The efficacy of chemodynamic therapy (CDT) is limited by low endogenous H₂O₂ levels, and monotherapy often fails to achieve complete tumor eradication. To overcome these challenges, we constructed a multifunctional nanoplatform named Ti₃C₂T_x@AuPt-FA (MAPF). The key innovation of this work lies in a self-supplementing cascade catalytic cycle. Au/Pt nanozymes provided H₂O₂ to generate ·OH by continuously consuming glucose, thus enhancing CDT. Photothermal therapy could synergistically enhance the effect of CDT. The MAPF platform exhibited high catalytic activity and efficient photothermal conversion (η = 52.8%). It potently induced apoptosis in 4T1 cells in vitro and achieved efficient tumor ablation in vivo. Moreover, MAPF enabled prolonged tumor retention and permitted real-time monitoring via computed tomography (CT) and infrared thermal (IRT) imaging. Safety evaluations confirmed that the platform possessed excellent biocompatibility with no significant systemic toxicity. This work provides a typical self-sustaining nanoplatform that addresses the fundamental limitations of CDT, offering a powerful theranostic strategy with high translational potential for precise breast cancer treatment.

Thermally activated delayed fluorescence (TADF) materials that simultaneously exhibit short-range (SR) and long-range (LR) charge-transfer (CT) excited states represent a promising new class of emitters for organic light-emitting diodes (OLEDs). Such systems combine the advantages of conventional donor–acceptor (D–A) and multi-resonance (MR) emitters, including high photoluminescence quantum yield (PLQY), fast radiative decay (k_r) and reverse intersystem crossing rates (k_RISC), and narrowband emission profiles. However, their molecular design principles and structure–property relationships remain largely unexplored. In this work, two new TADF emitters featuring both SR-CT and LR-CT excited states were developed by attaching electron donors to an MR fragment via a boron–meta–donor linkage. Together with reference compounds, these emitters enable a systematic investigation of the influence of the donor structure and linkage mode on the key photophysical properties of such light-emitting materials. Compared with conventional boron–para–donor linked emitters, the boron–meta–donor linked designs display highly hybridized SR–LR–CT character, manifested in distinctive emission bandwidths, enhanced solvatochromism, and donor-strength-dependent excited-state kinetics. Leveraging these features, high-performance narrowband OLEDs were fabricated, achieving a maximum external quantum efficiency (EQE_max) of 35.1% and exhibiting remarkably low efficiency roll-off, with an EQE of 18.1% maintained at a luminance of 10,000 cd·m⁻².

Two-dimensional conductive metal–organic frameworks (2D c-MOFs), constructed by coordination between metal ions and π-conjugated ligands, represent a unique class of materials that combine intrinsic porosity and electrical conductivity. However, the contribution of metal nodes to the overall electrical properties remains unclear. In this work, we systematically investigate the role of metal centers on a series of six highly crystalline hexahydroxytriphenylene (HHTP) based c-MOFs, M-HHTP, which incorporate alkaline earth including magnesium and calcium, as well as transition metals including cobalt, nickel, copper, and zinc. Comprehensive structural characterizations reveal that while all M-HHTP frameworks adopt a general honeycomb lattice, however, subtle variations in stacking patterns and coordination environments are induced by different metal ions. Electrical measurements show a pronounced dependence of conductivity on the nature of the metal nodes, in which the conductivity differs by four orders of magnitude due to the difference in metal centers. Furthermore, non-contact terahertz spectroscopy combined with theoretical calculations suggests that in alkaline earth metal-based MOFs, charge transport may proceed via a through-space hopping mechanism between organic ligands. This study elucidates the critical role of metal centers in governing charge transport in M-HHTP MOFs and offers valuable guidance for the rational design of high-performance 2D conductive frameworks.

