Understanding electrochemical interfacial processes remains a fundamental challenge due to the multiscale spatiotemporal coupling (mass transport, momentum transport, electrochemical reaction, etc.) between the electrochemical double layer and bulk phases. By combining classical density functional theory and atomic structural information from first-principles calculations, we developed an electrochemical model that bridges atomic-scale interfacial phenomena with macroscopic electrochemical behavior at metal-aqueous solution interfaces under experimental conditions. Our model takes into account the critical interfacial effects, including microscopic double-layer effects, mesoscopic mass transfer, and macroscopic fluid flow. At the microscopic level, key interfacial effects include the quantum effects (metal's electron spillover, adsorption-induced effects of water molecules/ions), solution effects (excluded volume effect and dielectric saturation effect), and redox reactions. In particular, quantum effects are crucial for metal-aqueous solution interfaces. Our model successfully reproduces the experimental differential capacitance curves for the Ag electrode in dilute electrolytes, quantifying the contribution of these effects. Moreover, the study of the hydrogen evolution reaction in dilute electrolytes demonstrates an analytical capability for electrochemical polarization curves across varying experimental conditions. This computationally efficient model enables multiscale interface simulations under experimental conditions, which were previously inaccessible to either atomistic simulations or traditional continuum models. Thus, it provides an improved approach for investigating physicochemical processes in electrochemical systems for energy storage and microelectronics applications.

Intramolecular through-space charge-transfer (TSCT)-enabled thermally activated delayed fluorescence (TADF) emitters have shown exceptional potential for advancing organic light-emitting diode (OLED) technologies, owing to their efficient utilization of triplet excitons and optimized photophysical properties. To date, the intrinsic correlation among molecular geometries, intramolecular non-covalent interactions, and photophysical properties in TSCT-TADF emitters remains unconfirmed, and this study theoretically clarifies this critical correlation. Specifically, through integrating molecular engineering, screening strategies, first-principles calculations, energy decomposition analysis, and statistical modeling, we systematically investigated 24 experimentally reported TADF molecules, and 54 newly designed structures in both solution and thin-film environments. We establish a clear geometric criterion for high-efficiency TSCT-TADF emitters: donor-acceptor (D-A) dihedral angles below 25° and interfragment distances within 4 Å—conditions validated by both theoretical predictions and experimental evidence. Based on this insight, we designed two novel molecular libraries with benzene- or carbazole-derivative bridges, using O-bridged triphenylamine (DPXZ) as the donor and quinolino [3,2,1-de]acridine-5,9-dione (QAO) as the acceptor. Our calculations confirm that sub-25° D-A dihedral angles correlate with exceptional delayed fluorescence efficiency, with predictions reaching up to 96

Per- and polyfluoroalkyl substances (PFASs), colloquially termed "forever chemicals" due to their environmental persistence, are characterized by the inherent chemical stability that facilitates global dissemination and bioaccumulation, leading to their ubiquitous detection in environmental and biological matrices. Substantial concerns regarding the adverse health implications of traditional PFASs, notably perfluorooctanesulfonic acid (PFOS) and perfluorooctanoic acid (PFOA), which encompass multiple biological negative effects, have precipitated regulatory restrictions and phase-out. This regulatory shift has spurred the introduction of substitutes, yet emerging evidence indicates that these replacements have themselves become pervasive contaminants, such as chlorinated polyfluoroalkyl ether sulfonate (Cl-PFAES, F-53B) and hexafluoropropylene oxide dimer acid (HFPO-DA, Genx), which have been shown to possess toxicological profiles comparable to or exceeding those of their predecessors. The present review aims to comprehensively synthesize the current state of knowledge concerning the neurotoxicity of traditional and emerging PFASs, integrating insights from epidemiological studies, elucidation of central nervous system (CNS) penetration mechanisms, in vitro and in vivo neurotoxicological evidence, and proposed molecular pathways underlying neuronal damage. This review identifies critical, persistent knowledge gaps and proposes prioritized directions for future research endeavors aimed at elucidating and mitigating the neurological health risks presented by this ubiquitous class of contaminants.

