completed in 189 h (59 h hands-on time).
Organic light-emitting diodes (OLEDs) simultaneously requiring high efficiency and narrowband emission are crucial for ultra-high-definition displays. Our previously developed spiro‑boron acceptor (Spiro-PMB) based on B ← N coordination, when combined with conventional donors, achieved an excellent external quantum efficiency (EQE) up to 30% but exhibited a broad emission spectrum with a full width at half maximum (FWHM) exceeding 80 nm, which is typical for donor–acceptor type thermally activated delayed fluorescence (TADF) materials. Here, we report a simple molecular engineering strategy to narrow the emission while preserving high efficiency by directly replacing the conventional donor unit with a three-coordinated boron multiple-resonance (MR) moiety (tCzBN). The resulting MR–D–A hybrid compound, B1, exhibits excellent thermal stability (Td = 492 °C), narrowband photoluminescence with FWHM of 25 nm in toluene, a small singlet–triplet energy gap (ΔEST) of 0.10 eV, and a fast reverse intersystem crossing rate of 5.81 × 105 s−1. Solution-processed OLEDs based on B1 emit green electroluminescence at 506 nm with a FWHM of 37 nm (a reduction from 83 to 90 nm for conventional D–A counterparts based on spiro‑boron acceptor) and achieve a maximum EQE of 22.8%. This work demonstrates that integrating an MR donor into the spiro‑boron acceptor framework is a simple yet powerful approach to upgrade existing high-efficiency TADF systems into narrowband emitters for solution- processable OLEDs.
In recent years, exciplex systems composed of donor-acceptor pairs exhibiting thermally activated delayed fluorescence (TADF) have gained increasing attention in organic light-emitting diodes (OLEDs). Reported herein is a novel blue TADF emitter, BO-QAD, which contains 2,12-di-tert-butyl-5,9-dioxa-13b-boranaphtho[3,2,1-de] anthracene (BO) as donor with quinolino[3,2,1-de]acridine-5,9-dione (QAD) as acceptor. BO-QAD emits an intense blue emission at 455 nm and 465 nm in its toluene and film, characterized by a narrow full width at half maximum (FWHM) of 27 nm. A high photoluminescence quantum yield (Phi PL) of 84.2 % was obtained in mCP: (2.0 wt%) BO-QAD blend film. Quantum calculations and photophysical experiments confirmed its TADF properties. Employed it as an identical exciplex acceptor and matching it with various electron-donating emitters (DMAC-DPS, TCTA, TAPC, or m-MTDATA), yellow-green, yellow, orange-red, and near-infrared (NIR) exciplexbased solution-processed OLEDs have been demonstrated for the first time, and exhibiting emission peaks at 559, 579, 600, and 718 nm with FWHM values of 94, 100, 102, and 188 nm, respectively. A white OLED employing a CBP host matrix and a BO-QAD:m-MTDATA exciplex guest system, achieving a color rendering index (CRI) of 76 at CIE coordinates of (0.33, 0.34), values close to D65 white light standard. Furthermore, three near-white OLEDs were fabricated by the same BO-QAD:m-MTDATA exciplex guest but different host matrices, mCP, mCBP, and 26-DCzPPy. This work highlights the promising potential of using NIR and white OLEDs in display applications.
Organic single crystals (SCs) are promising candidates for high‐performance optoelectronic devices due to their high mobility of charge carriers and oriented alignment of transition dipole moments (TDMs). However, organic single‐crystal‐based light‐emitting diodes (SC‐based OLEDs) have until now struggled with poor device efficiency because of the lack of appropriate SC emitters; the integration of superior charge‐transport property and light‐emitting behavior into one single SC remains a great challenge. Here, two anthracene‐derivative SCs, 2,6‐di(6‐ tert ‐butylnaphthyl)anthracene (TBU‐DNA) and 2,6‐di(2‐naphthyl)anthracene (2,6‐DNA), are introduced into the construction of high‐efficiency SC‐based OLEDs. Through systematic investigations, rational crystal packing is revealed to play a critical role in tailoring the optoelectronic properties of SCs. Thanks to the slipped herringbone packing motif, TBU‐DNA SC is endowed with a higher photoluminescence quantum yield (PLQY) of 71.47%, an enhanced light‐outcoupling efficiency of 22.9%, and higher charge‐carrier mobility reaching up to 1.44 cm 2 V −1 s −1 along the crystal c ‐axis, which are all responsible for better electroluminescence (EL) performances of TBU‐DNA SC‐based OLEDs. By optimizing the device structure with a hole‐blocking layer (HBL), the external quantum efficiency (EQE) of TBU‐DNA SC‐based OLEDs is approaching 3.46%, which is one of the highest EQE values for those OLEDs based on the SC emitting layer (EML) reported so far.