Achieving high electrical conductivity through doping without compromising the Seebeck coefficient remains a fundamental challenge in organic thermoelectrics, owing to the intrinsic trade-off between the two parameters. Here, we propose a rational molecular design strategy to enhance the charge delocalization by substituting thiophene with selenophene in donor-acceptor (D-A) type of conjugated polymers based on benzo[1,2-b:4,5-b']dithiophene (BDT) and diketone-functionalized benzo[1,2-c:4,5-c']dithiophene (BDD) units. The selenophene substitution, combined with backbone planarization via a phenyl substituent, increases the charge localization length from ~7 nm to ~11.5 nm. These structural modifications result in a significant improvement of electrical conductivity, from ~78 S cm^–1 to ~148 S cm^–1, while maintaining a high Seebeck coefficient, leading to a maximum power factor exceeding 130 μW·m^–1·K^–2. These results highlight selenium-driven charge delocalization as a promising approach to modulating charge transport and guide the molecular design of efficient organic thermoelectrics.

Organic photovoltaic (OPV) cells hold great promise as next-generation green energy owing to their tunable photoelectronic properties and compatibility with large-area solution printing. However, most high-performance materials have been optimized primarily for standard sunlight, with limited strategies for multi-spectral illuminations. Here, we report two wide-bandgap donor polymers, PDBQx-γ and PDBQx-β, integrating a dibenzo[f,h]quinoxaline unit and a two-dimensional benzodithiophene unit linked by alkyl-thiophene π-spacers. Optimized molecular design of PDBQx-β enables enhanced molecular packing, favorable morphology, and superior charge transport, delivering a power conversion efficiency (PCE) of 13.7% for PDBQx-β:FTCC-Br based on single-junction OPV cells under AM 1.5G illumination. Furthermore, the fabricated large-area OPV modules (23.6 cm²) achieve remarkable PCEs of 26.4% under 660 nm laser, 20.8% under underwater illumination, and 27.3% under indoor light. This study demonstrates a molecular design strategy for wide-bandgap polymers intrinsically compatible with diverse light sources, advancing OPV technology toward multi-scene applications.

Although asymmetric catalytic synthesis via dynamic kinetic resolution has proven to serve as a powerful tool for the efficient preparation of planar chiral pillar[5]arenes, the enantioselective synthesis of highly-functionalized pillar[5]arenes with more than two functional groups remains rarely explored. To tackle with this challenge, here we demonstrate the enantioselective synthesis of tetra-functionalized planar chiral pillar[5]arenes via catalytically four-fold asymmetric Sonogashira coupling, resulting in the successful synthesis of diverse planar chiral pillar[5]arenes with both high functionalization degree and very high enantioselectivities (in most cases, >99% e.e.). Attractively, facile derivatizations of the resultant planar chiral pillar[5]arenes further give access to chiral functional pillar[5]arenes with wide potential applications, making them promising building blocks for practical uses. This work not only enriches the synthetic methods for planar chiral pillararenes with high functionalization degree but also give access to diverse promising chiral building blocks for widespread applications.

Aminyl radicals of the type •NR₂, featuring a nitrogen-centered unpaired electron, are highly reactive intermediates that are notoriously difficult to isolate in the condensed phase. Herein, we report the synthesis of thio-, seleno- and telluro-aminyl radicals 2–4, obtained in one step from reactions of an isolable triplet nitrene with diphenyldichalcogenides. Radicals 3 and 4 represent the first stable examples of seleno- and telluro-substituted aminyl radicals. Compounds 2–4 were characterized by single-crystal X-ray diffraction, electron paramagnetic resonance and UV/Vis absorption spectroscopy. This work not only expands the family of isolable nitrogen-centered radicals, but also opens new avenues for main-group radical chemistry involving heavier p-block elements.

The high reactivity and transient nature of non-stabilized sp³-hybridized carbocations have long limited their application in enantiocontrolled transformations. In particular, the difficulty in regulating their lifetime and stereochemical environment has posed a fundamental challenge for asymmetric catalysis. Here, we report a catalytic strategy that addresses these challenges by harnessing cyclopropylcarbinyl cations as reactive yet controllable intermediates. These cations, known for their propensity to undergo rapid rearrangement, are strategically stabilized and directed within a chiral ion-pairing framework. Despite their rarity in asymmetric catalysis, these electrophiles enable highly enantioselective asymmetric Friedel–Crafts alkylation reactions when paired with newly developed phosphoramidimidate catalysts functioning as chiral Brønsted acids. The confined chiral environment provided by these catalysts effectively governs carbocation rearrangement pathways, allowing for precise stereochemical control. This method delivers excellent enantioselectivity and yields across a broad range of arenes, highlighting its generality in arene functionalization. Unlike conventional methods requiring substrate preactivation, our approach directly utilizes alcohol as electrophile precursors, forming water as the sole byproduct through an S_N1-type mechanism. The catalytic system promotes selective desymmetrization of prochiral substrates, converting simple and readily available starting materials into structurally complex chiral products. Importantly, controlled rearrangement of cyclopropylcarbinyl cations plays a key role in expanding molecular diversity without sacrificing enantioselectivity. Overall, this strategy significantly broadens the electrophile scope accessible in asymmetric synthesis. By integrating rearrangement control and chiral Brønsted acid catalysis, the present work establishes a new paradigm for exploiting highly reactive carbocation intermediates. These findings not only advance asymmetric catalysis but also open new avenues for enantiocontrolled transformations involving nonclassical carbocation chemistry.