The occurrence and environmental behavior of emerging contaminants have attracted increasing attention from environmental researchers worldwide. In this study, the spatial distribution, partition behavior, and potential environmental exposure risk of traditional (heavy metals, HMs) and emerging (organophosphate esters, OPEs; and per- and polyfluoroalkyl Substances, PFAS) contaminants in the surface water and sediments from three cities in Yunnan Province, China, were studied and compared. The total concentrations of the three kinds of contaminants in surface water and sediments showed a similar distribution, that is HMs (109 ± 149 μg/L in surface water, 2.1 ± 1.0 mg/g in sediments) > > OPEs (116 ± 56 ng/L, 8.8 ± 0.3 ng/g) > PFAS (2 ± 16 ng/L, 0.51 ± 0.44 ng/g), indicating that traditional contaminants HMs were still the predominant pollutants. The spatial distribution result and principal component analysis (PCA) showed a trend of that emerging contaminants (OPEs and PFAS) were higher in the northwest and traditional contaminants (HMs) were higher in the southeast. This indicated that the northwest was mainly affected by domestic pollution and the southeast by industrial pollution. The log values of the sediment–water partition coefficient Kd (log Kd) and organic carbon-corrected sediment–water partition coefficient Koc (log Koc) for HMs (4.6 ± 1.1, 6.4 ± 1.1) were significantly (P < 0.05) higher than those for PFAS (1.4 ± 0.4, 3.2 ± 0.4) and OPEs (1.7 ± 0.5, 3.5 ± 0.5), indicating that HMs were more likely to accumulate on solid phase particles than PFAS and OPEs in this field. The risk quotient (RQ) results showed that the aquatic ecological RQs of emerging pollutants PFAS and OPEs in the study area were all below 1, while the risk of HMs was high which should to be concerned.

As high emissivity emitters, traditional pseudobrookite ceramics are limited in thermal protection applications due to their structure degradation at high temperatures. In this work, a high-entropy pseudobrookite, (Mg,Co,Ni, Zn)Ti2O5, was designed, and CoTi2O5 was selected as a single-component counterpart to evaluate the high-entropy effect on phase stability and emissivity. After heating at 1400 degrees C for 15 h, (Mg,Co,Ni,Zn)Ti2O5 retained a single pseudobrookite phase with nearly unchanged emissivity, whereas CoTi2O5 exhibited obvious phase degradation and emissivity deterioration. The higher 2.5-7 mu m emissivity of (Mg,Co,Ni,Zn)Ti2O5 was attributed to its narrower band gap (2.66 eV) and a higher oxygen vacancy fraction (56.87%). When coated on alumina-silica fiber fabric, the (Mg,Co,Ni,Zn)Ti2O5 coating exhibited improved thermal-protection performance owing to its high infrared emissivity and reduced heat conduction, while maintaining good mechanical properties after heat treatment. These results demonstrate that (Mg,Co,Ni,Zn)Ti2O5 is a promising high-emissivity ceramic for extreme thermal environments.

All-inorganic gold halide perovskites exhibit excellent stability and tunable bandgaps, positioning them as environmentally sustainable alternatives to organic-inorganic lead halide perovskites in photovoltaics. A mechanistic understanding of how crystal phase and composition engineering regulates multi-level structural and electronic properties-thereby determining charge recombination dynamics and overall performance-requires systematical investigation. In this study, we synthesized Rb2Au2I6via hydrothermal methods, identifying a previously unreported monoclinic primitive (mP) phase, which is distinct from the known monoclinic C-centered (mC) phase. Additionally, we designed six partially chloride-substituted derivatives of Rb2Au2I6 with distinct space groups to facilitate bandgap tunability and optimize charge carrier dynamics. We employed multiscale simulations, combining first-principles calculations (HSE06 functional with spin-orbit coupling) and device-scale continuum models, to clarify the relationships among different crystal phases, compositional engineering, charge-carrier transport, and device performance. Our analysis identified mC-Rb2Au2Cl4I2 and mP-Rb2Au2Cl2I4 as optimal compositions, demonstrating superior thermal stability and optoelectronic properties. Device-scale modeling incorporating cross-scale parameter transfer reveals the kinetic mechanisms linking non-radiative recombination and charge transport imbalance. This approach directly predicts a power conversion efficiency of 20.42% for mC-Rb2Au2Cl4I2 under operating conditions. This study establishes a comprehensive, mechanism-guided roadmap for the rational design of high-efficiency, stable, all-inorganic gold halide perovskite materials through synergistic crystal phase and composition engineering.

