

Unlocking the Potential of Oxide‐Based Catalysts for CO2 Photo‐Hydrogenation: Oxygen Vacancies Promoted C─O Bond Cleavage in Key Intermediates
Structure-tailored Co3O4 is employed to investigate how oxygen vacancies perform during CO2 (photo-)methanation, revealing that oxygen vacancies boost the C─O bond scission, facilitating conversion of various oxygen-containing intermediates. Notably, the C─O bond cleavage in key intermediate formate, identified as the rate-limiting step, is accelerated on oxygen vacancy-rich M-Co3O4, leading to a high activity and selectivity in CH4 production.
Abstract
Oxygen vacancies are generally recognized to play significant roles in CO2 adsorption and activation during CO2 hydrogenation. However, by revisiting its structural/electronic affinity for a range of oxygen-containing intermediates in CO2 hydrogenation processes, the additional roles of oxygen vacancies can be long overlooked and underestimated. Herein, using CO2 (photo-)methanation as a model reaction, Co3O4 with abundant oxygen vacancies is employed to investigate the relationship between oxygen vacancies and the formation/conversion of oxygen-containing intermediates. Combined analyses of in situ diffuse reflectance infrared Fourier transform spectroscopy and theoretical calculations reveal that the key intermediate is formate, whose C─O bond cleavage is inferred to be the rate-limiting step during CO2 methanation on Co3O4. Remarkably, leveraging the oxygen vacancy-mediated C─O bond scission to accelerate the conversion of formate, the CH4 production activity (1108.1 mmol g−1 h−1) and selectivity (93%) are improved significantly. This comprehensive study provides valuable insights into the multifaceted roles of oxygen vacancies in CO2 hydrogenation reactions, establishing a solid foundation toward the design and development of high-performance oxide-containing/-based catalysts for the conversion of CO2 into various valuable chemicals.
One‐Step Symbiosis of Bimetallic Peroxides Nanoparticles to Induce Ferroptosis/Cuproptosis and Activate cGAS‐STING Pathway for Enhanced Tumor Immunotherapy
The designed zinc-copper bimetallic peroxides nanoparticles, which are synthesized through a one-step symbiotic method by co-hydrolysis of metal acetates, can release Zn2+, Cu2+, and H2O2 in TME to induce ferroptosis/cuproptosis and activate cGAS-STING pathway. Therefore, anti-tumor adaptive and innate immunotherapy can be simultaneously promoted to effectively inhibit tumor growth and metastasis with assistance of immune checkpoint inhibitor.
Abstract
To improve the efficiency and application prospects of metal peroxides in tumor therapy, the synthesis of bimetallic peroxides via simple yet effective approaches will be highly significant. In this work, hyaluronic acid modified zinc-copper bimetallic peroxides (ZCPO@HA) nanoparticles are synthesized through a one-step symbiotic method by co-hydrolysis of zinc acetate and copper acetate in weakly alkaline solution, followed by modification with sodium hyaluronate. Upon decomposition in the tumor microenvironment, ZCPO@HA nanoparticles can generate a considerable content of hydroxyl radical (·OH) by Fenton-like reaction between Cu2+ and self-compensating hydrogen peroxide, while downregulating the expression of glutathione peroxidase 4 to induce ferroptosis. The abundant release of Cu2+ leads to the aggregation of dihydrolipoamide S-acetyltransferase and the reduction of iron-sulfur cluster proteins, causing cuproptosis. The immunogenic cell death of tumor cells releases abundant damage associated molecular patterns, effectively activating the adaptive immune response. Zn2+ and ·OH cause mitochondrial damage, leading to the release of a substantial amount of mitochondrial DNA. This subsequently activates the cyclic guanosine monophosphate-adenosine monophosphate synthase-stimulator of interferon genes (cGAS-STING) pathway, enhancing the innate immune response. In conclusion, it synthesizes a new type of bimetallic peroxides by one-step symbiosis for activating anti-tumor immunotherapy combined with immune checkpoint inhibitor.
Low‐Temperature Pyrolysis: A Universal Route to High‐Loading Single‐Atom Catalysts for Fuel Cells
This work develops a molten salt strategy for synthesizing single-atom catalysts at 450 °C via LiCl/KCl-mediated Fe2+/Zn2+ exchange on nitrogen-doped carbon substrates. By stabilizing Fe2+ ions and suppressing the Fe-oxide nanoparticle formation—a common limitation in conventional high-temperature pyrolysis—it achieves a 3.9 wt.% Fe loading of atomically dispersed Fe-N4 sites, delivering superior H2—O2 fuel cell performance.
