Solid electrolyte interface (SEI) underpins the performance of lithium metal batteries (LMBs). While SEI has been probed to enhance interfacial stability and kinetics, the fast-charging capability of LMBs remains limited due to the growth of lithium dendrites and polarization at the interface. We have recently identified that ionic artificial SEI plays a crucial role in addressing these challenges, especially when integrating ionic fluoropolymers to optimize interfacial properties. Herein, we systematically studied the fundamental effect of ionic artificial SEI on interfacial kinetics by constructing a single-ion conducting polymer (P-SO₃Li) layer using spin-coating, and compared it with conventional linear polymers and bare lithium anodes. Molecular simulations revealed that the sulfonic acid groups (-SO₃^–) in the P-SO₃Li polymer could promote dissociation of Li⁺ owing to electrostatic interactions. Meanwhile, electrochemical experimental results showed that the P-SO₃Li polymer coating exhibited a lower desolvation energy barrier than PEO and bare lithium, and it had better dendrite suppression ability, while achieving exchange current densities comparable to bare lithium anodes. Through XPS observation of the lithium anode, it was found that the structure of the P-SO₃Li polymer coating remained basically unchanged before and after cycling. Therefore, fast-charging cycles up to 5 C were successfully achieved, with a Coulombic efficiency of 95.4% and a capacity retention rate of 86.5% after 100 charge-discharge cycles. In contrast, electrically neutral PEO and bare lithium anodes could only attain Coulombic efficiencies of 93.7% and 90.4%, respectively, along with capacity retention rates of merely 77.9% and 60.6% after 100 cycles. This work informs the fundamental effect of charged interfacial structures underpinning the enhancement of fast-charging performance in LMBs.

Despite the significant potential of planar chiral [2.2]paracyclophane (PCP) derivatives in medicinal chemistry, asymmetric catalysis, and material science, their efficient synthesis remains a great challenge. The organocatalytic asymmetric reductive amination (ARA) represents a cornerstone methodology in the production of optically active amines. However, the application of ARA for the control of planar chirality in [2.2]PCPs has yet to be explored. To fill this gap, we describe herein an unprecedented chiral phosphoric acid (CPA)-promoted ARA of center-symmetrical pseudo-para-diformyl [2.2]PCP with aromatic amines in the presence of Hantzsch ester, which involves a desymmetrization/kinetic resolution (KR) sequence. The CPA serves as a competent bifunctional catalyst to facilitate differentiation of enantiotopic faces, allowing for access to a wealth of benzylamine-containing 4,16-disubstituted planar chiral [2.2]PCPs with good yields and high to perfect enantioselectivities (up to 89% yield, >99% ee). The ARA-KR of racemic formyl [2.2]PCPs also proceeds smoothly with moderate to good selectivity factors. The diverse late-stage functionalization further highlights the value of current chemistry.

This study investigates the impact of calendar aging conditions on the subsequent cycling performance of lithium-ion batteries. The experiments utilized LiFePO₄/graphite (LFP/Gr) pouch cells, which were charged to two states of charge (SOC): 50% and 100%. After storage at 45 °C for 100 d, cycling aging tests were conducted. The results indicate that the pre-storage conditions significantly affect cycling stability: batteries stored at high SOC exhibited more severe capacity degradation and mechanical deterioration, whereas those stored at low SOC maintained better electrochemical reversibility and mechanical stability. Through a multiscale investigation, it was found that high SOC calendar aging induces side reactions at the electrode interface and promotes uneven formation of the solid electrolyte interphase (SEI) on the anode. The structural and chemical damages incurred during the storage process become potential failure sources and manifest during the cycling aging process. This research establishes a statistical correlation framework between calendar aging damage and cycling failure, suggesting that the performance degradation of lithium-ion batteries is not solely attributed to long-term cycling but is also significantly influenced by prior storage conditions. The findings provide important insights for optimizing SOC management and storage strategies to enhance battery lifespan and reliability.

