The cycloaddition of CO2 with epoxides proceeds with 100% atom economy, making it a particularly attractive route for CO2 chemical conversion. However, the chemical inertness of CO2 demands the design of highly active catalysts. In this work, a task-specific imidazolium ionic liquid [BBDCMIM]Br, bearing two carboxyl groups on the imidazolium ring, was synthesized via quaternization. Subsequently, post-synthetic grafting of [BBDCMIM] Br with different loadings onto UiO-66-NH2 support was achieved through nucleophilic substitution reaction between the alkyl bromide in [BBDCMIM]Br and-NH2 in UiO-66-NH2, affording [BBDCMIM]Br-x/UiO-66-NH2 (x = 1-3) catalysts. Among them, [BBDCMIM]Br-2/UiO-66-NH2 demonstrated outstanding catalytic activity under conditions of 100 degrees C, 1.0 MPa and 6 h, delivering 97% propylene carbonate yield with 99% selectivity. In addition, [BBDCMIM]Br-2/UiO-66-NH2 exhibited excellent recyclability and broad substrate scope. Kinetic studies indicated that the activation energy of the [BBDCMIM]Br-2/UiO-66-NH2-catalyzed CO2 cycloaddition was 60.97 kJ & sdot;mol-1. Finally, a reasonable mechanism was put forward for [BBDCMIM]Br-2/UiO-66-NH2. In this mechanism, the coordinatively unsaturated Zr metal centers acted as Lewis acidic sites and-COOH groups served as hydrogen bond donors, collectively activating the epoxide. The Br-then acted as a nucleophile to promote epoxide ring-opening. Meanwhile, the formed secondary amine (derived from partial-NH2 conversion) on UiO-66-NH2 and the tertiary amine in [BBDCMIM]Br served as basic sites and facilitated the activation of CO2. Overall, [BBDCMIM]Br-2/UiO-66-NH2 is a potential catalyst for sustainable conversion of CO2 into cyclic carbonates.

ABSTRACT Hydrogen energy, celebrated for its high energy density and zero carbon emissions, is widely regarded as an indispensable pillar of 21 st ‐century green energy systems. Against this backdrop, transition metal phosphides (TMPs) have attracted considerable attention due to their distinctive physicochemical properties when applied in electrochemical water splitting (EWS). Nevertheless, their intrinsic activity remains limited by the suboptimal adsorption energetics of reaction intermediates, high kinetic barriers for water dissociation, and often lengthy or energy‐intensive synthesis protocols. This review begins with a concise overview of microwave‐assisted synthesis, a rapid, energy‐efficient, and highly controllable strategy for material fabrication. Then, we provide a comprehensive introduction to the rational design of TMP‐based electrocatalysts through diverse modification strategies, with particular information on their dynamic electrochemical reconstruction behavior under operational conditions. Special focus is placed on advanced engineering approaches that enable scalable, efficient hydrogen production by integrating advanced techniques powered by renewable sources. The final section highlights recent application advances, ongoing challenges, and emerging opportunities for TMP electrocatalysts within the evolving landscape of next‐generation energy structure. Collectively, this review provides a comprehensive summary of precisely engineered TMP electrocatalysts with reconstruction behavior that functions as high‐performance bifunctional electrocatalysts for EWS‐based renewable energy generation.

Designing sustainable and surface-active carbon catalysts for efficient two-electron oxygen reduction (2e(-) ORR) requires precise control over interfacial chemistry and defect architecture. Current methods, however, rely on corrosive chemical oxidation or complex multi-step processes that degrade structural integrity. Herein, we propose a folic acid assisted surface reconstruction strategy to engineer oxygen/nitrogen co-functionalized carbon nanotubes (O-CNTs) through one-step green pyrolysis. Unlike conventional acid treatments, this approach leverages folic acid's thermally stable heterocyclic framework to synchronously graft oxygen functional groups (C=O/C-OH) and N dopants onto defective CNT surfaces, achieving defect property balance between catalytic activity and conductivity. The resulting O-CNTs exhibit an exceptional H2O2 selectivity (89 % at 0.5 V vs. RHE) and durability (95 % current retention over 50 h) in alkaline media, outperforming analogues crafted by HNO3 oxidation or plasma etching. Systematic characterization reveals that enhancing H2O2 selectivity correlates with folic acid-derived N/O co-doping, specifically through synergistic modulation of pyrrolic-N content (57.6 %) and electrophilic CO groups (32.1 %). While multiple defect types coexist, our control experiments using non-functionalized templates and molecular analogues (e.g., glucose/citric acid) indicate that O/N co-doping dominates the activity enhancement, contributing >85 % selectivity gains. This synergistic mechanism provides a versatile design strategy for sustainable H2O2 electrosynthesis.