Abstract
High-temperature pyrolysis (HTP, ≥900 °C) is a widely used method for synthesizing single-atom catalysts (SACs). However, the high operational temperatures required for HTP pose significant challenges in achieving high single-atom loading, primarily due to the Ostwald ripening effect. In this work, a low-temperature trans-metalation synthesis approach is developed which involves the exchange of cation between transition metal ions (M = Fe, Co, Cu, Ni, Mn, etc) and Zn2+ ions on a nitrogen-doped carbon (NC) matrix within a molten salt medium. This strategy effectively avoids phase transformations and enables the direct formation of high mass loading (3.7–4.7 wt.%) of atomically dispersed M-N4 sites. Both experimental and theoretical analyses confirm that this cation-exchange occurs at a lower temperature threshold of 450 °C, significantly reducing the energy barriers for SACs synthesis. Furthermore, the synthesized catalyst with atomically dispersed Fe sites demonstrate excellent performance toward oxygen reduction reaction and fuel cell with a peak power density of 1.12 W cm−2 in an H2─O2 fuel cell at 1.0 bar and 80 °C.
Carbon Dot‐Linked Hydrogel for TAMs Transform: Spatiotemporal Manipulation to Reshape Tumor Microenvironment
The CDs crosslinked egg white hydrogel loaded with lipopolysaccharide (LPS) and CA170 (TTF-L-C) can realize spatiotemporal tumor-associated macrophages (TAMs) transformation from multi-level dimensions, including spatial recruitment, cell phenotype reprogramming, and immune checkpoint molecule blockade. Finally, at the in vivo level, TTF-L-C can stimulate anti-tumor immunity through tumor microenvironment (TME) remodeling and reduce tumor recurrence with satisfactory biosafety.
Abstract
As one of the most crucial immune cells in the tumor microenvironment (TME), regulating tumor-associated macrophages (TAMs) is vital for enhancing antitumor immunity. Here, an injectable carbon dots (CDs)-linked egg white hydrogel was developed, termed TAMs Transform Factory (TTF-L-C), to spatiotemporally manipulate TAMs. The fabricated CDs significantly promoted macrophage migration. Notably, TTF-L-C achieved macrophage spatial enrichment through CDs-induced directional recruitment with molecular Ctnnd1 upregulation. Subsequently, the recruited macrophages were locoregionally reprogrammed within TTF-L-C, as well as blocking the upregulated PD-L1. Finally, through multi-stage regulation at spatial, cellular, and molecular levels, TTF-L-C released immune-activated M1 macrophages to the tumor site as it degraded. Moreover, TTF-L-C promoted dendritic cell (DCs) maturation and further boosted T cell activation, thereby reshaping the tumor-suppressive TME. Through peritumoral injection, TTF-L-C enhanced tumor immunotherapy in both subcutaneous and recurrent 4T1 tumor models with satisfactory biosafety. Therefore, TTF-L-C is proposed to become a safe and powerful platform for various biomedical applications.
High‐Performance Carbon Capture with Fluorine‐Tailored Carbon Molecular Sieve Membranes
A high-performance carbon capture using fluorine-tailored carbon molecular sieve (CMS) membranes is developed. By incorporating bent terphenyl monomers and both aliphatic/aromatic trifluoromethyl groups into the polymer precursor, the derived CMS membranes achieve exceptional CO₂ permeability of 47,190 Barrer and CO2/N2 selectivity of 28.3, maintaining 36,204 Barrer permeability and 35.3 selectivity under flue gas conditions.
