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Flat bands and nontrivial topological physics are two important topics of condensed matter physics. With a unique stacking configuration analogous to the Su-Schrieffer-Heeger model, rhombohedral graphite (RG) is a potential candidate for realizing both flat bands and nontrivial topological physics. Here, we report experimental evidence of topological flat bands (TFBs) on the surface of bulk RG, which are topologically protected by bulk helical Dirac nodal lines via the bulk-boundary correspondence. Moreover, upon in situ electron doping, the surface TFBs show a splitting with exotic doping evolution, with an order-of-magnitude increase in the bandwidth of the lower split band, and pinning of the upper band near the Fermi level. These experimental observations together with Hartree-Fock calculations suggest that correlation effects are important in this system. Our results demonstrate RG as a platform for investigating the rich interplay between nontrivial band topology, correlation effects, and interaction-driven symmetry-broken states., Competing Interests: Competing interests statement:The authors declare no competing interest.

Catalytic removal of alkynes is essential in industry for producing polymer-grade alkenes from steam cracking processes. Non-noble Ni-based catalysts hold promise as effective alternatives to industrial Pd-based catalysts but suffer from low activity. Here we report embedding of single-atom Pd onto the NiGa intermetallic surface with replacing Ga atoms via a well-defined synthesis strategy to design Pd 1 -NiGa catalyst for alkyne semi-hydrogenation. The fabricated Pd 1 Ni 2 Ga 1 ensemble sites deliver remarkably higher specific mass activity under superb alkene selectivity of >96 % than the state-of-the-art catalysts under industry-relevant conditions. Integrated experimental and computational studies reveal that the single-atom Pd synergizes with the neighbouring Ni sites to facilitate the σ-adsorption of alkyne and dissociation of hydrogen while suppress the alkene adsorption. Such synergistic effects confer the single-atom Pd on the NiGa intermetallic with a Midas touch for alkyne semi-hydrogenation, providing an effective strategy for stimulating low active Ni-based catalysts for other selective hydrogenations in industry., (© 2024 Wiley-VCH GmbH.)

Hole transport materials (HTMs) are essential for improving the stability and efficiency of perovskite solar cells (PSCs). In this study, we have designed and synthesized a novel organic small molecule HTM, cor-(DPA)5, characterized by a bowl-shaped core with symmetric five diphenylamine groups. Compared to already-known HTMs, the bowl-shaped and relatively compact structure of cor-(DPA)5 facilitates intermolecular π-π interactions, promotes film formations, and enhances charge transport. Consequently, the cor-[DPA(2)]5 HTM exhibits high charge mobility, exceptional hydrophobicity, and a significantly elevated glass transition temperature. Superior to previously reported HTMs such as spiro-OMeTAD and cor-OMePTPA, our newly synthesized cor-(DPA)5 HTM is free from any ionic dopants. As a result, the dopant-free cor-[DPA(2)]5-based PSC demonstrates an impressive efficiency of 24.01%, and exhibits outstanding operational stability. It retains 96% after continuous exposure to 1 sun irradiation for 800 hours under MPP (maximum power point) tracking in ambient air. These findings present a structurally compact novel HTM and exemplify a new approach to the molecular design of HTM for the development of stable and effective PSCs., (© 2024 Wiley‐VCH GmbH.)

The pursuit of sustainable practices through the chemical recycling of polyamide wastes holds significant potential, particularly in enabling the recovery of a range of nitrogen-containing compounds. Herein, we report a novel strategy to upcycle polyamide wastes to tertiary amines with assistance of H2 in acetic acid under mild conditions (e.g., 180 ºC), which is achieved over anatase TiO2 supported Mo single atoms and Rh nanoparticles. In this protocol, the polyamide is first converted into diacetamide intermediates via acidolysis, which are subsequent hydrogenated into corresponding carboxylic acid monomers and tertiary amines in 100% selectivity. It is verified that Mo single atom and Rh nanoparticles work together to activate both amide bonds of the diacetamide intermediate, and synergistically catalyze its hydrodeoxygenation to form tertiary amine, but this catalyst is ineffective for hydrogenation of carboxylic acid. This work presents an effective way to reconstruct various polyamide wastes into tertiary amines and carboxylic acids, which may have promising application potential., (© 2024 Wiley‐VCH GmbH.)

The geochemical composition of sediment cores can serve as a proxy for reconstructing past human and nature-driven environmental and climatic changes. We investigated the temporal variation in the concentrations and fluxes of polycyclic aromatic compounds (PACs) which include polycyclic aromatic hydrocarbons (PAHs), oxygenated PAHs, and azaarenes in the Sihailongwan Maar Lake and found that they remained low before 1950. The PAC concentrations and fluxes increased substantially since 1950, which was in good agreement with the fast socio-economic development, industrialization, and associated growth in fossil fuel consumption in China, particularly since the 1980s. After 2010, the PAC fluxes decreased, which was consistent with the implementation of air pollution control policies in China at that time. The concentration ratios of the sums of low to high molecular weight PAHs (LMW-PAHs/HMW-PAHs), benzo[ e ]pyrene/benzo[ a ]pyrene, and benzo[ a ]anthracene-7,12-dione/benzo[ a ]anthracene all decreased from bottom to top of the sediment core, reflecting the rapidly increasing contribution of emissions derived from high-temperature fossil fuel combustion (energy, transport and industry) to the PAC emissions in recent times at the expense of biomass burning. In addition, these data reflect the increasing local sources of PACs in more recent times because of the enhanced human activities in the area surrounding the Maar lake. Our results demonstrate that PAC fluxes and concentrations in sediment cores reflect the regional and national economic development and the efficiency of pollution control measures.

On-surface molecular self-assembly presents an important approach to the development of low-dimensional functional nanostructures and nanomaterials. Traditional strategies primarily exploit hydrogen bonding or metal coordination, yet the potential of chalcogen bonding (ChB) for on-surface self-assemblies remains underexplored. Here, we explore fabricating molecular networks via tellurium (Te)-directed chalcogen-organic interactions. Employing carbonitrile molecules as molecular building blocks, we have achieved extended 2D networks exhibiting a 4-fold binding motif on Au(111), marking a notable difference from the conventional coordinative interaction involving transition metals. Our findings, supported by density functional theory (DFT) and scanning tunneling spectroscopy (STS), show that the Te-carbonitrile interaction exhibits lower stability compared to the metal-organic coordination, and the construction of the Te-directed molecular networks does not alter the electronic properties of the involved molecules. Introducing chalcogen-directed interactions may expand the spectrum of strategies in supramolecular assembly, contributing to the design of advanced molecular architectures for nanotechnological applications.