ABSTRACT Methane, the most stable alkane, is significantly more stable than its partial oxidation products. This renders the highly selective conversion of CH 4 to CH 3 OH an extremely intractable challenge, especially when using molecular oxygen as the oxidant. In this work, we synthesized a bimetallic‐modified zeolite composite catalyst (PdCo bimetallic nanoclusters supported on H‐ZSM‐5 molecular sieve, denoted as PdCo@H‐ZSM‐5) via a simple impregnation method. PdCo@H‐ZSM‐5 can efficiently activate H 2 and O 2 to highly selectively oxidize CH 4 to CH 3 OH under mild conditions (70°C), achieving a remarkable CH 3 OH yield of 2349 µmol g cat −1 h −1 (249 mmol g Pd −1 h −1 ). Significantly, PdCo@H‐ZSM‐5 is the sole catalyst reported to date that can achieve over 99% CH 3 OH selectivity in the oxidation of CH 4 by molecular oxygen under mild conditions. This work is expected to inspire new technologies for industrial CH 4 to CH 3 OH conversion, promoting more sustainable chemistry and engineering. Furthermore, the low‐energy consumption, high‐efficiency activated oxygen catalyst eliminates the necessity for transporting and storing highly concentrated hydrogen peroxide, serving as a foundation for other green oxidation reactions.

The electrosynthesis of 2,5-furandicarboxylic acid (FDCA), a renewable polymer monomer for degradable plastics, represents a promising strategy for biomass upgrading, yet remains fundamentally limited by the challenge of accommodating diverse reaction intermediates involved in the multi-electron oxidation of 5-hydroxymethylfurfural (HMF). Here, we demonstrate that facet-controlled orbital-degeneracy-driven spin regulation in spinel NiCo2O4 offers an effective strategy to accelerate the electrosynthesis of FDCA. The exposed (110) facet modifies the orbital splitting of active-site Co and leads to a lifted Co 3d orbital degeneracy with a moderate-spin-associated electronic configuration. This electronic structure balances the adsorption-desorption behavior of key intermediates and lowers the overall reaction barrier. Such a design enables complete HMF conversion with a 99.9% yield for FDCA, while an integrated NiCo2O4 nanoarrays electrode with exposed (110) facets delivers Faradaic efficiencies of similar to 94% under industrial-level current densities, underscoring their scalability. These results establish a mechanistic framework for orbital-spin engineering in electrocatalyst design, offering broad implications for accelerating complex multi-electron transfer reactions.

Exosomes play a key role in intercellular communication and are involved in various pathophysiological processes. However, the efficient enrichment and sensitive detection of exosomes from complex biological fluids remain significant challenges. To address the enrichment difficulty, this study proposes a novel isolation strategy integrating light-responsive and pH-responsive mechanisms. By preparing immunomagnetic nanoparticles, namely CD63 aptamer-modified and NBA-modified magnetic nanoparticles termed CN-NPs, we achieved rapid capture and controlled release of exosomes. This method enables efficient separation through the coordinated regulation of external light stimulation and pH changes. Under 4 degrees C conditions, the CN-NPs efficiently captured exosomes from the culture supernatant of SH-SY5Y cells within 20 min, achieving a capture efficiency of 78.48%. Subsequently, under the synergistic dual response of 365 nm UV light and pH 8.0, exosome elution was completed within 6 min, with a release efficiency of 80.85%. The entire separation process required only 29 min, attaining an overall recovery rate of 63.45%. Compared to the gold-standard ultracentrifugation method, CN-NPs not only significantly shorten the processing time but also yield exosomes with higher purity. Cellular uptake experiments corroborated that exosomes isolated by this method retain significant biological activity. In addition, by employing a hybridization strategy involving FAM-labeled single-stranded DNA probes and complementary aptamers, we established a simple fluorescence quantification platform for the detection of captured exosomes, achieving a detection limit of 1.4 & times; 107particles/mL with a linear range from 2.8 & times; 107-2.0 & times; 108 particles/mL. This approach provides a sensitive and reliable optical readout for exosome enumeration and offers a convenient tool for downstream exosome analysis.