Allylic alcohols serve as highly versatile building blocks in organic synthesis. Despite their utility, catalytic methods for accessing fluoroalkyl allylic alcohols from simple alkynes remain scarce, particularly those enabling stereodivergent synthesis. Herein, we report a copper/photoredox dual-catalyzed hydrofluoroalkylation reaction of terminal alkynes with bromofluoroethanol benzoate reagent. This protocol provides stereodivergent access to (E)- and (Z)-fluoromethyl allylic alcohol derivatives in moderate to good yields. The transformation exhibits broad substrate scope and functional group tolerance, proceeds under mild conditions, and employs a readily available fluoromethyl synthon. Mechanistic studies reveal a radical pathway featuring aminoalkyl radical-mediated halogen-atom transfer (XAT), copper-assisted ketyl radical addition to the alkyne, and triplet energy transfer (EnT)-promoted double-bond isomerization as the key steps.

Interfacial defects and energy level mismatch in perovskite solar cells (PSCs) severely limit their efficiency and stability. Small-molecule passivators show great potential in addressing interfacial issues, but how electronic effects influence the performance of PSCs by modulating the electrostatic potential distribution of the entire molecule and its functional groups remains unclear. Herein, we introduced different benzylamine derivatives and found that they can all react with the formamidinium cation (FA⁺). Compared to 4-methoxybenzylamine (PMBA) and benzylamine (BA), 4-trifluoromethylbenzylamine (TFMBA) has a lower proton transfer energy barrier, facilitating the formation of TFMBAFA⁺. Compared to PMBAFA⁺ and BAFA⁺, TFMBAFA⁺ forms stronger hydrogen bonds with I^– better stabilizing the perovskite structure; simultaneously, its increased dipole moment promotes energy level alignment and charge carrier extraction. The introduction of the passivators reduced interfacial non-radiative recombination. Finally, TFMBA-modified devices (0.09 cm²) achieved an optimal power conversion efficiency (PCE) of 25.52%, while large-area devices (active area of 23.4 cm²) also attained a PCE of 20.44%. Under continuous illumination in N₂ atmosphere for 1300 h and dark storage at 60 °C, the devices retained 83% and 80% of their initial PCE, respectively.

Minimizing energy dissipation during charge transfer is essential for constructing efficient photocatalysts. However, the inherent steric constraints within building blocks inevitably induce torsional distortions in the photocatalyst framework, thereby impeding efficient charge migration. To address this, catalyst ring expansion was proposed to enhance catalytic performance. Conjugated microporous polymers (CMPs) were synthesized using [2,2']-bithiophene-5,5'-dicarbaldehyde (donor) and formyl positional isomers (1,3- or 1,4-diacetylbenzene linkers). Structural characterization revealed that compared to m-SSCMP (1,3-linker), p-SSCMP constructed with the 1,4-linker exhibits an expanded cyclic architecture, increased intramolecular D-A configurations and a reduced phenyl-pyridine dihedral angle. These structural modifications significantly accelerated charge migration efficiency. As a result, the optimized catalysts facilitated efficient C(sp³)-H phosphorylation reactions, offering a sustainable strategy for introducing phosphoryl groups into optoelectronic materials and bioactive molecules. Importantly, correlation between monomer structure and catalyst charge migration efficiency was established, providing molecular-level insights for the design of polymeric photocatalysts.

α-Azidoboronates, integrating both azido and boryl groups, are versatile intermediates for accessing α-aminoborons, α-triazolylborons, and bioorthogonal ligation handles. However, existing syntheses rely primarily on nucleophilic substitution of pre-functionalized α-haloboronates, which require multistep cryogenic Matteson homologation and involve unstable intermediates as well as hazardous azide reagents. Direct Cα–H azidation of alkyl boronates offers an appealing alternative but remains challenging due to competing radical addition to the sp²-boron center, leading to deborylation. Motivated by the unique stereoelectronic properties of B(MIDA) groups, which can stabilize α-radicals and promote boron-retentive transformations, we envisioned that selective radical C–H azidation of secondary B(MIDA)s could be feasible. Herein, we establish an iron-catalyzed protocol enabling efficient and site-selective Cα–H azidation of secondary MIDA boronates, leveraging σ(B–N) → p(C) hyperconjugation for α-radical stabilization. The protocol furnishes a broad range of α-azidoboronates in a single step. Preliminary studies further demonstrate their compatibility with click chemistry, underscoring their potential utility in functional molecule construction and bioorthogonal applications.