The narrowband emission required by wide color gamut display is an extremely important research topic for any luminescence mechanism, which has made significant progress in traditional fluorescence and thermally activated delayed fluorescence (TADF) based on purely organic compounds, but is far from mature in phosphorescence based on metal organic complexes. Herein, we propose a feasible molecular design paradigm for constructing the desirable narrowband-emission organic electroluminescence (EL) emitter by integrating an original multi-resonance thermally activated delayed fluorescent (MR-TADF) fragment into the classical heavy metal platinum (II) complex. The target model platinum (II) complex BNCPPt shows green emission with a single peak at 497 nm and the quite narrow full-width at half-maximum (FWHM) of 27 nm in toluene.
In this study, amorphous WO3 thin films were deposited on indium-tin oxide substrates using radio frequency magnetron sputtering. Anhydrous ethanol (AE) and propylene carbonate (PC) served as binary solvents, with the WO3 films evaluated in AE + PC-LiClO4 electrolytes. By adjusting the volume percentage of AE, the physical properties of the electrolytes were modified to improve the fluidity and wetting behavior. The analysis of several aspects, such as migration of ions, capillary flow of electrolyte and electrochemical reaction rate, highlights the important influence of AE + PC binary solvent in reducing the response time. Notably, WO3 films in AE + PCLiClO4 electrolyte with a 7/8 volume percentage of AE demonstrated exceptional optical modulation (Delta T = 75.7 %) and fast response times (tc = 6.41 s, tb = 2.29 s), alongside shortened the diffusion path, increased ion diffusion coefficients (Da=4.4678 x 10-10 cm2/s, Dc = 8.2968 x 10-10 cm2/s) and electrochemical active area. Based on these efforts, the feasibility of applying AE + PC binary solvent to WO3 electrochromic thin films has been confirmed. These results offer valuable insights for the development of efficient electrolytes and their application in electrochromic devices.
Solution-processing phosphorescent organic light-emitting diodes (s-PhOLEDs) based on heavy metal complexes deliver simpler fabrication processes, lower production costs, and higher material utilization rates than thermal-evaporation phosphorescent OLEDs (t-PhOLEDs), making them a strong competitor in large-sized panel manufacturing. However, s-PhOLEDs face two significant challenges: low electroluminescence efficiency and large efficiency roll-off at high luminance. Herein, the design and synthesis of an orbitally symmetric octahedral metallophosphor iridium(III) complex (BNPPy)2-Ir-acac containing dual B,N-embedded multiple resonance emitters are reported. By blending emitter (BNPPy)2-Ir-acac in a p-n type premixed host, the doped film fabricated by spin coating has a photoluminescence quantum yield of 91% and a horizontal emitting dipole orientation ratio of 73%. The emitter (BNPPy)2-Ir-acac-based s-PhOLED exhibits yellow emission with a peak of 552 nm. The external quantum efficiencies (EQEs) are 27.8% and 32.9% at 100 and 1000 cd m-2, respectively; the EQE reaches a maximum of 33.2% at 2118 cd m-2; and the EQEs remain 28.5% and 24.9% at 5000 and 10 000 cd m-2, respectively.