Modulating electronic structure and local coordination environment of electrocatalysts is a promising strategy to facilitate water adsorption and dissociation. Herein, we prepare polyoxometalate (POM) modulated Fe-doped Ni3S2 nanosheets (PMo12-Fe-Ni3S2) on a nickel foam (NF) substrate by a one-step hydrothermal method. The PMo12 clusters are homogeneously dispersed, preventing nanosheets from agglomerating, while rich electrons in PMo12 are conducive to promoting electron transfer, thereby tuning electronic configuration effectively. PMo12-Fe-Ni3S2 on NF exhibits superior electrocatalytic performance for water splitting in an alkaline medium, delivering an overpotential of 221 mV at 10 mA cm-2, a small Tafel slope of 37.7 mV dec-1, and long-term stability over 100 h for oxygen evolution reaction (OER). Further applying to an anion exchange membrane water electrolysis (AEMWE) electrolyzer, PMo12-Fe-Ni3S2 achieves a current density of 10 mA cm-2 at a cell voltage below 1.69 V. Physical characterizations and density functional theory (DFT) calculations prove that PMo12 is sacrificed while newly formed MoFe-doped NiOOH is the real active species after OER, thus accelerating electron transfer and optimizing adsorption energy of intermediates. This work provides an insightful POM engineering strategy for electronic modulation of POM-based electrocatalysts, possessing great potentials for water electrolysis applications.

Phase engineering effectively modulates the strong metal-support interaction (MSI) in heterogeneous catalysts. However, the dynamic manipulation of MSI through in situ phase transition remains underexplored. Herein, an acid-mediated strategy for in situ 1T -> 2H phase transformed MoSe2 has been reported to construct Ru sites (Ru-2H(PT)-MoSe2/CC) toward alkaline hydrogen evolution reaction, in contrast to direct Ru sites construction on the static 2H-phase MoSe2 (Ru-2H-MoSe2/CC). X-ray photoelectron spectroscopy demonstrates that, despite both catalysts sharing the same 2H-phase structure, the phase-evolved Ru-2H(PT)-MoSe2/CC exhibits significant electron accumulation at Mo and Se sites, enabling strong electrostatic interaction with the Ru3+ precursor, which dictates the final atomic configuration of Ru. Combined theoretical and experimental studies demonstrate that this strong MSI preferentially stabilizes Ru as single atoms at Mo sites concurrently with the formation of smaller Ru clusters. In stark contrast, the weak MSI in Ru-2H-MoSe2/CC leads to the predominant formation of larger Ru clusters. The resultant Ru-2H(PT)-MoSe2/CC yields a low overpotential of 26 mV at 10 mA cm-2 and long-term durability for 500 h at 100 mA cm-2. In situ Raman spectroscopy and theoretical calculations further corroborate that the unique Ru configuration optimizes interfacial water behavior and accelerates water dissociation kinetics.

Developing highly efficient catalysts for N2O abatement remains a critical challenge in environmental catalysis. In this study, a series of Fe-Co-Ce-Ox catalysts were synthesized via the impregnation method at different calcination temperatures, and their performance in the catalytic reduction of N2O was evaluated using NH3 as the reducing agent. The results demonstrate that the catalyst calcined at 300 degrees C exhibits the highest activity. Samples calcined at 400 and 500 degrees C maintain a N2O conversion of 92-95%, whereas a sharp decline in activity is observed upon increasing the calcination temperature to 600 degrees C. Comprehensive characterization reveals that the catalyst calcined at 300 degrees C possesses the largest specific surface area, a well-developed mesoporous structure, superior redox properties, and abundant medium-strength acid sites. Moreover, this moderate calcination temperature facilitates the enrichment of surface Fe3 + , Co3+, and Ce4+ species and promotes the formation of oxygen vacancies. In situ DRIFTS analysis confirms that NH3-SCR reduction of N2O proceeds via both Eley-Rideal and Langmuir-Hinshelwood mechanisms. These findings underscore that moderate low-temperature calcination was crucial for preserving the favorable physicochemical properties and surface active sites of the catalyst, thereby offering a theoretical basis for the design of efficient N2O abatement materials and advancing the fundamental understanding of the reaction mechanism.