For continuing to explore new high-entropy materials, the first high-entropy ilmenite-phase titanate, (Mg,Co,Ni, Zn)TiO3, is synthesized in this work, further introducing a new crystal structure type for high-entropy ceramics. The uniform chemical composition and typical ilmenite-phase structure of high-entropy (Mg,Co,Ni,Zn)TiO3 are verified by XRD, SEM, TEM, EDS, and XPS. Homogeneous element distribution and magnetically-coupled atomic arrangement are further performed using Rietveld refinement, Raman spectral fitting, and high-resolution STEM. On this basis, complementary density functional theory simulation with Hubbard correction (DFT + U) is conducted to reveal the band structure and a 2.529 eV bandgap of high-entropy (Mg,Co,Ni,Zn)TiO3, thereby enhancing the potential for high emissivity and electronic applications. Excellent thermal stability at 1000-1200 degrees C, a low thermal conductivity of 2.365 W & sdot;m-1 & sdot;K-1 at room temperature, a high hemispherical emissivity of 0.93 within the 3-14 mu m wavelength range, and a low dielectric constant of 22.23 are also demonstrated.

The complete miscibility of polar N,N-dimethylformamide (DMF) with nonpolar benzene (PhH) challenges the classic "like-dissolves-like" principle, highlighting the need for a molecular-level understanding. By synergistically combining multiple research methods, we identified amide-π interactions as the pivotal driving force of this miscibility. First-principles calculations revealed a near-parallel DMF-PhH alignment resembling biological motifs. Meanwhile, the interaction energy of this amide-π stacking was intermediate between those of PhH-PhH (π-π stacking) and water-water (hydrogen bonding) systems. Energy decomposition analysis quantitatively indicated the hybrid nature of amide-π interactions arising from a combination of correlation/dispersion and electrostatics forces. We further demonstrated this interaction's structural dominance and generality through statistical analysis of the Cambridge Structural Database. This work not only resolves the DMF-PhH miscibility paradox but also establishes amide-π interactions as a universal solvation mechanism, providing theoretical guidance for the rational solvent screening in synthetic chemistry.

The exceptional energy density and stability of fluorinated carbon (CFx) cathode materials have shone brightly in the field of Li primary batteries. However, the development of Li/CFx secondary batteries has hit a bottleneck due to the high dissociation energy and band gap energy of LiF. Herein, a fluorinated biomass hard carbon (FTS/Ni), with Ni functional layer rich in catalytic active sites deposited on CFx surface via magnetron sputtering, is synthesized, showing high reversibility of lithium ions storage. FTS/Ni cathode with 1.5 wt% Ni content exhibits high capacity of 250 mAh g-1 within voltage window of 1.5-5.0 V. Density functional theory (DFT) calculations confirm that Ni catalyst could reduce the dissociation energy of LiF, accelerating the conversion kinetics of LiF, thereby enhancing the secondary electrochemical performance of Li/CFx batteries. This work demonstrates that the reversibility of LiF within the voltage window of 1.5-5.0 V can be achieved through Ni catalytic action, pointing out a promising direction for the secondary rechargeability of Li/CFx batteries.

KVPO4F (KVPF) is a novel insertion-type anode for potassium ion batteries. For improving its electrochemical performance, the doping strategy was selected and a series of Fe-doped KVPF materials were synthesized by a facile solid-state sintering method to find out the suitable ratio. After comparation, KVPF sample with 5 % Fe-doped ratio (KVPF/Fe-5) delivers the best performance, e.g. rate capacity (94.3 mA h g-1 at 500 mA g-1) and long-term discharge capacity (74.1 mA h g-1 after 1000 cycles at 200 mA g-1, 0.03 % capacity decay ratio per cycle), which is mainly attributed to its larger K+ diffusion rate. The in-situ X-ray diffraction analysis clarify the two-step K+ storage mechanism of KVPF/Fe-5 anode, and the density functional theory calculations verify that Fe-doping can reduce diffusion energy barrier of K+ and increase electronic conductivity of KVPF. When used as cathode, KVPF/Fe-5 delivers 51.8 mA h g-1 at 100 mA g-1 after cycling 200 cycles. In addition, the symmetric cell by employing KVPF/Fe-5 as anode and cathode simultaneously was also assembled successfully, pointing out a new research direction for potassium-ion batteries.