Thioesters serve as indispensable pharmacophores and versatile functional building blocks, finding broad utility in pharmaceutical development, prodrug design, and functional material synthesis owing to their unique chemical reactivity, metabolic stability, and target-binding affinity; however, conventional thioester synthesis is plagued by critical limitations: reliance on toxic sulfur precursors, harsh reaction conditions, costly metal catalysts, and environmentally detrimental byproducts—factors impeding large-scale, sustainable manufacturing. Herein, we report a green and efficient protocol for thioester synthesis via TBADT-photocatalyzed sequential continuous hydrogenacylation of aldehydes with isothiocyanates, mechanistic studies showing this transformation proceeds via a radical cascade reaction enabled by photoinduced multi-step Hydrogen Atom Transfer (HAT) processes: photoexcited TBADT abstracts an aldehydic C–H H-atom to generate acyl radicals, which undergo regioselective addition to isothiocyanates, followed by HAT regeneration to afford thioesters. This protocol features notable advantages: a broad substrate scope encompassing linear/cyclic/branched alkyl aldehydes, electron-rich/deficient aryl isothiocyanates, and heteroaromatic scaffolds; water as a key co-solvent enhances reaction efficiency and sustainability, further by eliminating toxic reagents, external oxidants, and pre-functionalization steps, this work overcomes core challenges in traditional thioester synthesis, establishing a novel and sustainable platform for thioester preparation and functionalization of bioactive molecules—thus advancing green organic synthesis and pharmaceutical chemistry.

A general protocol for the trifluoromethylselenylative difunctionalization of aryne with the nucleophilic [Me₄N][SeCF₃] reagent is described. The NiCp₂-catalyzed cross-couplings of o-silylaryl triflates, [Me₄N][SeCF₃], and CsF with H₂O/CH₃CN, D₂O/CD₃CN, and n-C₄F₉I or C₆F₁₃Br or CCl₄ afforded the hydrotrifluoromethylselenylated products, deuterotrifluoromethylselenylated products, and halotrifluoromethylselenylated products, respectively, while the metal-free reaction of o-silylaryl triflates and [Me₄N][SeCF₃] with NFSI provided the bis(trifluoromethylselenylated) products. These reactions allowed for the facile synthesis of diverse difunctionalized SeCF₃ products in good yields, which are unprecedented and difficult to synthesize by other methods. In the Ni-catalyzed reactions, the key aryne intermediate is generated from o-silylaryl triflate in the presence of fluoride ion, coordinates with the nickel catalyst, undergoes ligand exchange with the ^–SeCF₃ anion, and is inserted into the carbon-carbon triple bond to form an o-trifluoromethylselenylaryl-nickel complex, which is then protonated with H₂O/CH₃CN to yield the hydrotrifluoromethylselenylated product, deuterated with D₂O/CD₃CN to produce the deuterotrifluoromethylselenylated product, or halogenated with n-C₄F₉I, C₆F₁₃Br or CCl₄ to afford the halotrifluoromethylselenylated product. In the metal-free reaction, the ^–SeCF₃ anion is first oxidized with NFSI to yield •SeCF₃ radical and fluoride ion, which activates o-silylaryl triflate in situ to form the aryne species, followed by radical addition with •SeCF₃ and subsequent trapping by another •SeCF₃ radical to produce the bis(trifluoromethylselenylated) product. The moisture-sensitive [Me₄N][SeCF₃] salt was successfully tolerated in the reactions with H₂O or D₂O. This work further demonstrated the rich chemistry of [Me₄N][SeCF₃] and the power of aryne-based functionalization as a linchpin step in the production of multi-substituted SeCF₃-arenes.