Pore space partition achieved through symmetry-matching ligand insertion in metal-organic frameworks (MOFs) has emerged as an important strategy for high-performance gas adsorbent material design. However, due to the constraints of symmetry matching during pore partition, such materials are still limited. Inspired by typical partitioned MIL-88-type frameworks, a symmetry-mismatch-guided topological evolution strategy for porespace-partitioned MOFs was demonstrated herein. The utilization of angular organic linkers induces a steric strain effect and reduce the symmetry of MIL-88-type parent architecture to generate a symmetry mismatch with pore partitioners, which is alleviated through cage defects and metal cluster orientation torsion, and thus yields nineteen MOFs with step-by-step topological evolution. Concretely speaking, when the bite angles of angular linkers alter from 122 degrees, 126 degrees to 152 degrees, the resulting MOF architectures change from 6-c nets for SNNU-401-403, 7c-nets for SNNU-404-405, 8-c nets for SNNU-406-415 to 9-c nets for SNNU-416-418. Detailed structural analysis indicates that SNNU-416 featuring three types of flexible cages provides an optimal condition for ethylene purification. The dynamic breakthrough experiments indicate that SNNU-416 can effectively separate C2H4/C2H6 and C2H4/C3H6 binary mixtures with the productivity reaching 75.1 L/kg (C2H4) and 83.4 L/kg (C3H6) as well as achieve efficient one-step C2H4 purification from their ternary mixture.

Understanding the hybrid structural characteristics of carbon remains a significant challenge, hindering the development of clear design principles for optimizing electrode materials in energy storage systems-particularly in lithium-ion (Li-ion) and sodium-ion (Na-ion) batteries. Traditionally, the localized structural disorder and intrinsic porosity of carbon have been regarded as the primary contributors to its high storage capacity in Na-ion batteries. However, our investigation reveals that the hybrid structural features of carbon play a more dominant role in enhancing energy storage performance in Li-ion systems compared to Na-ion counterparts. Through comprehensive materials characterization and electrochemical analysis, we establish a direct correlation between the local microstructural attributes of carbon and its ion storage kinetics which elucidate the distinct ion-storage mechanisms that differentiate Li-ion from Na-ion systems. This study reinforces our findings that configurational defects are crucial for achieving high initial storage capacity in carbon crafted with mixed-phase structures, but the in-plane size of nano-layered microdomains plays a key role in ensuring long-term stable storage capacity in rechargeable batteries.

Semiconductor-based photo-redox catalysis offers a sustainable route for green organic synthesis, yet efficient C(sp3)-H bond oxidation remains challenging due to slow charge separation and limited surface reactivity. Here, we report a CsPCN (cesium doped polymeric carbon nitride)-Cs3Bi2Br9 heterojunction that promotes efficient charge separation while retaining strong hole oxidation capability of Cs3Bi2Br9 and superior oxygen and reactant activation ability of CsPCN. In situ experimental and theoretical studies confirm the photoelectron transfer pathway from Cs3Bi2Br9 to CsPCN driven by the interfacial electric field, empowering efficient spatial charge separation and high affinity and activation capability toward oxygen and reactants. As a result, the heterojunction exhibits efficient C(sp3)-H bond oxidation performance and broad substrate applicability under visible-light irradiation, achieving a conversion rate of ethylbenzene to acetophenone up to 8420 µmol g-1 h-1, 4.3 times higher than blank Cs3Bi2Br9 (1950 µmol g-1 h-1). This work demonstrates a rational heterostructure design strategy to couple charge separation with surface reactant activation for efficient lead-free perovskite based photocatalytic C(sp3)-H functionalization.

Developing polymer electrolytes (PEs) with high ionic conductivity and compatibility with Mg metal anodes remains a key challenge for solid-state rechargeable magnesium batteries (RMBs). Herein, two PEs, G3-PE1 and G4-PE1, were prepared by immobilizing highly active MgCl2-AlCl3-triethylene glycol dimethyl ether (MgCl2-AlCl3-G3) and MgCl2-AlCl3-tetraethylene glycol dimethyl ether (MgCl2-AlCl3-G4) liquid electrolytes within crosslinked polymer networks, respectively. Benefiting from the retention of the solvation structure of the liquid electrolytes and the structural support provided by the crosslinked polymer networks, both G3-PE1 and G4-PE1 exhibited high ionic conductivity and stable electrochemical performance. At 30 °C, the ionic conductivities of G3-PE1 and G4-PE1 reached 2.14 × 10-3 and 1.07 × 10-3 S cm-1, respectively, with corresponding Mg2+ transference numbers of 0.5801 and 0.4267. Moreover, Mg//Mg symmetric cells employing these PEs maintained stable cycling for over 1500 h at a current density of 25 μA cm-2. Compared with G4-PE1, G3-PE1 exhibited weaker Mg2+-ether coordination, resulting in superior electrochemical performance. The Mo6S8//G3-PE1//Mg full cell delivers a discharge capacity of 54.6 mAh g-1 after more than 350 cycles at 0.1C, demonstrating excellent cycling stability. Immobilizing highly active liquid electrolytes within crosslinked polymer networks therefore provides an effective route for developing high-performance PEs for RMBs.