Perovskite solar cells (pero-SCs) have undergone a rapid development in the last decade. However, there is still a lack of systematic studies to investigate whether the empirical rules of working lifetime assessment used in silicon solar cells can be applied to pero-SCs. It is commonly believed that pero-SCs show enhanced stability under day/night cycling due to the reported self-healing effect in the dark. 1,2 While we discovered that the degradation of highly efficient FAPbI 3 pero-SCs is in fact much faster under natural day/night cycling mode, questioning the widely accepted approach to estimate the operational lifetime of pero-SCs based on continuous mode testing. We reveal the key factor to be the lattice strain caused by thermal expansion/shrinking of the perovskite during the operation, an effect that gradually relaxes under the continuous-illumination mode but cycles synchronously under the cycling mode. 3,4 The periodic lattice strain under the cycling mode results in deep trap accumulation and chemical degradation during operation, decreasing the ion migration potential and hence the device lifetime. 5 We introduce phenylselenenyl chloride (Ph-Se-Cl) to regulate the perovskite lattice strain during day/night cycling, which achieved the certified efficiency of 26.3% and a 10-time improved T 80 lifetime under the cycling mode after the modification., (© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)

Exploring high-performance and low-platinum-based electrocatalysts to accelerate the oxygen reduction reaction (ORR) at the air cathode of zinc-air batteries remains crucial. Herein, by combining electroless deposition and carbothermal reduction, a nitrogen-doped carbon-supported highly dispersed PtSn alloy nanocatalyst (PtSn/NC) was prepared for a high-efficiency ORR process. Electrochemical measurements show that PtSn/NC exhibits excellent electrocatalytic ORR activity with a half-wave potential of 0.850 V versus reversible hydrogen electrode (RHE), which is higher than that of commercial Pt/C (0.815 V). The PtSn/NC-based (20 μg Pt cm -2 ) rechargeable Zn-air battery exhibited astonishing performance with a maximum power density of up to 150.1 mW cm -2 , as well as excellent rate performance and charge/discharge stability. Physical characterization reveals that carbothermal reduction could compel the transformation of Sn oxide into metallic Sn, which then alloys with the deposited Pt atoms to form the PtSn nanoalloy, in which electrons are transferred from Sn atoms to neighboring Pt atoms, thereby improving the ability of Pt-based active sites to catalyze the ORR process in PtSn/NC by optimizing the unoccupied d -band of Pt atoms. This work provides a reliable and innovative route for the rational design of highly dispersed Pt-based alloy ORR electrocatalysts.

Grain boundaries (GBs) and surface defects within perovskite films are inherent challenges that affect the photovoltaic performance of perovskite solar cells  (PSCs. In this work, Nylon 11 (N11) is utilized, a long-chain polymer, for post-treating the GBs and surface defects within FAPbI 3 films. The multifunctional groups of N11 exhibit unique passivation abilities, enabling self-regulation and selective correction of reverse-charged defects. Post-treating with N11 results in high-quality FAPbI 3 films characterized by tight GBs and low surface defect density. Despite fabrication under full open-air conditions, the N11 post-treatment significantly enhances the power conversion efficiency (PCE) value of FAPbI 3 PSCs, increasing it from the reference value of 21.89% to 23.54%. Importantly, the long alkyl chain present in N11 significantly enhances the humidity stability of the PSCs. Unencapsulated PSCs treated with N11 maintain 89% of their initial PCE after exposure to air with 30% relative humidity (RH) for 1000 h, demonstrating resilience to elevated humidity levels. This work highlights the substantial improvement in the photovoltaic performance of PSCs achieved through the post-treatment with N11., (© 2024 Wiley‐VCH GmbH.)

Speech features have been investigated as novel digital biomarkers for many psychiatric and neurocognitive diseases. Microphones are the most used devices for speech recording but inevitably suffering from several disadvantages such as privacy leakage and environmental noises, limiting their clinical applications particularly for long-term ambulatory monitoring. The aim of the present study is therefore to explore the feasibility of extracting speech features from the acceleration recorded on the sternum. Ten healthy subjects volunteered in our study. Two speech tasks, that is, repeating one sentence 20 times and reading 20 different sentences, were performed by each subject, with each task repeated eight times under different speech rate and loudness. Voice signals and speech-caused chest vibrations were simultaneously recorded by a microphone and an accelerometer placed on the sternum. Forty-two acoustic features and six time-related prosodic features were extracted from both signals using a standard toolbox, and then compared by a linear fit and correlation analysis. Good agreement between the acceleration features and microphone features is observed in all six time-related prosodic features for both tasks, but only in 19 and 17 acoustic features for task 1 and 2, respectively, with most of them loudness- or pitch-related. Our results suggest the sternum acceleration to track time-related speech prosody, loudness, and pitch very well, demonstrating the feasibility of deriving digital biomarkers from the acceleration signal for diseases strongly related to time-related prosodic and loudness features., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 The Voice Foundation. Published by Elsevier Inc. All rights reserved.)

Ionic hybrid perovskites face challenges in maintaining their structural stability against non-equilibrium phase degradation, therefore, it is essential to develop effective ways to reinforce their corner-shared [PbI 6 ] 4- octahedral units. To strengthen structural stability, redox-active functional polyoxometalates (POMs) are developed and incorporated into perovskite solar cells (PSCs) to form a robust polyoxometalates/perovskite interlayer for stabilizing the perovskite phase. This approach offers several advantages: 1) promotes the formation of an interfacial connecting layer to passivate interfacial defects in addition to stabilize the [PbI 6 ] 4- units through exchanged ammonium cations in POMs with perovskites; 2) facilitates continuous structural repairing of Pb 0 - and I 0 -rich defects in the [PbI 6 ] 4- unit through redox electron shuttling of the electroactive metal ions in POMs; 3) provides guidance for selecting suitable redox mediators based on the kinetic studies of POM's effectiveness in reacting with targeted defects. The POM-reinforced device maintains 97.2% of its initial PCE after 1500 h of shelf-life test at 65 °C, while also enhancing the long-term operational stability. Additionally, this approach can be generally applicable across scalable sizes and various bandgap perovskites in devices, showing the promise of using functional POMs to enhance perovskite photovoltaic performance., (© 2024 Wiley‐VCH GmbH.)