The development of efficient and sustainable catalytic systems based on earth-abundant metals for hydrogen storage and green organic synthesis represents a significant and urgent challenge. While ammonia borane (AB) is a promising hydrogen carrier, its catalytic dehydrogenation and subsequent transfer hydrogenation have predominantly relied on precious-metal catalysts, and existing cobalt-based systems often lack the combination of ultrahigh activity and broad utility. Addressing this gap, this work introduces a well-defined macrocyclic bispyridyldiimine-supported binuclear cobalt complex that serves as a highly efficient catalyst for both AB dehydrogenation, achieving high H₂ release and a wide range of AB-mediated transfer hydrogenation reactions under mild conditions. The system demonstrates exceptional performance by facilitating the reduction of diverse substrates—including alkenes, indoles, nitriles, and carbonyl compounds—in high yields. Its unprecedented activity is highlighted by the transfer hydrogenation of olefins at an ultralow catalyst loading of just 0.01 mol%, and its capability to hydrogenate challenging substrates like indoles at room temperature, overcoming the need for traditional harsh conditions. A key mechanistic insight is the distinct bimetallic advantage: the corresponding mononuclear cobalt complex is catalytically inactive under identical conditions, underscoring that the superior activity arises from the synergistic binuclear structure. These findings establish synergistic binuclear cobalt catalysis as a highly active, and sustainable platform for reductive transformations using AB, fundamentally advancing the field of earth-abundant metal catalysis.

The lead-free metal halide perovskites (MHPs) have emerged as prospective, environmentally friendly, and high-performance candidates for X-ray detection owing to their prominent X-ray absorption capacity and low toxicity. Nevertheless, the energy consumption caused by high external operational voltages and severe ion migration limit the stability of lead-free MHPs for X-ray detection. Here, through the incorporation of alternating chiral–achiral spacer cations, we synthesized a novel lead-free chiral-polar perovskite, (R-MPA)₂(PA)₂AgBiBr₈ (1R, R-MPA = R-methylphenethylammonium, PA = propylamine). The intrinsic spontaneous electric polarization yields an obvious bulk photovoltage (0.25 V), facilitating the separation and transport of photogenerated carriers, which makes self-driven detection possible. Consequently, the 1R-based X-ray detector achieves a high sensitivity (131 μC·Gy^–1·cm^–2) and a detection limit as low as 62.6 nGy·s^–1 at 0 V bias. This study indicates the huge potential of chiral-polar lead-free MHPs in realizing superior self-driven X-ray detection, and provides an approach to the design of highly promising self-driven X-ray detection materials.

The rapid development of non-fullerene acceptors (NFAs), particularly Y6 and its derivatives, has propelled organic photovoltaics (OPVs) to power conversion efficiencies (PCEs) exceeding 20%. This achievement stems from the rational design of core structures that regulate energy levels, optical absorption, and molecular packing. However, the potential of the 1,2,4-triazine motif remains underexplored despite its unique electronic features. Here, we introduce the benzo[1,2,4]triazine (BTAZI) core as a promising building block for NFAs. Density functional theory calculations reveal that BTAZI possesses lower-lying energy levels than the benzothiadiazole (BT) unit in Y6, arising from its reduced electron density. Through heteroatom substitution (S, O, and Cl), we finely tune the σ-inductive and p-π conjugative effects, yielding three BTAZI-based acceptors: BTAZI-IC-SMe, BTAZI-IC-OMe, and BTAZI-IC-Cl. Among them, BTAZI-IC-SMe achieves an optimal balance between molecular orbital alignment and absorption profile with the donor polymer D18, affording a PCE of 18.14%, surpassing the others. This study highlights the benzo[1,2,4]triazine framework as a new core unit for efficient NFAs and offers valuable insights into the molecular design of high-performance and stable OPVs.

Access to safe and clean water is fundamental to human health and economic development. While the practical impact of emerging technologies depends on their successful demonstration at large scales, capacitive deionization (CDI) has garnered significant attention as a promising approach for efficient desalination of seawater and brackish water. Among the various 2D materials explored for CDI (e.g., graphene, MXenes, covalent organic frameworks), their derived 2D/2D heterostructures, with unique lamellar morphology and interfacial engineering, offer an ideal platform for effectively modulating charge transfer behavior and ion diffusion. Despite a variety of 2D/2D heterostructures with diverse construction modes have been developed as CDI electrodes in recent years, a dedicated review focusing on the design strategies, synergistic effects, water desalination performance, and prevailing challenges remains lacking. In this review, we highlight the cutting-edge research progress of 2D/2D heterostructures for CDI applications. After an overview of 2D materials and synthetic strategies of 2D/2D heterostructures, the relationships between the morphology/structure/composition and the water desalination performance are discussed in detail. Thereafter, we discuss current limitations and propose future directions for the rational design of 2D/2D heterostructures. This review will promote exploitation of 2D/2D heterostructures with an ideal performance of CDI towards water remediation.

