bluuebunny/crossref_metadata_2025_split huggingface dataset:
3d‐Orbital High‐Spin Configuration Driven From Electronic Modulation of Fe3O4/FeP Heterostructures Empowering Efficient Electrocatalyst for Lithium−Sulfur Batteries
Authors: Wang Zhengyi , Huang Wenzhi , Wu Hao , Wu Yujie , Shi Kaixiang , Li Junhao , Zhang Weigang , Liu Quanbing 
Published: August 2024

AbstractThe intricate lithium polysulfides (LiPSs) shuttle and uncontrollable lithium dendrite growth critically hinder the commercialization of lithium−sulfur (Li−S) batteries. The rational and orderly assignment of multi‐electron induced flow is the critical link in sulfer redox reaction. Herein, the yolk‐shell Fe3O4/FeP@C heterostructure nanoreactors are fabricated to modulate electronic structure, including spin‐related charge behavior and orbital orientation control, which can demonstrate the interaction between catalytic activity and spin‐state conformation. The orbital spin splitting of Fe3O4/FeP@C induces the electron transition from low‐spin to high‐spin, where the non‐degenerate orbitals contribute to energy level up‐shift, guiding electron migration from FeP to Fe3O4, and activating more electronic states in 3d orbitals. Spin polarization guides electron flow and induces sulfur closed‐loop conversion, which are confirmed by DFT simulations and in situ Raman. Hence, the electrochemical performances are remarkable at ultra‐high current density and sulfur loading. Even an initial specific capacity of 928.5 mAh g−1 of a Li−S pouch cell reveals the practical prospect of Fe3O4/FeP@C/PP separator. The Li//Li symmetric cell cycles steadily for 4000 h, confirming the interlayer simultaneously promotes sulfur evolution kinetics and sieves lithium ions. This work deciphers the principles of spin‐orbit coupling, achieving the topological modulation of “charge−spin−orbit” toward electrocatalysts.
Toward Predicting the Formation of Integral‐Asymmetric, Isoporous Diblock Copolymer Membranes
Authors: Blagojevic Niklas , Das Shibananda , Xie Jiayu , Dreyer Oliver , Radjabian Maryam , Held Martin , Abetz Volker , Müller Marcus 
Published: August 2024

AbstractThe self‐assembly and nonsolvent‐induced phase separation (SNIPS) process of block copolymers and solvents enables the fabrication of integral‐asymmetric, isoporous membranes. An isoporous top layer is formed by evaporation‐induced self‐assembly (EISA) and imparts selectivity for ultrafiltration of functional macromolecules or water purification. This selective layer is supported by a macroporous bottom structure that is formed by nonsolvent‐induced phase separation (NIPS) providing mechanical stability. Thereby the permeability/selectivity tradeoff is optimized. The SNIPS fabrication involves various physical phenomena—e.g., evaporation, self‐assembly, macrophase separation, vitrification – and multiple structural, thermodynamic, kinetic, and process parameters. Optimizing membrane properties and rationally designing fabrication processes is a challenge which particle simulation can significantly contribute to. Using large‐scale particle simulations, it is observed that 1) a small incompatibility between matrix‐forming block of the copolymer and nonsolvent, 2) a glassy arrest that occurs at a smaller polymer concentration, or 3) a higher dynamical contrast between polymer and solvent results in a finer, spongy substructure, whereas the opposite parameter choice gives rise to larger macropores with an elongated shape. These observations are confirmed by comparison to experiments on polystyrene (PS)‐block‐poly(4‐vinylpyridine) (P4VP) diblock copolymer membranes, varying the chemical nature of the coagulant or the temperature of coagulation bath.
Quantum Mechanical Derived (VdW‐DFT) Transferable Lennard–Jones and Morse Potentials to Model Cysteine and Alkanethiol Adsorption on Au(111)
Authors: Ventura‐Macias Emiliano , Martinez P. M. , Pérez Rubén , Vilhena J. G. 
Published: August 2024