Atomically dispersed transition metal sites on nitrogen-doped carbon catalysts hold great potential for the electrochemical CO 2 reduction reaction (CO 2 RR) to CO due to their encouraging selectivity. However, their intrinsic activity is restricted by the hurdle of the high energy barrier of either *COOH formation or *CO desorption due to the scaling relationship. Herein, we discover a p-block aluminum single-atom catalyst (Al-NC) featuring an Al-N 4 site that enables disentangling this hurdle, which endows a moderate reaction kinetic barrier for *COOH formation and *CO desorption, as validated by in situ attenuated total reflection infrared spectroscopy and theoretical simulations. As a result, the developed Al-NC shows a CO Faradaic efficiency (FE CO ) of up to 98.76% at -0.65 V vs RHE and an intrinsic catalytic turnover frequency of 3.60 s -1 at -0.99 V vs RHE, exceeding those of the state-of-the-art Ni-NC and Fe-NC counterparts. Moreover, it also delivers a partial CO current of 309 mA·cm -2 at 93.65% FE CO and 605 mA at >85% FE CO in a flow cell and membrane electrode assembly (MEA), respectively. Strikingly, when using low-concentration CO 2 (30%) as the feedstock, this catalyst can still deliver a partial CO current of 240 mA at >80% FE CO in the MEA. Considering the earth-abundant character of the Al element and the high intrinsic activity of the Al-NC catalyst, it is a promising alternative to today's transition metal-based single-atom catalysts.

The aqueous zinc-ion batteries (AZIB) have emerged as a promising technology in the realm of electrochemical energy storage. Despite its potential advantages in terms of safety, cost-effectiveness, and inherent safety, AZIB faces significant challenges. Issues attributed to unsupported thermodynamics and non-uniform potential distribution and deposition, present formidable obstacles that necessitate resolution. To tackle these challenges, a novel strategy adapting hybrid organic-inorganic in-situ derived solid-to-hydrogel electrolyte interface (StHEI) has been developed from coordination reactions and self-respiratory process, establishing uniform diffusion channels by ion bridges and accelerating ion transport. Self-respiratory pattern of StHEI realized through in-situ inorganic component conversion further prolongs the protecting duration, which effectively mitigates corrosion and passivation but enhance the mechanical properties of the StHEI measured through Young's modulus. This novel StHEI promotes well-distributed potential lines within the Helmholtz regions. Zn2+ are finally induced to deposit and nucleate in a compact, fine, and uniform manner. Asymmetrical batteries assembled with the modified Zn electrode and bare Zn exhibit exceptional stability over 3000 h (1 mA cm-2- 0.5 mAh cm-2). The asymmetrical Cu//Zn cell achieved an outstanding average Coulombic efficiency (CE) of 99.6% over 1200 cycles., (© 2024 Wiley‐VCH GmbH.)

In this work, poly(l-lactic acid) (PLLA) Janus shape memory membranes with uniform vertically penetrative channels (SMEUVs) with slit pores have been fabricated with the help of template-assisting spray-coating and uniaxial tension at high temperature. During fog collection, superhydrophobic and hydrophilic surfaces act as the front (fog-facing) side and back side, respectively, in which the structural characteristics play essential roles. On one hand, the vertically penetrative channels in SMEUVs and the special pore geometry contribute to lower resistance, accelerating the transport of captured water through membranes (from the superhydrophobic side to the hydrophilic side). On the other hand, the movement of water droplets along the back side has been guided by the oriented structures of slit pores, promoting the detachment of droplets from the hydrophilic surface. Their synergistic effect removes captured water in a timely manner and provides fresh sites for the subsequent nucleation of water, enhancing fog collection performance. As a result, the optimal specimen (Janus SMEUVs with a draw ratio of 2.5, placed in the parallel direction) exhibits a much higher water collection rate (∼6×) relative to references (superhydrophobic and hydrophilic membranes). Our results are significant for sustainable development in view of both fog collection in arid regions and the biodegradability of PLLA.

Salt efflorescence is one of the major hazards to cultural heritages, masonries, and highways etc. It is now generally accepted that damages caused by salt efflorescence are mainly due to continuous cycles of salt crystallization/dissolution or hydration/dehydration in confined spaces. The position where salt efflorescence occurs and its type are closely related to the degree of damages caused by salt efflorescence. It is known that water is the key environmental factor determining the salt crystallization position. But influence of the correlation between water supply and evaporation on the position of salt crystallization is still not clearly understood. In this work, a set of experiments are designed to investigate salt efflorescence in porous matrix. It is found that the types and positions of salt efflorescence have little to do with nucleation, but are mainly governed by crystal growth, which is controlled by the rates of water evaporation, water and salt supply, capillary forces and surface properties of the porous matrices., (© 2024. The Author(s).)

Finely tuning the pore structure of traditional nanofiltration (NF) membranes is challenging but highly effective for achieving efficient separations. Herein, we propose a concept of using macrocyclic amines (1,4,7-triazacyclononane, 3A; 1,4,7,10-tetraazacyclododecane, 4A1; and 1,4,8,11-tetraazacyclotetradecane, 4A2) with different intra-annular apertures to finely modulate the pore structure of microporous membranes via interfacial polymerization (IP). The boost in the intracavity size of the building blocks results in heightened steric hindrance of these amine monomers, leading to a controlled increase in membrane pore size, as demonstrated by both film characterizations and multiscale simulations. In conjunction with the increased intracavity size, the water permeability follows an augmented trend of 3A-TMC, 4A1-TMC, and 4A2-TMC (TMC: trimesoyl chloride) while exhibiting increased molecular weight cut-offs due to larger free-volume elements and stronger pore interconnectivity. Our proposed macrocyclic amine design strategy provides a guideline for finely regulated microporous membranes with high potential in NF-related applications.

Urea synthesis under mild conditions starting from the electrocatalytic coupling of carbon dioxide (CO 2 ) and nitrate represents a promising alternative experimentally to conquer the huge energy consumption in the industrial Haber-Bosch process. Herein, an electrocatalyst consisting of CuRu alloy nanoparticles on carbonized cellulose (CuRu-CBC) is designed and realizes the urea yield rate of 394.85 ± 16.19 μg h -1 mg cat -1 and an ultrahigh faradaic efficiency (FE) of 68.94 ± 3.05% at -0.55 V ( vs. RHE) under ambient conditions. Further XAS analyses indicated that the favored internal electron transfer between Cu and Ru dual active sites significantly improved the C-N coupling activity. Various characterizations, including in situ ATR-SEIRAS and DEMS analysis highlighted the favorable generation of key intermediates *CO and *NH, making CuRu-CBC a promising catalyst for urea synthesis.