Singlet fission (SF) is a process in which the absorption of a single photon results in the generation of a pair of triplet excited states, showing potential for enhancing solar conversion efficiency. The thermodynamic driving force behind SF is determined by the energy difference between the first singlet excited state and the first triplet excited state, denoted as ΔE1 = E(S1) - 2E(T1). In general, an excessively large ΔE1 value (i.e., excessive exoergicity) can facilitate alternative relaxation pathways for excitons, thereby diminishing SF efficiency. Consequently, when designing high-efficiency SF chromophores, optimization of ΔE1 becomes crucial. Herein, we introduce a helically locked tethering strategy to optimize ΔE1 for low-efficiency SF chromophores. Specifically, different dihedral angles are induced by tethering tethers of different lengths (Cn = -(CH2)n-, n = 1-6) to tetraazaacenes, allowing us to systematically monitor the variational characteristic as a function of the dihedral angle. Tethered products show strong chirality with a high energy barrier to twist back and forth. A tunable ΔE1 has been realized by adjusting the tether length, allowing us to identify the optimal ΔE1 of 0.29, 0.26, and 0.11 eV at tether lengths of n = 3 or 2. Our results suggest that this strategy could be applied to existing low-efficiency SF databases that are not typically considered for future application in the SF field, thereby creating novel high-efficiency and stable SF chromophores. This strategy not only makes full use of the existing resources but also greatly expands the SF arsenal.

Small chiral metabolic molecules are increasingly recognized as pivotal biomarkers for disease monitoring and treatment. Here, a wearable microfluidic patch is presented that integrates chiral 3D plasmonic nanostructures with surface-enhanced Raman spectroscopy (SERS) sensing activity for the in situ and real-time metabolic profiling of chiral molecules in sweat. The microfluidic patch is designed for the direct, in situ capture and storage of microliter volumes of sweat. By exploiting the 3D chiral plasmonic coupling interactions within the nanostructures, the integrated SERS sensor on the patch allows for highly sensitive and quantitative enantiomer detection through their unique fingerprint SERS spectra. In a proof-of-concept demonstration, the first in situ, real-time quantitative detection of chiral drug metabolite and pH in human sweat using this device is successfully conducted. This capability enables the capturing of an individual's dynamic metabolic profile. Leveraging this solution, pharmacokinetic correlations are established, showcasing the potential application of the device in assessing human health.

Lithium/fluorinated carbon (Li/CFx) battery possesses ultra-high energy density, yet the poor conductivity of CFx pose certain limitations on its electrochemical performance. In this work, a CF1.05-SeS2 composite material with both high energy density and power density is prepared. The abundant pore structure of CF1.05 provides ample space for the loading of SeS2 and numerous reaction sites for electrochemical reactions. During 70 % of the discharge depth of CFx, SeS2 can participate the discharge reaction, further enhancing its discharge performance. The CF1.05-SeS2 exhibits excellent electrochemical performance, with maximum energy density reaching 2534 Wh kg-1 and maximum power density of 57,725 W kg- 1 simultaneously. Density functional theory (DFT) calculations reveal that the introduction of SeS2 can reduce the Lithium-ion diffusion energy barrier and increase the Lithium-ion adsorption energy. This work provides new insights into modifying CFx materials to enhance their energy density and power density.

One of the most critical challenges in organic light‐emitting diodes (OLEDs) is the development of efficient blue emitters, which require high exciton utilization efficiency, short exciton lifetime, and well‐balanced carrier mobility. Herein, a blue hot exciton emitter, TPA‐SBF‐OXZ, is synthesized by incorporating a triphenylamine donor and an oxadiazole acceptor into the spirobifluorene (SBF) skeleton. TPA‐SBF‐OXZ exhibits a high photoluminescence quantum yield of 70.7%, and balanced hole and electron mobilities in neat film. Additionally, due to the anti‐aggregation‐caused‐quenching characteristics of the SBF skeleton, the non‐doped OLED achieves a maximum external quantum efficiency (EQE) of 10.6% at 2396 cd cm −2 and 10.2% even at 11181 cd cm −2 , ranking the leading position in non‐doped blue fluorescent OLEDs. The proof‐of‐concept phosphorescent OLED using TPA‐SBF‐OXZ as host achieves remarkable performance metrics, including an ultra‐low turn‐on voltage of 2.2 V, a high EQE of 30.4%, a maximum power efficiency of 109.1 lm W −1 , and an exceptionally high luminance of over 130000 cd m −2 . This work offers a feasible approach for the development of high‐performance non‐doped blue electro‐fluorescence and low power‐consumption PhOLEDs.