AbstractThe cysteine and alkanethiol adsorption on Au(111) surfaces is investigated using density functional theory (DFT) and classic molecular dynamics (MD). Understanding the S–Au interaction across different scales poses major challenges. DFT provides atomic‐level precision but it hardly provides insight on nanosecond scale dynamics of this interface. Alternatively, MD, although it enables modeling larger systems for longer periods, its accuracy heavily relies on the parameterization of the force fields (FF). To address this, an MD potential is fitted using DFT calculations, bridging the gap in accuracy and efficiency. At the DFT level, it is found that PBE with DFT‐D3 reproduces complex approaches at a fraction of the computational cost. Separating PBE and DFT‐D3 contributions reveals consistent PBE energy across molecules (chemisorption), while dispersion varies (physisorption). Thus, the interaction energy of cysteine and two short‐chain alkanethiols is calculated to parameterize both Morse and Lennard–Jones (LJ) potentials. The parameterization improves the potential energy in the preferred adsorption sites: the threefold hcp and fcc with respect to the previous proposals in the literature. Furthermore, the transferability is here demonstrated. At last, these results show that LJ potentials outperform more complex Morse potentials. The procedure is general, and the codes and supporting inputs are publicly available, allowing swift generation of potential energy surfaces (PES) at the DFT level, and fitted LJ or Morse potentials to any molecular interface.
Circularly Polarized Luminescent Liquid Crystal Copolymers Constructed by Triplet–Singlet Förster‐Resonance Energy Transfer: Achieving Large Glum Values, Long Lifetime, and High Photoluminescence Quantum Yield
Authors: Zhou Mengdie , Lu Peng , Xu Zhipeng , Wang Yuyi , Yuan Yongjie , Gong Yongyang , Zhang Hailiang 
Published: August 2024

AbstractCircularly polarized luminesce (CPL) materials are crucial for various applications, including display devices and bionics. However, existing CPL materials face difficulties in simultaneously meeting large luminescence asymmetry factors (glum), high photoluminescence quantum yields (PQY), and long lifetime. Here, a simple strategy to prepare a series of high‐performance CPL liquid crystal copolymers is constructed by triplet–singlet Förster‐resonance energy transfer (TS‐FRET). A series of chiral liquid crystal copolymers are successfully synthesized by copolymerizing phosphorescent donor bearing chiral cholesterol mesogen with fluorescence acceptor bearing naphthalimide chromophore. The introduction of the naphthalimide component promotes the formation of twist grain boundary smectic‐A phase (TGBA*) and behaves distinctive selective reflective effect. An effective TS‐FRET process occurs in the two components of copolymers, and dual emission characteristics of thermally activated delayed fluorescence and room‐temperature phosphorescence are observed in the copolymer films. When the naphthalimide content of copolymer is 10%, the luminescence lifetime can achieve 83.0 ms. As the naphthalimide content increases, the glum initially increases and subsequently decreases, reaching a maximum of −1.15. In addition, the copolymer films possess enhanced photoluminescence quantum yield by TS‐FRET with a maximum value of 68%. The application of copolymers in information security is also explored.
Er:LiNbO3 Quantum Memory Platform Optimized with Dynamic Defect Annealing
Authors: Slusar Tetiana , Azarov Alexander , Galeckas Augustinas , Hallén Anders , Ju Jung Jin , Moon Kiwon , Kuznetsov Andrej 
Published: August 2024

AbstractLithium niobate (LiNbO3) exhibits poor radiation resistance when conventionally implanted with Er at room temperature. To repair the structural disorder, high‐temperature post‐implantation anneals are typically required; however, such treatments can cause sample cracking and dopant redistribution, which are incompatible with device applications. The optimized approach is proposed by performing implants at elevated but acceptably low temperatures to in situ minimize the structural defects generated in the collision cascades, via so‐called “dynamic defect annealing”. Thus, a gradual increase in Er optical activity is shown as a function of irradiation temperature in the range of 25–450 °C, in striking correlation with a decreasing trend for the residual disorder. The impact of moderate post‐implantation anneals is also investigated by comparing the results of anneals of samples implanted at 25 °C and 450 °C. This comparison further confirms the higher optical activation of Er and lower residual structural disorder when the material is initially implanted at elevated temperatures. Based on these data, it is concluded that the use of dynamic defect annealing during the Er implantation of LiNbO3 is a promising strategy for optimizing it as a quantum memory platform, resolving otherwise inevitable trade‐offs.
Large‐Scale Fabrication of Room‐Temperature Phosphorescence Cellulose Filaments with Color‐Tunable Afterglows
Authors: Peng Fang , Qiu Changjing , Wu Pingping , Hu Songnan , Chen Pan , Li Xingxing , Li Mengke , Chen Zijian , Su Shi‐Jian , Qi Haisong 
Published: August 2024