Weak intra- and inter-layer bonding within the SnO2 electron transport layer and at the SnO2/perovskite interface is a primary cause of performance degradation in perovskite solar cells under prolonged illumination. Here, the intra- and inter-molecular bridging strategy employing 1,2,4-butanetricarboxylic acid (BTC) is proposed to simultaneously reinforce intra-layer cohesion and interfacial coupling. Specifically, the 2- and 1,4-carboxyl groups of BTC coordinate with Sn4+ sites, thereby reinforcing interparticle connectivity within the SnO2 layer. Concurrently, BTC forms coordination bonds between Sn4+ in SnO2 surface and Pb2+ in the perovskite, forming strong interfacial coordination interactions. More importantly, the strong electronic coupling induced by BTC constructs efficient charge transport across the buried interface, facilitating electron extraction. Meanwhile, the combined intra- and inter-layer bridging effects reduces defect density, optimizes energy-level alignment, and alleviates lattice strain of perovskite films. As a result, devices incorporating BTC exhibit both enhanced photovoltaic performance and operational stability, retaining 85.32% of initial power conversion efficiency after 200 h of continuous exposure to 365 nm ultraviolet irradiation at 50 mW cm−2, and 91.46% after 1000 h of maximum power point tracking at 65°C following the ISOS-L-2I protocol.

The design of a low-Ir-loading anode catalyst with high activity and stability is crucial for the proton exchange membrane water electrolysis (PEMWE), yet it remains a formidable challenge. Herein, an ordered Ba2EuIrO6 double perovskite is demonstrated as a promising anode material for catalyzing oxygen evolution reaction (OER) in acid electrolyte. The Ba2EuIrO6 achieves a low overpotential of 250 mV at 10 mA cm-2 and high mass activity with 1.39 A mg-1 toward OER, outperforming BaIrO3 and commercial IrO2 catalysts. It is discovered that the oxygen bridged Ir─Obri─Eu unit in Ba2EuIrO6 plays a critical role as the catalytically active center. In situ spectroscopic studies, isotope labeling measurements and theoretical calculations reveal that the Ir─Obri─Eu units possess strong proton affinity for proton capture from OOH* and OH*, triggering the bridging oxygen-mediated deprotonation mechanism to break traditional scaling relationships during the OER. Furthermore, the incorporation of Eu modulates the Ir dz2 orbital to increase the spin density of adsorbed oxygen, accelerating ─OH attack and reducing the energy barrier for OOH* formation. The Ba2EuIrO6-loading PEMWE delivers over 1.0 A cm-2 at only 1.67 V and operates stably for 350 h at 1.0 A cm-2, demonstrating its good potential for practical applications.

A ruthenium-catalyzed addition of sulfonic acids to acetylene is reported. This method employs bulk industrial feedstock acetylene as C2 synthon under atmospheric pressure to access vinyl sulfonates in good to excellent yields without using toxic mercury catalysts, offering high atom economy and practical scalability. The resulting vinyl sulfonates serve as versatile vinylating reagents and can be readily transformed into diverse functionalized molecules.

Understanding the relationship between chemical composition, atomic scale structure, and mechanical property remains a fundamental challenge in bulk metallic glasses due to the lack of long-range order. This study systematically investigates this relationship across four compositionally tunable bulk metallic glass systems: Pdx(NiCu2)(80-x)/3P20, Zrx(Al0.25Ni0.25Cu0.5)100-x, Ti41Zr25Be34-xNix, and Ti41Zr25Be34-xCux. A combined approach of experimental nanoindentation and molecular dynamics simulations is employed. Nanoindentation reveals a strong composition-dependent mechanical response: hardness and elastic modulus reduce monotonically with increasing Pd or Zr content in the Pd- and Zr-based systems, while a non-monotonic dependence is observed with rising Ni content in the Ti–Zr–Be–Ni system, and a monotonic decrease is found with rising Cu content in the Ti–Zr–Be–Cu system. X-ray diffraction analysis, using the diatomic gas model, shows that these mechanical trends inversely correlate with the average atomic spacing (d/K) consistently across all four investigated systems. To elucidate the atomistic origin of this correlation, molecular dynamics simulations were performed on the Zr-based system. The simulations reveal that increasing Zr content enlarges the nearest-neighbor distance, increases free volume fraction, and reduces atomic packing efficiency, as evidenced by radial distribution functions. These structural changes enable the activation of shear transformation zones, thereby reducing hardness and elastic modulus. This work demonstrates a consistent structure–property correlation across the investigated bulk metallic glasses by linking composition-dependent atomic packing to nanoscale mechanical behavior, providing valuable insights for designing bulk metallic glasses with tailored mechanical properties.