Highly efficient blue phosphorescent solid supramolecular assemblies are constructed by three triazine derivatives with different carboxylate substitution positions (TAB, TAC and TAD), hydroxypropyl-beta-cyclodextrin (HPCD) and polyvinyl alcohol (PVA). The encapsulation of HPCD to TAB/C/D effectively promotes phosphorescence lifetimes and quantum yields of the guests by the host-guest interaction and hydrogen bonds suppressing the nonradiative decays. Impressively, TAD-HPCD/PVA with blue phosphorescence boasts an ultrahigh phosphorescence quantum yield (Phi(P)) of 71.65 %. By further separately doping with fluorescent dyes Fluorescein sodium, Rhodamine B and Sulfo-Cyanine5, supramolecular polymeric films with water responsiveness, regulable lifetimes and multicolor delayed fluorescence are obtained via triplet-to-singlet and singlet-to-singlet F & ouml;rster resonance energy transfer. Polymeric phosphorescence supramolecular materials mediated by HPCD are desirable for optical anti-counterfeiting patterns and information encryption.
A series of fluorinated pyrrole-derived thioamide ligands was synthesized via a solvent-free reaction of (substituted) pyrrole with various aryl isothiocyanates. Subsequent reactions of these ligands with cis-[PtCl2(PPh3)2] afforded a set of charge-neutral platinum(II) complexes, featuring a variety of fluorine-containing substituents on the phenyl ring of the ligand. All compounds were characterized by NMR spectroscopy and electrospray ionization-mass spectrometry. Single-crystal X-ray diffraction analysis of a representative complex revealed that the ligand coordinated to the platinum center in a bidentate fashion through the deprotonated pyrrole nitrogen and the sulfur atom of the thioamide group, forming a five-membered chelate ring. The antiproliferative activity of selected ligands and their corresponding Pt(II) complexes was evaluated against HCT116, NCI-H460, A2780, and A2780cis human cancer cell lines, and significantly increased potency was found for a Pt complex as compared to its ligand.
Adhesive conductive hydrogels have a broad application prospect in the field of flexible sensors, but existing adhesive hydrogels often struggle to balance adhesion performance and mechanical strength, and their adhesion stability is poor, which limits their long-term applications. In this study, a dual-network-structured hydrogel with durability, conductivity, and adhesion was prepared using a photoinitiated polymerization process, and its potential application in flexible sensors was explored. The hydrogel is based on thiosemicarbazone-modified chitosan (CS-SCM) as the backbone, introducing a reducible group into the system, acrylic acid (AA), tannic acid (TA), and Fe3+ are incorporated, endowing the hydrogel with excellent electrical conductivity and adhesion durability through multiple hydrogen bonds, electrostatic interactions, and metal-phenol complexation effects. The experimental results show that the hydrogel is able to maintain stable and long-lasting adhesion on the surface of various substrates, and its adhesion to plank remains above 90 kPa after 5 days of storage and more than 20 kPa after 13 days, which is significantly better than traditional hydrogels. Moreover, the durable adhesion of this hydrogel is highly valuable for research and applications in flexible sensors, smart wearables, and bioelectronic devices.
ABSTRACTOrganic single crystals with long‐range molecular periodic ordering ensure superior charge‐transport properties and low defect density, which have been considered promising candidates for charge‐transporting materials in organic light‐emitting devices (OLEDs). The functional interfaces of OLEDs play a critical role in charge‐transporting and light‐emitting behaviors, while the interfacial properties of organic single crystals in OLEDs and their impact on device performance have been rarely investigated. Herein, two typical organic single crystals, 1,4‐bis(4‐Methylstyryl)benzene (BSB‐Me) and 2,6‐diphenylanthracene (DPA) with different molecular formulas and packing structures, are introduced as the single‐crystal hole‐transporting layers (HTLs) for a systematic investigation of the interfacial properties between single‐crystal HTLs and active emissive layers. BSB‐Me single‐crystal HTLs offer satisfied surface wettability and enhanced interfacial interaction, which dominate the charge‐transporting and light‐emitting behaviors of the OLEDs. Such improved interfacial properties are responsible for the superior light out‐coupling efficiency of BSB‐Me single‐crystal OLEDs with efficient exciton recombination and minimal Joule heat loss. In consequence, BSB‐Me single‐crystal OLEDs exhibit a maximum luminance of 50,170 cd/m2 and a peak EQE of 8.78%, which are better than DPA‐based devices. Furthermore, BSB‐Me single‐crystal HTLs with favorable interfacial properties enable large‐area OLEDs with uniform EL emission over the whole light‐emitting area of 1 mm × 1 mm.