A practical photoinitiated synthetic method for the site-selective γ - and α-chlorination of C(sp³)–H bonds of ketones, (E)-1,3-enones, and alkylbenzenes by chloramine-T (CAT) and N-chlorosuccinimide (NCS) under blue LED (λ_max = 456 nm) light irradiation is reported. Mechanistic studies suggest the reaction to proceed via a radical pathway where the chlorination reagent dichloramine-T (DCT) is generated in situ from the reaction of CAT with NCS. Its premised controlled formation along with that of the carbon-centered radical species derived from the substrate is thought to contribute to product site-selectivity. The developed protocol operates under mild reaction conditions at room temperature and demonstrates excellent functional group tolerance as exemplified by the site-selective γ-C(sp³)–H bond chlorination of carboxylic esters and amides, and late-stage functionalization of several bioactive natural products and drug molecules. The study also highlights the potential of CAT for the first time as a versatile and controllable chlorine radical atom source for site-selective halogenation reactions, expanding its synthetic utility beyond traditional applications.

Photocatalytic semihydrogenation of coal-derived acetylene using water as a hydrogen source under ambient conditions offers a sustainable and petroleum-independent route for ethylene production, yet suffers from the utilization of expensive photosensitizers, weak acetylene adsorption and insufficient generation of active hydrogen (H*). Herein, we fabricate a Co single-atom catalyst anchored on nitrogen-vacancy-rich carbon nitride (Co/C₃N₄-V_N) via in-situ co-polymerization. Owing to enhanced light absorption and charge separation efficiency, the Co/C₃N₄-V_N exhibits a considerably high ethylene production rate of 3916.5 μmol·g_cat⁻¹·h⁻¹ under 420 nm light-emitting diode (LED) illumination without photosensitizers, surpassing bulk C₃N₄ by 53-folds and outperforming previously reported photocatalysts. The photocatalytic experiments, acetylene temperature-programmed desorption analysis, in-situ photo-chemical infrared spectra and theoretical simulations together reveal that N vacancies and Co single atoms in Co/C₃N₄-V_N synergistically promote the acetylene adsorption, H* generation from water dissociation and acetylene hydrogenation, thereby accelerating the kinetics of photocatalytic acetylene semihydrogenation.

Recently, circularly polarized luminescence (CPL) and room-temperature phosphorescence (RTP) materials have attracted significant attention across various fields. The stereogenic biaryl units are critical sources of CPL and RTP activity, including binaphthyl, binaphthalenediol, and binaphthalenediamine derivatives. However, the stereoselective transformation and chiroptical functionalization of 1,1′-binaphthyl-2,2′-diphemyl phosphine (BINAP) and its oxide (BINAPO) are largely unexplored. Herein, a series of axially chiral luminous molecules is prepared by modular covalent-linking of BINAP/BINAPO and arylamine donors (N-phenylcarbazole (CZ) or triphenylamine (TPA)) at 4,4′-positions to study their photoluminescence and chiroptical properties. Intriguingly, the molecules based on BINAPO emit intense fluorescence, and the persistent RTP of 301−578 ms is achieved when these compounds are doped in the polymer matrixes, which contributes to the formation of the optimized energy gap and intersystem crossing (ISC) by virtue of intramolecular charge transfer (ICT) states and heavier phosphorus atoms. Circular dichroism (CD) spectral studies reveal that all BINAP/ BINAPO derivatives exhibit decent optical activity in dichloromethane (DCM) and weak CPL due to the inferior electro-magnetic transition environment. On the contrary, the co-aggregates, consisting of chiral BINAPO derivatives with helical structures and commercial nematic liquid crystals (N-LCs, 5CB), show significantly enhanced CD and CPL signals with the improved FM value of 0.05−0.10.