Using an alternating electric field is a versatile way to control particle assembly. Programming DNA-AuNP assembly via an electric field remains a significant challenge despite the negative charge of DNA. In DNA-AuNP assembly, a critical percolation state is delicately constructed, where the DNA bond is loosely connected and sensitive to electric fields. In this state, an FCC crystal structure can be successfully constructed by applying a high-frequency electric field to assemble DNA-AuNPs without altering the temperature, which is favorable for temperature-sensitive systems. In addition, the regulation of electric fields can be adjusted through parameters such as the frequency and voltage, which offers more precise control than temperature regulation does. The frequency and voltage can be used to precisely tune the phase structure of DNA-AuNPs from dissolved to disordered or FCC. These findings broaden the potential of DNA-based crystal engineering, revealing new opportunities in electronic nanocomposites and devices.

The synthesis of multicarbon (C 2+ ) products remains a substantial challenge in sustainable CO 2 electroreduction owing to the need for sufficient current density and faradaic efficiency alongside carbon efficiency. Herein, we demonstrate ampere-level high-efficiency CO 2 electroreduction to C 2+ products in both neutral and strongly acidic (pH=1) electrolytes using a hierarchical Cu hollow-fiber penetration electrode (HPE). High concentration of K + could concurrently suppress hydrogen evolution reaction and facilitate C-C coupling, thereby promoting C 2+ production in strong acid. By optimizing the K + and H + concentration and CO 2 flow rate, a faradaic efficiency of 84.5 % and a partial current density as high as 3.1 A cm -2 for C 2+ products, alongside a single-pass carbon efficiency of 81.5 % and stable electrolysis for 240 h were demonstrated in a strong acidic solution of H 2 SO 4 and KCl (pH=1). Experimental measurements and density functional theory simulations suggested that tensile-strained Cu HPE enhances the asymmetric C-C coupling to steer the selectivity and activity of C 2+ products., (© 2024 Wiley-VCH GmbH.)

Anti-wear and anti-oxidation abilities are two key properties of lubricants that play a crucial role in ensuring long-term stable equipment operation. In this study, we aimed to develop a base oil with good anti-oxidation and anti-wear properties for use under extreme pressure. The as-prepared metallocene polyalphaolefin (mPAO) was chemically modified using the trifluoromethanesulfonic acid (TfOH) catalysis through an alkylating reaction with triphenyl phosphorothioate (TPPT). During the experiments, when the reaction temperature exceeded 70 °C or the concentration of TfOH exceeded 2.67%, the β-scission reaction in the alkylation process became significantly more pronounced. The physical and chemical properties of TPPT-modified mPAO (T-mPAO) were evaluated by nuclear magnetic resonance spectroscopy, Fourier trans-form infrared spectroscopy, gel-permeation chromatography, and ASTM standards. T-mPAO showed significantly improved antioxidant capacity, with the initial oxidation temperature increasing by 32 °C compared to the base oil, and it exhibited the slowest increase in acid number in the 96-h oven oxidation test. The tribological tests showed that T-mPAO had the lowest friction coefficient, wear track, and wear rate (72.7% lower than that of mPAO) as well as the highest P B (238 kg) and P D (250 kg) among all tested samples. Compared to mPAO, the average friction coefficient of TPPT-modified mPAO in the four-ball friction test was reduced by 30.5%, and by 16.4% in the TE77 reciprocating friction test. Based on the experimental results, T-mPAO had strong anti-oxidation ability and excellent lubricating performance.The successful synthesis of multifunctional mPAO has enabled lubricant base oil additization, making it possible to use it in more demanding work scenarios, greatly broadening its application scope and making lubricant formulation blending more flexible.

Surface passivation has been developed as an effective strategy to reduce trap-state density and suppress non-radiation recombination process in perovskite solar cells. However, passivation agents usually own poor conductivity and hold negative impact on the charge carrier transport in device. Here, we report a binary and synergistical post-treatment method by blending 4-tert-butyl-benzylammonium iodide with phenylpropylammonium iodide and spin-coating on perovskite surface to form passivation layer. The binary and synergistical post-treated films show enhanced crystallinity and improved molecular packing as well as better energy band alignment, benefiting for the hole extraction and transfer. Moreover, the surface defects are further passivated compared with unary passivation. Based on the strategy, a record-certified quasi-steady power conversion efficiency of 26.0% perovskite solar cells is achieved. The devices could maintain 81% of initial efficiency after 450 h maximum power point tracking., (© 2024. The Author(s).)

Solar-driven H2O2 production via the oxygen reduction reaction (ORR) and water oxidation reaction (WOR) dual channels is green and sustainable, but severely restricted by the sluggish reaction kinetics. Constructing intriguing photocatalysts with effective active centers is a shortcut to breaking the kinetic bottleneck with great significance. Herein, we synthesize two novel neutral phenanthridine-based covalent organic frameworks (PD-COF1 and PD-COF2) for photosynthesizing H2O2. Compared to the no phenanthridine counterpart (AN-COF), the H2O2 photosynthetic activities of PD-COF1 and PD-COF2 are markedly boosted. In air and pure water without sacrificial agents, under Xe lamp and natural sunlight, the H2O2 photogeneration rate of PD-COF2 is 6103 and 3646 μmol g-1 h-1, respectively. Further experimental and theoretical inspections demonstrate that introducing phenanthridine units into COFs smoothly modulates the charge carrier dynamics and thermodynamically favors the generation of crucial OOH* and OH* intermediates in the ORR and WOR paths, respectively. Additionally, this is the first time the neutral phenanthridine moiety serves as the photooxidation unit for 2e- WOR towards H2O2 photoproduction. The current work sheds light on exploring novel catalytic centers for high-performance H2O2 evolution., (© 2024 Wiley‐VCH GmbH.)