Significant progress has been made in the development of 2D/2D heterostructures for capacitive deionization (CDI) applications towards versatile ion capture. This collection of pioneering work underscores a clear trajectory in the field: the strategic construction of 2D/2D heterostructures is a powerful and versatile paradigm for advancing CDI. By intelligently combining different 2D materials, researchers have successfully engineered heterointerfaces with enhanced ion adsorption capacity, superior selectivity, and improved stability, paving the way for next-generation, high-performance desalination and water remediation technologies.

Over the course of the past decade, microdroplet chemistry has rapidly evolved into a transformative field, offering unprecedented opportunities in chemical synthesis by leveraging the distinctive physicochemical properties of gas–liquid interfaces. Water-containing microdroplets exploit unique physicochemical characteristics at the gas-liquid interface, including intense interfacial electric fields, localized concentration effects, partial solvation and droplet evaporation, which collectively enable spontaneous chemical reactions and extraordinary reaction acceleration, achieving rate enhancements of several orders of magnitude compared to conventional bulk-phase systems. The confined microenvironment of microdroplets not only enhances mass transfer and molecular collision frequencies but also stabilizes reactive intermediates, facilitating reaction pathways that are otherwise kinetically or thermodynamically constrained. This review begins with a summary of key methods for microdroplet generation, including electrospray ionization, gas nebulization, ultrasonic atomization, levitation techniques, and adiabatic expansion, highlighting how these techniques influence the key characteristics and reactivity of microdroplets. The discussion then advances to the application of these unique properties of microdroplets in diverse chemical synthesis reactions, including redox chemistry, coupling reactions, abiotic synthesis of biomolecules and quasi-electrochemical reactions. The enhanced reaction performance observed in these systems stems from the synergistic contributions of enhanced mass transfer, localized concentration enrichment, interfacial electric fields, and droplet evaporation. Furthermore, the ability of microdroplets to stabilize reactive intermediates under mild conditions enables green synthesis approaches, significantly reducing the reliance on hazardous reagents, metal catalysts, and energy-intensive processes. Despite their enormous potential, microdroplets continue to face challenges related to scalability and process control. Ongoing advances in reactor design, thin-film deposition, solvent recycling, and computational modeling are steadily addressing these limitations. By bridging fundamental research with practical applications, microdroplets chemistry presents its unique value for green synthesis and sustainable chemical production, offering innovative solutions to global challenges across chemistry and related disciplines.

Over the past decade, microdroplet chemistry has rapidly developed in both fundamental properties and applications. In 2011, Cooks et al. first proposed the accelerated reaction characteristics of water microdroplets, laying the foundation for subsequent research.^[1] In the same year, Banerjee and co-workers reported unusual chemical transformations in electrosprayed droplets that are unattainable in the bulk phase, thereby highlighting the concept of the microdroplet as a “tiny reaction vessel.”^[2] In 2015, Zare's group first achieved the syntheses of isoquinoline and substituted quinolines under ambient conditions by leveraging the properties of microdroplets, providing a novel strategy of "tiny reaction vessels" for organic synthesis.^[3] In 2018, this group demonstrated that high electric fields and gas-liquid interfacial effects of microdroplets could significantly accelerate chemical reactions, and in the following year, they reported the spontaneous generation of H₂O₂ in water microdroplets.^[4-5] In 2020, the research teams led by Zare and Min Wei collaborated to determine that the electric field strength at the water microdroplets interface is on the order of 10⁹ V/m.^[6] In 2022, Zhang et al. experimentally captured free electrons and hydroxyl radicals on the interface of microdroplets, providing direct evidence for the interfacial effects in microdroplet chemistry.^[7] In the same year, the team of Teresa Head-Gordon computationally determined that the electric field on water microdroplet interfaces follows a Lorentzian distribution, averaging 1.6 × 10⁹ V/m.^[8] In 2024, Fan and coworkers integrated microdroplets with electrochemistry, employing them as microreactors to facilitate electrochemical reactions.^[9] In 2025, Zhang et al. further advanced the scale-up of microdroplets reactors, steadily propelling microdroplet technology toward industrial implementation.^[10]