Luminescent metal halides have garnered significant attention due to their tunable emission characteristics and exceptional optoelectronic properties. Nevertheless, achieving metal halides that exhibit near-infrared (NIR) emission upon blue-light excitation remains a significant challenge. In this study, blue-light-induced NIR emission was successfully realized in the zero-dimensional (0D) (BTP)2ZnBr4:Sb3+ single crystal [BTP+:(3-Bromopropyl) triphenylphosphonium cation] via a straightforward energy transfer from the host (BTP)2ZnBr4 to the self-trapped exciton (STE) state generated by Sb3+. Upon excitation with blue light, (BTP)2ZnBr4:12.5 % Sb3+ exhibits broad NIR emission characterized by a peak at approximately 725 nm, a Stokes shift of about 295 nm, and a notably large full width at half maximum (FWHM) of 179 nm. Additionally, the analysis of experimental data in conjunction with density functional theory (DFT) calculations elucidated the blue light emission mechanism of the host as well as the doped NIR emission. The study demonstrated potential night vision applications by utilizing the (BTP)2ZnBr4:12.5 % Sb3+ phosphor combined with a 430 nm light-emitting diode (LED) chip in the dark.

Multi-resonance thermally activated delayed fluorescence (MR-TADF) materials have emerged as promising emitters for organic light-emitting diodes (OLEDs) due to their highly efficient narrow-band emission. Peripheral structure modification represents a simple and feasible strategy to improve the luminescence properties of MRTADF materials. Herein, we report two TADF materials, NBO-Ac and NBO-PXZ, which are synthesized by incorporating electron-donor groups with varying electron-donating abilities at the para-position of the boron atom in a boron/nitrogen/oxygen ternary-doped MR framework (NBO). Both theoretical and experimental studies demonstrate that modification of the peripheral donor groups effectively regulates the excited states, thereby influencing the photoluminescence and electroluminescence (EL) properties of these materials. Incorporating the moderate-strength donor dimethylacridine effectively accelerates the reverse intersystem crossing process by introducing intermediate long-range charge transfer (LRCT) states, while simultaneously preserving the narrow-band deep-blue emission from short-range charge transfer (SRCT) states, in comparison to the parent molecule NBO. In contrast, the incorporation of a stronger donor, phenoxazine, results in a significantly stabilized emissive singlet state with predominant LRCT characteristics, leading to broader and redshifted emission. Moreover, incorporating peripheral donor units can significantly increase the ratio of horizontal transition dipole orientation of these emitters in films. Consequently, both the NBO-Ac-based deep-blue OLEDs and the NBO-PXZbased sky-blue OLEDs exhibit EL performance far superior to that of the control NBO-based devices. The unsensitized and sensitized OLEDs using NBO-Ac as the emitter achieve EQEs of 32.0% and 33.6%, with Commission Internationale de L'Eclairage (CIE) coordinates of (0.134, 0.097) and (0.137, 0.106), respectively.

All-polymer organic photovoltaics (OPV) demonstrate remarkable potential for simultaneous lightwave information and power transfer (SLIPT), enabling integrated energy harvesting and high-speed optical communication. Through innovative cathode interfacial layer (CIL) engineering, we have developed a breakthrough approach to optimize the interface contact between the active layer and electrode in all-polymer OPVs. By employing PNDIT-F3N as the CIL, we achieved stable OPVs with exceptional performance metrics: a power conversion efficiency of 15.16% (AM 1.5G) and 17.71% (indoor lighting), coupled with a device bandwidth of 3.4 MHz. In optical wireless communication tests, our optimized devices attained a record peak communication rate of 70.3 Mbps at 1.8 meter transmission distance while maintaining a bit error rate of 3.010 ?3 and simultaneous energy harvesting of 3.13 mW. This breakthrough in CIL engineering not only enhances wireless data communication capabilities but also paves the way for developing self-powered optical communication systems, offering significant potential for extending battery lifespan in mobile devices and advancing energy-efficient communication technologies.