Abstract
Increasing energy consumption and climate change present an urgent global challenge to achieve carbon neutrality, with CO2 capture as a top priority. Among various carbon capture technologies, CO2 membrane separation stands out for its simplicity and energy efficiency in applications including gas purification and industrial gas recovery. Herein, a series of fluorine-tailored porous carbon molecular sieve (CMS) membranes derived from precisely designed precursors, achieving a well-balanced high permeability and selectivity for CO2 separation are developed. Incorporating bent terphenyl monomers and both aliphatic/aromatic trifluoromethyl groups disrupted dense chain packing and promoted pore formation with enhanced permeability and selectivity for CO2 separation. The TFM-550 membrane, derived from a fluorinated stretched polymer backbone precursor, exhibits exceptional performance with a CO2 permeability of 47 190 ± 3204 Barrer and a CO2/N2 selectivity of 28.3 ± 5.7, while TFM-800 presented a higher selectivity of 71.8 ± 11.5, surpassing the 2019 upper bound. Furthermore, under flue gas conditions (CO2/O2/N2 = 1/1/4 in molar ratio), the CMS membrane demonstrate high CO2 permeability of 36,204 ± 2,235 Barrer and outstanding CO2/N2 selectivity of 35.3 ± 1.8. The results here highlight the effectiveness of fluorine tailoring and the potential of fluorinated CMS membranes for sustainable industrial carbon capture applications.
Interlayer Expanded MXene Film Cathodes with Rich Defects for Flexible 2‐Electron Oxalate‐Based Li–CO2 Batteries: A New Path to Enhanced Energy Efficiency and Durability
A defect-rich, interlayer-expanded MXene (Ex-Ti3C2T x -3) film cathode, with abundant uncoordinated titanium atoms, stabilizes the bi-electron pathway in Li–CO2 batteries, improving energy efficiency and durability. Its extended interlayer spacing and mesoporous structure enhance ion and CO2 transport, and the surface functionalization suppresses interfacial oxidation and maintains integrity. The battery achieves low polarization (0.39 V), high capacity (3452.33 µAh cm−2), and long life (>1660 h). The foldable Ex-Ti3C2T x -3 cathode enables flexible Li–CO2 batteries, offering potential in wearable electronics.
Abstract
Aprotic Li–CO2 batteries have garnered significant attention owing to their high theoretical energy density and potential in zero-carbon technology. However, their practical application remains hindered by sluggish CO2 reduction/evolution reaction (CRR/CER) kinetics and limited flexibility. While 2D graphene-like materials are commonly employed to settle these issues, their four-electron pathway limits efficiency and reversibility. Herein, a defect-rich, interlayer-expanded Ti3C2T x (Ex-Ti3C2T x ) film cathode is presented for flexible Li–CO2 batteries. The extended interlayer space, reduced ─OH groups, and additional uncoordinated titanium atoms of Ex-Ti3C2T x enable abundant catalytic active sites, enhance ion and CO2 transport, and these surface functionalizations suppress interfacial oxidation. Notably, Ex-Ti3C2T x stabilizes the bi-electron product Li2C2O4 via Ti3+/Ti2+ coupling bridges, effectively preventing disproportionation into Li2CO3, thereby significantly improving CRR/CER reversibility and lowering overpotential. Benefiting from these properties, Li–CO2 batteries with Ex-Ti3C2T x deliver a remarkable discharge capacity of 3452.33 µAh cm−2, a low polarization potential of 0.39 V, an energy efficiency exceeding 88.9%, and an ultra-long cycling life (>1600 h). Furthermore, the belt-shaped flexible battery exhibits excellent flexibility and stable electrochemical performance under deformation highlighting its potential in wearable electronics. This work underscores the critical role of MXene-based materials in bi-electron electrocatalytic mechanisms, providing insights for advancing reversible Li–CO2 batteries and flexible energy storage technologies.
Advanced Air Electrodes for Reversible Protonic Ceramic Electrochemical Cells: A Comprehensive Review
Reversible protonic ceramic electrochemical cells (R-PCECs) face challenges from sluggish and unstable oxygen reduction and evolution reactions in the air electrode. This review discusses recent progress in triple-conducting air electrodes, emphasizing mechanisms, performance factors, and design strategies, offering guidance for creating efficient and stable air electrode materials for R-PCECs.
Abstract
Reversible protonic ceramic electrochemical cells (R-PCECs) have great potential for efficient and clean power generation, energy storage, and sustainable synthesis of high-value chemicals. However, the sluggish and unstable kinetics of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in the air electrode hinder the R-PCEC development. Durable H+/e−/O2− triple-conducting air electrode materials are promising for enhancing reaction kinetics and improving catalytical stability. This review synthesizes the recent progress in triple-conducting air electrodes, focusing on their working mechanisms, including electrode kinetics, lattice and its defect structure in oxides, and the generation and transport processes of H+, O2−, and e−. It also examines the required physicochemical properties and their influencing factors. By synthesizing and critically analyzing the latest theoretical frameworks, advanced materials, and regulation strategies, this review outlines the challenges and prospects shaping the future of R-PCEC technology and air electrode development. Based on these theories and multiple strategies about the bulk triple conducting properties and surface chemical states, this review provides practical guidance for the rational design and development of efficient and stable air electrode materials for R-PCECs and related electrocatalytic materials.