Hydrodynamic cavitation and ozone nanobubble-coupled hydrodynamic cavitation have demonstrated effective algae control in laboratories, but their in-situ potential, especially impact on nutrient salt degradation and microbial communities remain unclear. This study applied two-stage nanobubble technology, combining hydrodynamic cavitation and ozone nanobubbles, in a 3300 m 2 semi-enclosed area of Taihu Lake to address these gaps. Results show that the technology efficiently controls algae, reduces odors, improves anaerobic conditions, and lowers ammonia nitrogen. Over 20 days, chlorophyll-a concentration reduced by 77.46% and cyanobacterial phycocyanin by 89.47%. Additionally, the concentrations of 2-MIB, GSM, and DMTS fell below threshold values. Notably, the relative abundance of Cyanobacteria in sediment dropped from 8.53% in the control area to only 1.59% ∼ 3.65% in the experimental area. The technology also achieved a significant reduction in ammonia nitrogen, with removal efficiencies of 78.53% in the water column and 39.17% in sediments, though the removal of total phosphorus was limited. Furthermore, the two-stage nanobubble system enhanced the abundance of nitrogen-cycling microorganisms and genes in the water, while promoting nitrogen- and phosphorus-related microbial communities in sediments and inhibiting the cyanobacteria-associated genus Cyanobium PCC-6307. Thus, Two-stage nanobubble technology can be employed for in-situ algal control in aquatic ecosystems., Competing Interests: Declaration of Competing Interest ☒ The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. ☐ The authors declare the following financial interests/personal relationships which may be considered as potential competing interests:, (Copyright © 2024. Published by Elsevier Inc.)

Helicobacter pylori is the primary cause of gastric adenocarcinoma, which afflicts more than half of the world's population and seriously affects human health. However, achieving efficient treatment of H. pylori infection by effective drug delivery and bioavailability after oral administration remains a challenge due to the harsh microenvironment, short drug retention time, and physiological barriers in the stomach. Moreover, H. pylori has shown resistance to many clinical antibiotics. Antimicrobial peptides (AMPs) exhibit substantial therapeutic efficacy against H. pylori, while they are not likely to induce drug resistance, suggesting their potential utility for the treatment of diseases related to H. pylori . In this paper, we report the design and synthesis of an AMP (GE33) hydrogel with pH-responsive and controlled peptide release properties, in which the minimal inhibitory concentration of the AMP against H. pylori is as low as 1 μg/mL. GE33 self-assembles into a stable peptide hydrogel under neutral pH conditions but decomposes into monomers or oligomers under acidic conditions. Upon oral administration of the hydrogel, the acidic gastric environment would facilitate rapid release of active AMP molecules from the hydrogel and immediate targeting of H. pylori in the stomach wall. Additionally, the remaining peptide is protected in the hydrogel, extending its retention time in the stomach, so that persistent drug release is achieved. The controlled and sustained release manner of the active molecule GE33, which enhances drug bioavailability, along with its excellent bactericidal efficacy opens a great potential for treating H. pylori infection.

Ni-based electrocatalysts have been predicted as highly potential candidates for hydrogen evolution reaction (HER); however, their applicability is hindered by an unfavorable d-band energy level ( E d ). Moreover, precise d-band structural engineering of Ni-based materials is deterred by appropriative synthesis methods and experimental characterization. Herein, we meticulously synthesize a special single-iodine-atom structure (I-Ni@C) and characterize the E d manipulation via resonant inelastic X-ray scattering (RIXS) spectroscopy to fill this gap. The complex catalytic mechanism has been elucidated via synchrotron radiation-based multitechniques (SRMS) including X-ray absorption fine structure (XAFS), in situ synchrotron radiation-based Fourier transform infrared (SR-FTIR) spectroscopy, and near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS). In particular, RIXS is innovatively applied to reveal the precise regulation of Ni E d of I-Ni@C. Consequently, the role of such single-iodine-atom strategy is confirmed to not only facilitate the moderate E d of the Ni site for balancing the adsorption/desorption capacities of key intermediates but also act as a bridge to enhance the electronic interaction between Ni and the carbon shell for forming a localized polarized electric field conducive to H 2 O dissociation. As a result, I-Ni@C exhibits an enhanced alkaline hydrogen evolution performance with an overpotential of 78 mV at 10 mA/cm 2 and superior stability, surpassing the majority of the reported Ni-based catalysts. Overall, this study has managed to successfully tailor the d-band center of materials from the SRMS perspective, which has crucial implications for nanotechnology, chemistry, catalysis, and other fields.

Organic-inorganic hybrid resists offer a solution to the issue of low sensitivity in organic photoresists like poly(methyl methacrylate) (PMMA). In this study, an organic-inorganic hybrid resist (PMMA-Al 2 O 3 ) with high sensitivity and resolution was prepared by depositing metal oxides into PMMA using sequential infiltration synthesis (SIS). PMMA-Al 2 O 3 was prepared by precisely controlling the number of SIS cycles (<23) in various atomic layer deposition (ALD) processes to facilitate the growth of metal oxides within PMMA pores. The impact of different metal oxide contents and distributions on the sensitivity and resolution of electron beam exposure was investigated. Numerical simulations of the deposit formation within the PMMA pores were performed by solving the pore-scale ALD governing equations fed by the reactor-scale boundary conditions. The gradual pore constriction with SIS cycles was predicted and validated by the experimental charaterizations. The results demonstrated that PMMA-Al 2 O 3 was prepared using 20 SIS cycles, which corresponds to the numerically predicted occurrence of the pore blockage at the upper region of the PMMA layer, exhibiting optimal electron beam (e-beam) resolution while enabling line exposure with a width of 50 nm. While the corresponding sensitivity was lower than those of the samples prepared using 5 and 10 SIS cycles, the degradation of the PMMA structure was affected under exposure. The pattern transfer results showed that the line width was well retained for 20 cycles of deposition because of the high etching resistance of Al 2 O 3 . This research is expected to provide an effective approach to developing next-generation high-performance photoresists.

Metal-organic frameworks (MOFs) have been widely studied due to their versatile applications and easily tunable structures. However, heteroatom-metal coordination dominates the MOFs community, and the rational synthesis of carbon-metal coordination-based MOFs remains a significant challenge. Herein, two-dimensional (2D) MOFs based on silver-carbon linkages are synthesized through the coordination between silver(I) salt and isocyanide-based monomers at ambient condition. The as-synthesized 2D MOFs possess well-defined crystalline structures and a staggered AB stacking mode. Most interestingly, these 2D MOFs, without π-π stacking between layers, exhibit narrow bandgaps down to 1.42 eV. As electrochemical catalysts for converting CO2 to CO, such 2D MOFs demonstrate Faradaic efficiency over 92%. Surprisingly, the CO2 reduction catalyzed by these MOFs indicates favorable adsorption of CO2 and *COOH on the active carbon sites of the isocyanide groups rather than on silver sites. This is attributed to the critical σ donor role of isocyanides and the corresponding ligand-to-metal charge-transfer effect. This work not only paves the way toward a new family of MOFs based on metal-isocyanide coordination but also offers a rare platform for understanding the electrocatalysis processes on strongly polarized carbon species., (© 2024 Wiley‐VCH GmbH.)