BT.2020‐compliant deep‐blue emitters for organic light‐emitting diodes (OLEDs) are in high demand to achieve a wide color gamut for ultrahigh‐definition displays. Herein, we report deep‐blue thermally activated delayed fluorescent emitters featuring a unique donor1‐donor2‐acceptor (D 1 ‐D 2 ‐A) molecular configuration in which C 1 ‐N linked carbazole derivatives serve as dual‐function donors and an oxygen‐bridged triarylboron unit acts as the acceptor. The new design strategy focuses on constructing excited states with multipathway charge transfer characteristics—including multiresonance, through‐bond, and through‐space charge transfer—by precisely tuning the relative electron‐donating strengths of the D 1 and D 2 units. Experimental and theoretical studies reveal that the optimized emitter, BO‐BTC, achieves a well‐balanced trade‐off among emission efficiency, color purity, singlet–triplet energy gap, and horizontal dipole orientation ratio. Consequently, OLEDs using BO‐BTC as the terminal emitter or as the sensitizer for ν ‐DABNA achieve high‐efficiency deep‐blue electroluminescence, with external quantum efficiencies of up to 24.7% and 37.9%, Commission Internationale de l’Éclairage‐y values of 0.038 and 0.106, respectively.

Manganese halides are emerging as promising alternatives to traditional inorganic phosphors and X-ray scintillators due to their low toxicity, high attenuation coefficients, high light yield, and cost-effective solution-processability. We synthesized a novel manganese chloride, (4CTP)2MnCl4 (4CTP = (4-chlorobenzyl)triphenylphosphonium), via solvent volatilization. The crystal exhibits a narrow-band (∼48 nm) green emission at 516 nm under ultraviolet or blue light excitation, attributed to the Mn2+ d-d transition, with a photoluminescence quantum yield (PLQY) of 95.7% and a nearest Mn···Mn distance of 9.909 Å. A white light-emitting diode (LED) for backlight displays was fabricated using (4CTP)2MnCl4, a 450 nm blue LED chip, and K2SiF6: Mn4+, achieving a color gamut of 112.1% at 20 mA. Substituting the red phosphor with (Sr, Ca)AlSiN3: Eu2+ produced a white LED for solid-state lighting with a color rendering index (CRI) of 92.4 and a correlated color temperature (CCT) of 4097 K. The crystal also demonstrated excellent X-ray scintillation properties (a light yield of 63,400 photons/MeV). A flexible (4CTP)2MnCl4@PMMA film enabled high-resolution X-ray imaging (10.4 lp/mm). This work showcases a simple route to develop high-performance manganese halides for LEDs and X-ray imaging.

We present a theoretical design for a series of multifunctional nanomaterials that exhibit superior performance in singlet fission (SF) as well as exceptional nonlinear optical (NLO) performance. Our study focuses on a systematic investigation into the aromaticity, diradical character, excited state transition and (hyper)polarizability of the [n]benzocyclobutadiene carbon nanobelt system. To provide further guidance for designing multifunctional nanomaterials, our quantum chemical calculations propose empirical rules regarding the influence of aromatics on SF and NLO: Through an exploration of SF properties, we observed significant diradical character with radical sites exclusively located at anti-aromatic positions. Furthermore, these anti-aromatic positions serve as transition sites for excited state transitions to achieve the necessary low triplet excited states energy for SF. Then, by conducting calculations on NLO properties, we ascertain that the main tensor components of first-order hyperpolarizability (beta total) and second-order hyperpolarizability (gamma total) come from the anti-aromatic region. However, there exists a contrasting impact of anti-aromaticity on first- and second-order hyperpolarizability density. The positive and negative contributions to first-order hyperpolarizability density mainly come from both aromatic and anti-aromatic regions while for second-order hyperpolarizability density it is contradictory. This study elucidates the role of aromatic sites in multifunctional nanomaterials with respect to diradical sites, excited state transition regions, and (hyper)polarizability density distribution.