Suppression of Charge Recombination Induced by Solid Additive Assisting Organic Solar Cells with Efficiency over 20%
The work highlights the strong morphological optimization capacity of the solid additive DIDOB and elucidates its impact on molecular packing to suppress both bimolecular and geminate recombination in OSCs. As a result, DIDOB not only demonstrates universality in various non-fullerene-based OSCs but also achieves an impressive efficiency of 20.11% with a remarkable fill factor of 81.8% in the D18:PM6:L8-BO-based device.
Abstract
A volatile solid additive strategy, which can effectively optimize the morphology of the photoactive layer with an ideal domain size and purity, has emerged as a promising approach to improve the photovoltaic performance of organic solar cells (OSCs). However, the precise role of solid additives in modulating charge and exciton dynamics, especially the recombination process, remains not fully understand. In this study, a solid additive, 1,4-diiodo-2,5-dimethoxybenzene (DIDOB), is developed to improve the photovoltaic performance of OSCs and conduct a comprehensive investigation into its effect on the charge recombination process. As a result, the PM6:L8-BO-X-based binary OSC processed with DIDOB achieves an excellent efficiency of 19.75% with a remarkable fill factor of 81.9%, owing to the optimal fiber network morphology, tighter and ordered molecular packing, as well as the suppression of both bimolecular and geminate recombination. Notably, the DIDOB exhibits broad universality as an additive in other non-fullerene acceptor-based OSCs. Impressively, the D18:PM6:L8-BO-based ternary device processed with DIDOB yielded an excellent efficiency of 20.11% (certified as 20.03%). This work highlights the effect of the solid additive on the charge recombination process within active layer and provides insights for the further development of OSCs.
Decoupling Strategy of Metasurface to Realize Independent Sensing and Wave Manipulations at the Same Time
In this article, a decoupling strategy of metasurface to realize independent sensing and wave manipulations at the same time is proposed. By allocating the reflectivity of all meta-atoms across the space-time dimensions, it is possible to realize arbitrary manipulation of electromagnetic waves while simultaneously sensing the wireless environment by the metasurface without integrating any sensors. An adaptive STCDM system is constructed and measured, showing excellent performances of sensing and wave manipulations in wireless communication scenarios.
Abstract
In recent years, integrating electromagnetic (EM) sensing and wave manipulation has become crucial for future wireless developments, significantly enhancing the application performance by acquiring complex environmental information and optimizing the distribution of EM resources. Metasurface offers unprecedented control over sensing and wave manipulation, yet a conflict arises in achieving both simultaneously. To solve the problem, a decoupling strategy is proposed to simultaneously realize sensing and wave manipulation using a space-time-coding digital metasurface (STCDM) without integrating any sensors. A space-time-coding matrix is constructed by allocating the reflectivity of all meta- atoms across the space-time dimensions, enabling arbitrary manipulation of EM waves while simultaneously acquiring the sensing information at the incident frequency from metasurface. Excellent accuracy of direction-of-arrival estimation and wave manipulation confirms the decoupling method. An adaptive STCDM system is built up to validate the strategy in wireless communications. The measured results show that the adaptive STCDM enables independent sensing and wireless communications at the same time for targets located at different positions without integrating any sensors. The proposed method may find potential applications in wireless communication, radar, and Internet of Things systems.
Nonlinear Optical Properties of 0D Chiral Hybrid Bismuth Iodides
Optically stable lead-free 0D chiral (R/S-methyl-benzyl-amine)-bismuth-iodide crystals showcase promising second and third-order nonlinear optical properties. The chiral compounds show significant circularly polarized second harmonic generation. The achiral counterpart exhibits the most efficient third-order optical nonlinearity.