Electrochemical water splitting for hydrogen (H₂) production represents a promising technology to achieve carbon neutrality. However, its widespread application is severely limited by the sluggish kinetics and high theoretical potential (1.23 V) of the anodic oxygen evolution reaction (OER), which dominates the overall energy consumption. Hybrid water splitting (HWS) systems, which integrate thermodynamically more favorable anodic oxidation reactions of small molecules with the cathodic hydrogen evolution reaction (HER), provide an innovative approach for efficient and energy-saving H₂ production. Crucially, achieving operation at industrially relevant high current densities (> 200 mA·cm⁻²) is paramount for the practical implementation of these HWS systems. This review systematically summarizes recent advances in the development of high-performance anodic electrocatalysts for high-current-density applications. Key design strategies of anodic electrocatalysts are elaborated, including (i) surface chemistry engineering (e.g., elemental doping, defect/strain/phase engineering, heterostructure construction) to optimize electronic structure and intermediates adsorption energetics; (ii) micro-/nano-structure design (e.g., nanowires, nanosheets, microspheres, aligned- channel electrodes) to enhance mass transport and expose active sites; and (iii) catalyst-electrolyte interface tuning (e.g., leveraging local electric fields, pH effects, introducing adsorbed anions) to regulate reactant concentrations and reaction pathways. We then comprehensively discuss the coupling of various small molecules (e.g., urea, hydrazine, methanol, ethanol, glycerol, aldehyde, glucose, amine and sulfion) oxidation reactions with the HER for efficient and energy-saving H₂ production under high current density conditions, with a particular focus on mitigating the competition from the OER. Finally, we present perspectives on the remaining challenges and future research directions, including the rational design of catalysts with high intrinsic activity and selectivity, in-depth mechanistic investigations using advanced in situ/operando techniques, the development of efficient flow reactors and membrane electrode assemblies for industrial operation, and strategies to enhance long-term stability. This review aims to provide valuable insights for the advancement of hybrid water splitting systems toward large-scale, cost-efficient and energy-saving H₂ production.

The development of high-performance liquid electrolytes is pivotal for advancing rechargeable lithium batteries, which are central to global electrification and renewable energy integration. Conventional electrolyte design, heavily reliant on empirical trial-and-error approaches, faces significant challenges in simultaneously optimizing a complex set of properties, including ionic conductivity, electrochemical stability window, thermal resilience, and most critically, compatibility with electrode interfaces. The efficiency of charge transfer processes and the stability of interphases formed on electrode surfaces, such as the solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI), are fundamentally governed by electrolyte composition. The nonlinear dependencies among these properties and the vast, unexplored chemical space render traditional methods inefficient. Emerging data-driven strategies represent a paradigm shift, leveraging artificial intelligence (AI) and machine learning (ML) to accelerate the discovery and rational design of next-generation electrolytes. This review comprehensively surveys recent progress in this rapidly evolving field. We begin by systematically outlining the fundamental properties of liquid electrolytes and establishing advanced descriptors for quantifying ion-solvent and ion-anion interactions. The core AI workflow encompassing data acquisition from diverse sources, feature engineering, and the application of various models from supervised learning to generative AI is critically examined. We then showcase the transformative applications of data-driven methodologies, including performance-targeted electrolyte formulation for extreme conditions, prediction of interfacial reaction pathways and SEI/CEI evolution mechanisms, and the development of novel AI algorithms and integrated computational platforms for end-to-end discovery. Despite promising advances, challenges remain, such as data scarcity and standardization, limited model generalizability, and the difficulty of multi-objective optimization balancing performance, safety, and sustainability. By synthesizing these developments and outlining a clear research trajectory, this review aims to provide novel perspectives and inspire continued innovation in the design of high-performance, safe, and sustainable electrolytes, ultimately enabling more reliable and powerful rechargeable lithium batteries for a clean energy future.