Modulating the electronic structure of catalysts to effectively couple the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is essential for developing high-efficiency anion exchange membrane water electrolyzer (AEMWE). Herein, a coral-like nanoarray composed of nanosheets through the synergistic layering effect of cobalt and the 1D guiding of vanadium is synthesized, which promotes extensive contact between the active sites and electrolyte. The HER and OER activities can be enhanced by modulating the electronic structure through nitridation and phosphorization, respectively, enhancing the strength of metal-H bond to optimize hydrogen adsorption and facilitating the proton transfer to improve the transformation of oxygen-containing intermediates. Resultantly, the AEMWE achieves a current density of 500 mA cm -2 at 1.76 V for 1000 h in 1.0 M KOH at 70 °C. The energy consumption is 4.21 kWh Nm -3 with the producing hydrogen cost of $0.93 per kg H 2 . Operando synchrotron radiation and Bode phase angle analyses reveal that during the high-energy consumed OER, the dissolution of vanadium species transforms distorted Co-O octahedral into regular octahedral structures, accompanied by a shortening of the Co-Co bond length. This structural evolution facilitates the formation of oxygen intermediates, thus accelerating the reaction kinetics., (© 2024 Wiley‐VCH GmbH.)

Developing advanced functional carbon materials is essential for electrocatalysis, caused by their vast merits for boosting many key energy conversion reactions. Herein, the covalent organic frameworks (COFs) is utilized on metal-organic frameworks (MOFs) as the template, under the controllable metal atoms thermal migration process successfully in situ constructs Pd-Co alloy nanoparticles on hollow cubic graphene. The electrocatalytic oxygen reduction reaction (ORR) evaluation showed excellent performances with a half-wave potential of 0.866 V, and a limited current density of 4.975 mA cm -2 , that superior to the commercial Pt/C and Co nanoparticles. The contrast experiments and X-ray absorption spectrum demonstrated the aggregated electrons at highly dispersed Pd atoms on Co nanoparticle that promoted the main activities. This work not only enlightens the novel carbon materials designing strategies but also suggests heterogeneous electrocatalysis., (© 2024 Wiley‐VCH GmbH.)

Formic acid (FA) dehydrogenation and CO 2 hydrogenation to FA/formate represent promising methodologies for the efficient and clean storage and release of hydrogen, forming a CO 2 -neutral energy cycle. Here, we report the synthesis of highly dispersed and stable bimetallic Pd-based nanoparticles, immobilized on self-pillared silicalite-1 (SP-S-1) zeolite nanosheets using an incipient wetness co-impregnation technique. Owing to the highly accessible active sites, effective mass transfer, exceptional hydrophilicity, and the synergistic effect of the bimetallic species, the optimized PdCe 0.2 /SP-S-1 catalyst demonstrated unparalleled catalytic performance in both FA dehydrogenation and CO 2 hydrogenation to formate. Remarkably, it achieved a hydrogen generation rate of 5974 mol H2  mol Pd -1  h -1 and a formate production rate of 536 mol formate  mol Pd at 50 °C, surpassing most previously reported heterogeneous catalysts under similar conditions. Density functional theory calculations reveal that the interfacial effect between Pd and cerium oxide clusters substantially reduces the activation barriers for both reactions, thereby increasing the catalytic performance. Our research not only showcases a compelling application of zeolite nanosheet-supported bimetallic nanocatalysts in CO -1  h -1 at 50 °C, surpassing most previously reported heterogeneous catalysts under similar conditions. Density functional theory calculations reveal that the interfacial effect between Pd and cerium oxide clusters substantially reduces the activation barriers for both reactions, thereby increasing the catalytic performance. Our research not only showcases a compelling application of zeolite nanosheet-supported bimetallic nanocatalysts in CO 2 -mediated hydrogen storage and release but also contributes valuable insights towards the development of safe, efficient, and sustainable hydrogen technologies., (© 2024 Wiley-VCH GmbH.)

Water transportation to developing tissues relies on the structure and function of plant xylem cells. Plant microtubules govern the direction of cellulose microfibrils and guide secondary cell wall formation and morphogenesis. However, the relevance of microtubule-determined xylem wall thickening patterns in plant hydraulic conductivity remains unclear. In the present study, we identified a maize (Zea mays) semi-dominant mutant, designated drought-overly-sensitive1 (ZmDos1), the upper leaves of which wilted even when exposed to well-watered conditions during growth; the wilting phenotype was aggravated by increased temperatures and decreased humidity. Protoxylem vessels in the stem and leaves of the mutant showed altered thickening patterns of the secondary cell wall (from annular to spiral), decreased inner diameters, and limited water transport efficiency. The causal mutation for this phenotype was found to be a G-to-A mutation in the maize gene α-tubulin4, resulting in a single amino acid substitution at position 196 (E196K). Ectopic expression of the mutant α-tubulin4 in Arabidopsis (Arabidopsis thaliana) changed the orientation of microtubule arrays, suggesting a determinant role of this gene in microtubule assembly and secondary cell wall thickening. Our findings suggest that the spiral wall thickenings triggered by the α-tubulin mutation are stretched during organ elongation, causing a smaller inner diameter of the protoxylem vessels and affecting water transport in maize. This study underscores the importance of tubulin-mediated protoxylem wall thickening in regulating plant hydraulics, improves our understanding of the relationships between protoxylem structural features and functions, and offers candidate genes for the genetic enhancement of maize., Competing Interests: Conflict of interest statement. None declared., (© The Author(s) 2024. Published by Oxford University Press on behalf of American Society of Plant Biologists. All rights reserved. For commercial re-use, please contact reprints@oup.com for reprints and translation rights for reprints. All other permissions can be obtained through our RightsLink service via the Permissions link on the article page on our site—for further information please contact journals.permissions@oup.com.)