Abstract
Chiral hybrid metal halides show great promise for nonlinear optical (NLO) applications like circularly polarized second harmonic generation (SHG). The inherent toxicity of lead is a concern for the widespread adoption of frequently explored lead-based chiral hybrid halides. Here, we report the second and third-order NLO properties of lead-free 0D chiral compounds, (R-/S-MBA)4Bi2I10, and their achiral counterpart, (Rac-MBA)4Bi2I10 (MBA: methylbenzylammonium) under excitation wavelength ranging 1360–1590 nm. Chiral (R-/S-MBA)4Bi2I10 exhibits strong SHG along with stronger third harmonic generation (THG). The chiral crystals showed high sensitivity to the handedness of circularly polarized pump light (g SHG − CD ≈ 9% at 1510 nm). The THG response shows resonance enhancement matching the excitonic absorption. Achiral (Rac-MBA)4Bi2I10 exhibits the maximum THG response (χ(3) = 1.05 × 10⁻¹⁸ m2 V− 2). Z-scan measurements with non-resonant femtosecond pulse excitation at 800 nm yield high nonlinear absorption coefficients (β) and nonlinear refractive index (n2) for all three samples, with (Rac-MBA)4Bi2I10 exhibiting the highest values. These hybrid chiral metal halides, with efficient second and third-order nonlinearity, and high optical stability, are potential candidates for NLO applications such as Kerr-based optical switching, circularly polarized up-conversion, and communication.
Simultaneously Tailoring Hydrostability and Photoelectroactivity in Heterocluster Metal–Organic Frameworks for Efficient Photocatalytic Hydrogen Production
The first heterocluster-based crystalline MOF photocatalysts integrating copper-sulfur and copper-halide clusters are obtained through the heterocluster assembly engineering and localized microenvironment regulation, demonstrating an unprecedented synergistic enhancement of hydrostability and photoelectroactivity, facilitating the efficient synthesis of green hydrogen at an exceptionally high rate under visible light.
Abstract
The simultaneous enhancement of structural stability and photoelectroactivity in metal-organic frameworks (MOFs) remains a critical challenge for sustainable photocatalytic hydrogen (H2) production. Herein, an atomically-precise heterocluster assembly approach is presented to construct two isostructural 3D MOFs, CuSL-CuX (X = Cl, Br), featuring a cds net. CuSL-CuXs integrate hexanuclear copper-sulfur {Cu6S6} cluster and dinuclear copper-halogen {Cu2X2} cluster, which not only impart exceptional stability across a broad pH range (1–14) but also enable wide visible-light absorption, tailored redox potentials, and efficient charge-carrier dynamics. Notably, halogen substitution markedly boosts photocatalytic activity: CuSL-CuBr achieves an efficient H2 evolution rate of 50.28 mmol g−1 h−1 without noble metals, doubling that of CuSL-CuCl (26.99 mmol g−1 h−1) and surpassing most reported MOF-based photocatalysts. Both experimental and theoretical investigations indicate that bromine substitution optimizes electronic structure, refines orbital distribution, and accelerates charge separation, ultimately leading to promoted photocatalytic efficiency. This research provides insights into the structure-property interplay in heterocluster MOFs and establishes a paradigm for designing robust, high-performance photocatalysts through precise cluster engineering.
Tailoring Synergistic Ion Environment for Copper Telluride toward High‐Capacity and Ultrastable Acidic Multivalent‐Ion Batteries
Cu2-xTe electrodes are disclosed in acidic multivalent-ion batteries for the first time to achieve a high capacity of up to 409 mAh g−1 and a long cycling lifespan of 40 000 cycles. Composite in situ X-ray diffraction measurements and spectroscopic analyses show that the synergistic copper-ion/proton electrolyte environment ensures stable reversible storage of copper-ions and prevents potential material oxidation.
Abstract
Acidic batteries permit a reliable energy supply at low temperatures with low cost and intrinsic safety, yet the development of stable acid-resistant electrodes with high capacity and a reliable lifespan is still challenging. Herein, nonstoichiometric copper telluride (Cu2-xTe) nanosheets are first explored as high-performance electrodes for acidic batteries to provide a stable capacity release of 409 mAh g−1 with a record-breaking lifespan of 40 000 cycles and excellent kinetics, enabling operation at a high current density of 20 A g−1. In contrast to the inherent perception of corrosive destruction of electrode materials by strongly acidic environments, the electrolyte environment enriched with copper ions and hydrogen ions synergistically stabilizes the Cu2-xTe electrode and drives reversible multielectron transfer asymmetric deep conversion, which is confirmed by in situ synchrotron X-ray diffraction, X-ray absorption spectroscopy, first-principal calculations, and composite electrochemical characterization. Therefore, Cu2-xTe provides an impressive accumulation capacity of over 4764 Ah g−1, exceeding that of most acidic batteries, and works well at −20 °C. High-performance Cu2-xTe electrodes also promote the establishment of Cu2-xTe//Mn2O3 and Cu2-xTe//Fe acidic full cells enabling stable operation at room temperature and low temperature, offering promising opportunities for electrode progress in advanced acidic batteries.