A bifunctional catalyst that can efficiently catalyse the hydrogen evolution reaction (HER) and urea oxidation reaction (UOR) plays a crucial role in advancing sustainable energy systems. We report a three-dimensional (3D) hierarchical core-shell nanowire architecture with a multi-interface heterostructure (NiMn LDH/Ni3S2/Co9S8) integrated with nickel foam (NF) (NiMn LDH/Ni3S2/Co9S8/NF). Initially, NiCo-precursor nanowire arrays grown on NF served as precursors, which were transformed into Ni3S2/Co9S8 cores via hydrothermal sulfuration. Subsequent electrodeposition coated these cores with shells of amorphous NiMn LDH nanosheets, resulting in NiMn LDH/Ni3S2/Co9S8 core-shell nanowires. The catalyst demonstrated outstanding HER and UOR performance, achieving 100 mA & sdot;cm-2 at-0.221 and 1.343 V vs. reversible hydrogen electrode (RHE) for the HER and UOR, respectively. This enhanced activity is based on three key factors: (i) the three-hierarchical core-shell nanowires with abundant heterointerfaces enhance conductivity, ion diffusion kinetics, and gas release, exposing more active sites; (ii) the interfacial built-in electric field between the core and shell optimises the electronic structure to facilitate water and urea dissociation; and (iii) the synergistic interactions between amorphous NiMn LDH and Ni3S2/Co9S8 further boost the catalytic efficiency for both reactions. This approach introduces a multi-interface engineering strategy for developing high-performance bifunctional electrocatalysts for the HER and UOR applications.

The development of earth-abundant, low-cost, highly active catalysts to accelerate hydrogen absorption/desorption kinetics in Mg-based materials is critical for hydrogen energy applications. Here, we synthesize three MAX phases with nonconventional A-site elements─Nb2FeC, Nb2NiC, and Nb2CuC─and directly incorporate them into MgH2 matrices without hazardous HF etching. All three MgH2-10 wt % Nb2AC (A = Fe, Ni, Cu) composites exhibit a reduction in onset dehydrogenation temperature from 320 °C to approximately 190 °C, and their dehydrogenation temperature and kinetic behavior are markedly superior to Nb2AlC, demonstrating that substituting the A-site element Al with late transition metals substantially enhances catalytic performance toward MgH2 dehydrogenation. Among them, the MgH2-10 wt % Nb2NiC composite shows optimal performance, releasing ∼6.30 wt % H2 at 300 °C within 10 min and absorbing ∼5.01 wt % H2 at 175 °C within 3 min, while maintaining good cyclic stability. Experimental and theoretical results jointly confirm that Nb2NiC functions as an efficient electron-mediated catalyst, weakening Mg-H bonds and promoting H2 dissociation via interfacial electron transfer, thus significantly improving hydrogen storage kinetics.

The hygroscopic nature and severe ions diffusion of conventional dopant Li-TFSI, along with interfacial ionic defects, limiting the efficiency and stability of n-i-p perovskite solar cells (PSCs). To address this, we propose a single-dopant strategy employing a multifunctional, star-shaped dopant 2,4,6-tris(3,4,5-tri fluorophenyl)boroxine (TBRX) with a Lewis acidic boroxine core and highly electronegative fluorinated aryl groups, incorporated into Spiro-OMeTAD. Theoretical and experimental results indicate that TBRX significantly enhances hole mobility, conductivity and the flatness of hole-transporting layer (HTL) while passivating interfacial defects (Pb2' , VI), leading to a reinforced perovskite/HTL interface. Additionally, the corresponding p-dopant effectively reduces the energy barrier between the perovskite and the HTL, promoting efficient hole extraction. Consequently, Spiro-OMeTAD:TBRX-based devices deliver a high PCE of 25.57 % (certified at 25.01 %) with excellent long-term operational stability obtained for over 1000 h, retaining similar to 94 % of its initial efficiency after 1000 h according to ISOS-L-2 protocols, highlighting the significance of utilizing multifunctional single-dopant framework. (c) 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.