Smc5/6 is a member of the eukaryotic structural maintenance of chromosomes (SMC) family of complexes with important roles in genome maintenance and viral restriction. However, limited structural understanding of Smc5/6 hinders the elucidation of its diverse functions. Here, we report cryo-EM structures of the budding yeast Smc5/6 complex in eight-subunit, six-subunit and five-subunit states. Structural maps throughout the entire length of these complexes reveal modularity and key elements in complex assembly. We show that the non-SMC element (Nse)2 subunit supports the overall shape of the complex and uses a wedge motif to aid the stability and function of the complex. The Nse6 subunit features a flexible hook region for attachment to the Smc5 and Smc6 arm regions, contributing to the DNA repair roles of the complex. Our results also suggest a structural basis for the opposite effects of the Nse1-3-4 and Nse5-6 subcomplexes in regulating Smc5/6 ATPase activity. Collectively, our integrated structural and functional data provide a framework for understanding Smc5/6 assembly and function., (© 2024. The Author(s), under exclusive licence to Springer Nature America, Inc.)

Osteoarthritis (OA) is a degenerative bone and joint disease characterized by decreased cartilage lubrication, leading to continuous wear and ultimately irreversible damage. This situation is particularly challenging for early-stage OA, as current bio-lubricants lack precise targeting for small inflammatory lesions. In this work, an antibody-mediated targeting hydrogel microspheres (HMS) is developed to precisely lubricate the local injury site of cartilage and prevent the progression of early OA. Anti-Collagen type I (Anti-Col1) is an antibody that targets cartilage injury sites in early OA stages. It is anchored on a HMS matrix made of Gelatin methacrylate (GelMA) and poly (sulfobetaine methacrylate) (PSBMA) to create targeted HMS (T-G/S HMS). The T-G/S HMS's high hydrophilicity, along with the dynamic interaction between its surficial Anti-Col1 and the Col1 on cartilage injury site, ensures its precise and effective lubrication of early OA lesions. Consequently, injecting T-G/S HMS into rats with early OA significantly slows disease progression and reduces symptoms. In conclusion, the developed injectable targeted lubricating HMS and the precisely targeted lubrication strategy represent a promising, convenient technique for treating OA, particularly for slowing the early-stage OA progression., (© 2024 Wiley‐VCH GmbH.)

The fouling phenomenon of membranes has hindered the rapid development of separation technology in wastewater treatment. The integration of materials into membranes with both excellent separation performance and self-cleaning properties still pose challenges. Here, a self-assembled composite membrane with solar-driven self-cleaning performance is reported for the treatment of complex oil-water emulsions. The mechanical robustness of the composite membrane is enhanced by the electrostatic attraction between chitosan and metal-organic frameworks (MOF) CuCo-HHTP as well as the crosslinking effect of glutaraldehyde. Molecular dynamics (MD) simulations also revealed the hydrogen bonding interaction between chitosan and CuCo-HHTP. The composite membrane of CuCo-HHTP-5@CS/MPVDF exhibits a high flux ranging from 700.6 to 2350.6 L∙m -2 ∙h -1 ∙bar -1 and excellent separation efficiency (>99.0%) for various oil-water emulsions, including crude oil, kerosene, and other light oils. The addition of CuCo-HHTP shows remarkable photothermal effects, thus demonstrating excellent solar-driven self-cleaning capability and antibacterial performance (with an efficiency of ≈100%). Furthermore, CuCo-HHTP-5@CS/MPVDF can activate peroxomonosulfate (PMS) under sunlight, quickly removing oil-fouling and dyes. Density functional theory (DFT) calculations indicate that the bimetallic sites of Cu and Co in CuCo-HHTP effectively promoted the activation of PMS. This study provides distinctive insights into the multifaceted applications of MOFs-derived photothermal anti-fouling composite membranes., (© 2024 Wiley‐VCH GmbH.)

Purpose: Acute erythroleukemia (AEL) is a rare and highly aggressive subtype of acute myeloid leukemia (AML) with an extremely poor prognosis when treated with available drugs. Therefore, new investigational agents capable of inducing remission are urgently required., Methods: Bioinformatics analysis, western blot and qRT-PCR were used to reveal the potential biological mechanism of bryostatin 4 (B4), an antineoplastic macrolide derived from the marine bryozoan Bugula neritina. Then, in vivo experiments were conducted to evaluate the role of transforming growth factor (TGF)-β signaling in the progression of AEL., Results: Our results revealed that the proliferation of K562 cells and TF-1 cells was significantly inhibited by B4 at IC 50 values of 37 nM and 52 nM, respectively. B4 inhibited TGF-β signaling and its downstream pathway targets, particularly the phosphorylation of Smad2, Smad3, Ras, C-RAF, ERK1/2, and MEK. B4 also played an important role in cell invasion and migration in K562 cells and TF-1 cells by reducing the protein levels of the mesenchymal cell marker vimentin. Moreover, Flow cytometry and western blot analyses demonstrated that B4 induced apoptosis and initiated G0/G1 phase arrest by modulating mitochondrial dysfunction and cyclin-dependent kinase (CDK) expression., Conclusion: These findings indicated that B4 could inhibit the proliferation, migration, invasion, and TGF-β signaling pathways of AEL cells, thus suggesting that B4 possesses therapeutic potential as a treatment for AEL., (© 2024. Springer Nature Switzerland AG.)

Halorhodospira (Hlr.) halochloris is a triply extremophilic phototrophic purple sulfur bacterium, as it is thermophilic, alkaliphilic, and extremely halophilic. The light-harvesting-reaction center (LH1-RC) core complex of this bacterium displays an LH1-Q y transition at 1,016 nm, which is the lowest-energy wavelength absorption among all known phototrophs. Here we report the cryo-EM structure of the LH1-RC at 2.42 Å resolution. The LH1 complex forms a tricyclic ring structure composed of 16 αβγ-polypeptides and one αβ-heterodimer around the RC. From the cryo-EM density map, two previously unrecognized integral membrane proteins, referred to as protein G and protein Q, were identified. Both of these proteins are single transmembrane-spanning helices located between the LH1 ring and the RC L-subunit and are absent from the LH1-RC complexes of all other purple bacteria of which the structures have been determined so far. Besides bacteriochlorophyll b molecules (B1020) located on the periplasmic side of the Hlr. halochloris membrane, there are also two arrays of bacteriochlorophyll b molecules (B800 and B820) located on the cytoplasmic side. Only a single copy of a carotenoid (lycopene) was resolved in the Hlr. halochloris LH1-α3β3 and this was positioned within the complex. The potential quinone channel should be the space between the LH1-α3β3 that accommodates the single lycopene but does not contain a γ-polypeptide, B800 and B820. Our results provide a structural explanation for the unusual Q y red shift and carotenoid absorption in the Hlr. halochloris spectrum and reveal new insights into photosynthetic mechanisms employed by a species that thrives under the harshest conditions of any phototrophic microorganism known., (© 2024 The Authors. Journal of Integrative Plant Biology published by John Wiley & Sons Australia, Ltd on behalf of Institute of Botany, Chinese Academy of Sciences.)