Harnessing Near‐Infrared Light for Enhanced Solar Hydrogen Production from Escherichia coli Interfaced with Biocompatible Low‐Bandgap Conjugated Polymer Nanosheets
Biocompatible, low-bandgap conjugated polymer nanosheets are interfaced with non-photosynthetic and non-genetic engineered Escherichia coli for solar hydrogen production using near-infrared light. The rationally designed polymer nanosheets play a crucial role in harnessing the broad solar spectrum and injecting photo-generated electrons into bacteria, thereby enhancing hydrogen production.
Abstract
The efficient conversion of solar energy into clean hydrogen fuel presents a promising pathway for sustainable energy production. However, utilizing the full solar spectrum, particularly the near-infrared (NIR) region, remains underexplored in photosynthetic biohybrid systems. In this study, biocompatible, low-bandgap conjugated polymer nanosheets (PyTT-tBAL-HAB) are developed to integrate with non-photosynthetic, non-genetically engineered Escherichia coli (E. coli) for enhanced solar-driven biological hydrogen production. The PyTT-tBAL-HAB nanosheets exhibit unique NIR light absorption properties. Integrating these nanosheets with E. coli facilitates efficient electron transfer, resulting in a 1.96-fold increase in hydrogen production rate under NIR light. Consequently, this photosynthetic biohybrid system achieves a quantum efficiency of 18.36% at 940 nm. This study demonstrates the potential of using low-bandgap conjugated polymer nanosheets as advanced photosensitizers in semi-artificial photosynthetic systems, offering a robust platform for the effective utilization of the solar spectrum.
Azepination‐Induced Frontier Molecular Orbital Delocalization of Multiple Resonance Emitters: Constructing Highly Efficient Narrowband Electroluminescent Materials
A strategy for azepination-induced frontier molecular orbital (FMO) delocalization of multiple resonance (MR) emitters is proposed to construct long-wavelength MR materials. Organic light-emitting diode based on m-PAz-BNCz exhibits excellent electroluminescence performances with Commission Internationale de L'Eclairage coordinates of (0.26, 0.70) and a maximum external quantum efficiency of 36.2%.
Abstract
Developing diversified construction strategies for high-color-purity and efficient multiple resonance thermally activated delayed fluorescence (MR-TADF) materials is a major strategic demand to meet the requirements of ultra-high-definition organic light-emitting diode (OLED) displays, posing a significant challenge to the design and synthesis of emitters at the molecular level. Herein, a strategy is proposed for azepination-induced frontier molecular orbital (FMO) delocalization of MR emitters, that is, embedding azepine into the prototype molecule BNCz can effectively improve the π-conjugation degree and extend the FMO delocalization, thereby constructing a series of long-wavelength MR-TADF materials with narrowband emission. Through an intramolecular Scholl reaction, these target molecules with an azepine-embedded core are afforded by one-fold heptagonal cyclization of BNCz core and the phenyl ring attached to (aromatic amine-substituted) aryl precursor. They all exhibit efficient green emission around 520 nm and narrow full-widths at half-maximum (FWHMs) of ≤ 37 nm in toluene. OLEDs employing these emitters show excellent electroluminescence (EL) performances, among which m-PAz-BNCz-based OLED exhibits the optimal EL performances with a peak of 528 nm, a FWHM of 37 nm, Commission Internationale de L'Eclairage (CIE) coordinates of (0.26, 0.70), and a maximum external quantum efficiency (EQE) of 36.2%.
Europium(II) Complex with d‐f Transition: New Emitter for Blue Light‐Emitting Electrochemical Cells with an External Quantum Efficiency of 19.8%
A lanthanide Eu(II) complex is demonstrated as an emitter in light-emitting electrochemical cells (LECs) for the first time. The bis[hydrotris(3-tert-butylpyrazolyl)borate]europium(II) complex based LEC achieved a record-breaking external quantum efficiency of 19.8% with Commission Internationale de L'Eclairage coordinates of (0.12, 0.18).
Abstract
Light-emitting electrochemical cells (LECs) have good prospects in the solid-state lighting field due to their simple single-layer structure and low manufacturing cost. However, the lack of high-efficiency blue LECs limits their development and further application. To solve this problem, many luminescent materials with various mechanisms such as fluorescence, phosphorescence, and thermally-activated delayed fluorescence are studied as emitters in LECs. Besides these materials, herein lanthanide europium(II) (Eu(II)) complex with d-f transition is demonstrated as a new type of emitter for LECs. In detail, a blue emitting Eu(II) complex bis[hydrotris(3-tert-butylpyrazolyl)borate]europium(II) is dispersed into 9-(3-(triphenylsilyl)phenyl)-9H-3,9′-bicarbazole host and tetrahexylammonium tetrafluoroborate electrolyte to make a blend film, which attains a high photoluminescence quantum yield of ≈100%. The LEC using the blend film as an active layer achieves a blue emission with Commission Internationale de L'Eclairage coordinates of (0.12, 0.18) and a record-breaking external quantum efficiency of 19.8%, corresponding to an exciton utilization efficiency of ≈100%. This work reveals that Eu(II) complex with d-f transition is a promising emitter toward high-performance blue LECs, which can inspire further research on Eu(II) complex based LECs.
Correction to “Multifunctional Copper‐Phenolic Nanopills Achieve Comprehensive Polyamines Depletion to Provoke Enhanced Pyroptosis and Cuproptosis for Cancer Immunotherapy”
Robust Homogeneous Segmented Power Generator Driven by Sb2Te3‐Based Thermoelectrics
The Cd–S co-alloying-induced microstructural evolution enables high-performance Sb2Te3-based thermoelectrics. Subsequently, an innovative full-scale Bi–Sb–Te segmented power generator is fabricated, extending the operational range of conventional Bi2Te3-based modules from 500 to 650 K and achieving an exceptional efficiency of 9.3% under a distinct ΔT = 350 K. Notably, it exhibits remarkable stability after 80-cycle thermal shock and 160-h thermal durability, highlighting great potential for low-grade waste heat recovery.
Abstract
Thermoelectric (TE) technology offers a promising solution for waste heat recovery, particularly in applications involving abundant low-grade heat (<650 K). However, for over half a century, TE power generators have predominantly relied on Bi2Te3 alloys with limited efficiencies below 7%. Herein, Cd and S are doped into Sb2Te3 to promote microstructural regulation characterized by dense twin boundaries and dislocations, resulting in a 45% reduction of lattice thermal conductivity at 300 K. Combined with the optimized density-of-states effective mass and expanded band gap, the Cd0.04Sb1.96Te2.94S0.06 sample attains a peak ZT of 1.1 at 650 K and an average ZT of 1.0 from 500 to 650 K, while exhibiting remarkable compressive and bending strengths of 197 and 56 MPa. Most importantly, a well-designed, homogeneous segmented TE power generator, constructed entirely from Bi–Sb–Te alloys, achieves a remarkable efficiency of 9.3% under a temperature gradient of 350 K, as certified by third-party validation. This work provides new insights into extending the operation temperature of Bi2Te3, demonstrating great potential for low-grade waste heat harvest.
Designing Cellulose Triacetate‐Based Universal Binder for High‐Voltage Sodium‐Ion Battery Cathodes with Enhanced Ionic Conductivity and Binding Strength
Cellulose triacetate-based binder with broad compatibility, high ionic conductivity, and superior binding strength has been successfully designed and validated through its application in high-voltage polyanionic cathodes (Na3V2(PO4)2O2F), layered oxide cathodes (NaNi1/3Fe1/3Mn1/3O2), and tunnel-type oxide cathodes (Na0.61[Mn0.27Fe0.34Ti0.39]O2). This work presents a sustainable and effective strategy for achieving high-performance sodium-ion batteries.