Since the discovery in 2000, conversion-type materials have emerged as a promising negative-electrode candidate for next-generation batteries with high capacity and tunable voltage, limited by low reversibility and severe voltage hysteresis. Heterogeneous construction stands out as a cost-effective and efficient approach to reducing reaction barriers and enhancing energy density. However, the second term introduced by conventional heterostructure inevitably complicates the electrochemical analysis and poses great challenges to harvesting systematic insights and theoretical guidance. A model cell is designed and established herein for the conversion reactions between Na and TM SA -SnO 2 , where TM SA -SnO 2 represents single atom modification of eight different 3d transition elements (V, Cr, Mn, Fe, Co, Ni, Cu or Zn). Such a model unit fundamentally eliminates the interference from the second phase and thus enables independent exploration of activation manifestations of the heterogeneous architecture. For the first time, a thermodynamically dependent catalytic effect is proposed and verified through statistical data analysis. The mechanism behind the unveiled catalytic effect is further elucidated by which the active d orbitals of transition metals weaken the surface covalent bonds and lower the reaction barriers. This research provides both theoretical insights and practical demonstrations of the advanced heterogeneous electrodes., (© 2024 Wiley-VCH GmbH.)

Unconventional 1T'-phase transition metal dichalcogenides (TMDs) have aroused tremendous research interest due to their unique phase-dependent physicochemical properties and applications. However, due to the metastable nature of 1T'-TMDs, the controlled synthesis of 1T'-TMD monolayers (MLs) with high phase purity and stability still remains a challenge. Here we report that 4H-Au nanowires (NWs), when used as templates, can induce the quasi-epitaxial growth of high-phase-purity and stable 1T'-TMD MLs, including WS 2 , WSe 2 , MoS 2 and MoSe 2 , via a facile and rapid wet-chemical method. The as-synthesized 4H-Au@1T'-TMD core-shell NWs can be used for ultrasensitive surface-enhanced Raman scattering (SERS) detection. For instance, the 4H-Au@1T'-WS 2 NWs have achieved attomole-level SERS detections of Rhodamine 6G and a variety of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) spike proteins. This work provides insights into the preparation of high-phase-purity and stable 1T'-TMD MLs on metal substrates or templates, showing great potential in various promising applications., (© 2024. The Author(s), under exclusive licence to Springer Nature Limited.)

The electrocatalytic valorization of polyethylene terephthalate-derived ethylene glycol to valuable glycolic acid offers considerable economic and environmental benefits. However, conventional methods face scalability issues due to rapid activity decay of noble metal electrocatalysts. We demonstrate that a dynamic potential cycling approach, which alternates the electrode potential between oxidizing and reducing values, significantly mitigates surface deactivation of noble metals during electrochemical oxidation of ethylene glycol. This method enhances catalyst activity by 20 times compared to a constant-potential approach, maintaining this performance for up to 60 h with minimal deactivation. In situ Raman and X-ray absorption spectroscopy show that this effectiveness results from efficient removal of surface oxide during the reaction. The strategy is applicable to polyethylene terephthalate hydrolysates and various noble metals, such as palladium, gold, and platinum, with palladium showing a high conversion rate in recent studies. Our approach offers an efficient and durable method for electrochemical upcycling of biomass-derived compounds., (© 2024. The Author(s).)

As the global energy structure evolves and clean energy technologies advance, electrocatalysis has become a focal point as a critical conversion pathway in the new energy sector. Transitional metal electrocatalysts (TMEs) with their distinctive electronic structures and redox properties show great potential in electrocatalytic reactions. However, complex reaction mechanisms and kinetic limitations hinder the improvement of energy conversion efficiency, highlighting the necessity for comprehensive studies on structure and performance of electrocatalysts. X-ray Absorption Fine Structure (XAFS) spectra stand out as a robust tool for examining the electrocatalyst's structures and performance due to its atomic selectivity and sensitivity to local environments. This review delves into the application of XAFS technology in characterizing TMEs, providing in-depth analyses of X-ray Absorption Near-Edge Structure (XANES) spectra, and Extended XAFS (EXAFS) spectra in both R-space and k-space. These analyses reveal intrinsic structural information, electronic interactions, catalyst stability, and aggregation morphology. Furthermore, the paper examines advancements in in-situ XAFS techniques for real-time monitoring of active site changes, capturing critical intermediate and transitional states, and elucidating the evolution of active species during electrocatalytic reactions. These insights deepen our understanding on structure-activity relationship of electrocatalysts and offer valuable guidance for designing and developing highly active and stable electrocatalysts., (© 2024 Wiley‐VCH GmbH.)

The microstructure plays a crucial role in the manufacturing and application of polyacrylonitrile fibers, which serve as precursors for carbon fibers. Synchrotron radiation small angle x-ray scattering (SR-SAXS) is a non-destructive and precise technique for analyzing fiber structures. This study employed one-dimensional SR-SAXS mapping to extract key structural parameters such as periodicity, lamellae thickness, and the extent of amorphous regions, as well as the directional orientation in γ-irradiated, pre-oxidized polyacrylonitrile fibers. The analysis revealed a three-layered structure comprising a surface skin, a transitional layer, and a central core. Notably, the lamellar thickness exhibits a "U"-shaped distribution, while the long-period structures, amorphous regions, and orientational properties demonstrate a "wave-like" pattern. Within this structure, the skin exhibits a higher level of orientation, with the orientation decreasing progressively from the skin toward the core layer. The structure of the layered crystal was further corroborated by the morphological analysis. In addition, molecular simulations were performed to propose the mechanisms underlying the formation of this layered structure. This comprehensive investigation using SR-SAXS and one-dimensional mapping provides detailed insights into the microstructural and morphological characteristics of polyacrylonitrile fibers, which can inform future advancements in material processing and refinement techniques for the production of advanced fibers., (© 2024 Author(s). Published under an exclusive license by AIP Publishing.)