Abstract
Binders play a pivotal role in the performance of sodium-ion battery (SIB) cathodes, but traditional binders often struggle to balance broad compatibility, high ionic conductivity, superior binding strength, and environmental sustainability. In this study, a universal cellulose triacetate (TAC)-based binder (TAC-MMT) composed of TAC and natural montmorillonite (MMT) is designed to facilitate rapid Na+ transport pathways and establish a robust hydrogen-bonding network. This innovative TAC-MMT binder features a unique chemical structure that achieves high ionic conductivity through a self-enrichment and fast-transport mechanism, while its superior binding strength is attributed to hydrogen-bonding crosslinks between proton acceptors (C═O) in TAC and proton donors (−OH) in MMT. More importantly, the outstanding solubility and film-forming properties of TAC-MMT contribute to stable electrode protection and broad compatibility with high-voltage SIB cathodes. Benefiting from these advantages, the Na3V2(PO4)2O2F (NVPOF) electrodes with the TAC-MMT binder demonstrate exceptional performance, including a high capacity retention of 95.2% over 500 cycles at 5C and a rapid rate response of up to 15C. The versatility of the TAC-MMT binder is further confirmed with high-voltage NaNi1/3Fe1/3Mn1/3O2 and Na0.61[Mn0.27Fe0.34Ti0.39]O2 cathodes. This study highlights the potential of biomass-based binders as a sustainable and effective solution for advancing high-performance sodium-ion batteries.
Multiple Functional Engineering Strategies and Active Site Identification in Ru‐Based Electrocatalysts for Catalytic Conversion Reactions
This review provides a comprehensive analysis of engineering modification strategies for ruthenium (Ru)-based catalysts, highlighting their critical role in optimizing electronic structures and surface properties to enhance electrocatalytic conversion. Furthermore, it emphasizes the integration of multiple engineering strategies aimed at improving catalytic performance, while also addressing key commercialization challenges.
Abstract
Electrochemical conversion has been regarded as an ideal technology for achieving clean and sustainable energy, showing significant promise in addressing the increasingly serious energy crisis and environmental pollution. Ru-containing electrocatalysts (RUCE) outperform other precious metals due to elevated intrinsic activity and superior cost-effectiveness, developing into a promising candidate for electrochemical conversion reactions. A significant challenge in the field of catalyst discovery lies in its heavy reliance on empirical methods, rather than approaches that are rooted in rational design principles. This review first concentrates on the catalytically active sites and critical factors governing catalytic activity and performance durability. Then, a comprehensive summary of multifunctional modification strategies ranging from nanoscale to atomic scale is explored to control the structure and improve the performance. By unveiling the roles of each component in the modified RUCE at the atomic level, their intrinsic active sites are identified and discussed to establish the structure-performance relationship of the catalysts. Finally, the challenges and perspectives of Ru-based materials for electrochemical hydrogen, oxygen, and nitrogen conversion reactions are presented to inspire further efforts toward understanding RUCE to meet the ever-growing demand in the future.
Electrochemical Lattice Engineering of Bismuthene for Selective Glycine Synthesis
A Bi-based catalyst is developed via the electrochemical transformation of bismuth-oxide composites, inducing enhanced lattice strain to optimize catalytic performance. At an applied potential of −0.76 V versus RHE, the catalyst exhibits outstanding efficiency in glycine electrosynthesis, achieving a Faradaic efficiency (FE) of 79.1% and a record-high glycine concentration of 0.17 m, significantly outperforming conventional Bi-based systems. Moreover, the introduction of glycolaldehyde and hydroxylamine as reactants further elevate the glycine FE to 91.3%, with an impressive production rate of 2433.3 µmol h−1 under identical conditions.
Abstract
Glycine plays a crucial role in various industrial and daily applications. However, traditional synthesis methods are often associated with high toxicity, energy intensity, and inefficiency. This study introduces an efficient and eco-friendly method for synthesizing glycine via the reductive coupling of oxalic acid and nitrate using a Bi metal catalyst, enhanced by lattice strain from Bi and oxide composites undergoing electrochemical transformation. At an applied potential of −0.76 V versus the reversible hydrogen electrode (RHE), the Bi catalyst achieves an impressive glycine Faradaic efficiency (FE) of 79.1%, yielding a record concentration of 0.17 m, substantially higher than conventional Bi-based systems. Furthermore, the introduction of glycolaldehyde and hydroxylamine as reactants raise the glycine FE to 91.3% with a production rate of 2433.3 µmol h−1 under identical conditions. Electrochemical analysis and theoretical calculations demonstrate that lattice expansion notably boosts glycine synthesis by facilitating NH2OH formation and promoting the efficient reduction of oxime intermediates. These results underscore the significance of lattice engineering in enhancing active site performance and accelerating reaction kinetics, offering a sustainable and efficient alternative to traditional glycine synthesis methods.