AbstractThe large‐scale fabrication of long‐lived and sustainable room‐temperature phosphorescence (RTP) materials with color‐tunable afterglow is of considerable practical importance in diverse optoelectronic applications but remains challenging. Herein, based on a process for the mass production of cellulose acetoacetate filaments, large‐scale RTP filaments are synthesized by introducing amino‐bearing luminophores via a mild enamine reaction. Attributed to efficient intersystem crossing facilitated by acetoacetyl and benzoyloxy groups alongside a rigid environment provided by multiple hydrogen bonding, the resulting filaments exhibit impressive RTP with a lifetime of 772 ms and a phosphorescence quantum yield of 45.06%. Furthermore, the afterglow color of RTP filaments is rationally modulated from blue to greenish‐yellow to rosy‐red through triplet‐to‐singlet Förster resonance energy transfer. Meanwhile, the formation of diverse clusters with comparable but different lifetimes leads to interesting excitation‐dependent afterglows. This work not only provides an effective strategy to construct long‐lived, color‐tunable, sustainable afterglows but also establishes large‐scale and continuous preparation routes for functional cellulose filaments.
Loss of Smek1 Induces Tauopathy and Triggers Neurodegeneration by Regulating Microtubule Stability
Authors: Duan Ruo‐Nan , Liu Ai , Sun Yue‐Qing , Xie Yun‐Fang , Wei Shi‐Jun , Gao Shang , Liu Yi‐Ming , Li Xi , Sun Wen‐Jie , Li Jiang‐Xia , Yan Chuan‐Zhu , Liu Qi‐Ji 
Published: August 2024

AbstractSuppressor of Mek1 (Smek1) is a regulatory subunit of protein phosphatase 4. Genome‐wide association studies have shown the protective effect of SMEK1 in Alzheimer's disease (AD). However, the physiological and pathological roles of Smek1 in AD and other tauopathies are largely unclear. Here, the role of Smek1 in preventing neurodegeneration is investigated in tauopathy. Smek1 is downregulated in the aged human brain. Through single‐cell sequencing, a novel neuronal cluster is identified that possesses neurodegenerative characteristics in Smek1−/− mice. Smek1 deficiency caused markedly more severe motor and cognitive impairments in mice, as well as neuronal loss, gliosis, and tau hyperphosphorylation at major glycogen synthase kinase 3β (Gsk3β) sites. Protein‐protein interaction analysis revealed that the Ran‐binding domain (RanBD) in the N‐terminus of Smek1 facilitated binding with kinesin family member 2A (Kif2a). Depletion of Smek1 resulted in cytoplasmic aggregation of Kif2a, axon outgrowth defects, and impaired mitochondrial axonal trafficking. Downregulation of Kif2a markedly attenuated tau hyperphosphorylation and axon outgrowth defects in shSmek1 cells. For the first time, this study demonstrates that Smek1 deficiency progressively induces neurodegeneration by exacerbating tau pathology and mitochondrial dysfunction in an age‐dependent manner.
Blocking ACSL6 Compromises Autophagy via FLI1‐Mediated Downregulation of COLs to Radiosensitize Lung Cancer
Authors: Ding Wen , Bao Shijun , Zhao Qingwei , Hao Wei , Fang Kai , Xiao Yanlan , Lin Xiaoting , Zhao Zhemeng , Xu Xinyi , Cui Xinyue , Yang Xiwen , Yao Liuhuan , Jin Hai , Zhang Kun , Guo Jiaming 
Published: August 2024

AbstractLung cancer (LC) is the leading cause of cancer‐related mortality worldwide. Radiotherapy is the main component of LC treatment; however, its efficacy is often limited by radioresistance development, resulting in unsatisfactory clinical outcomes. Here, we found that LC radiosensitivity is up‐regulated by decreased expression of long‐chain acyl‐CoA synthase 6 (ACSL6) after irradiation. Deletion of ACSL6 results in significant elevation of Friend leukemia integration 1 transcription factor (FLI1) and a marked decline of collagens (COLs). Blocking of ACSL6 impairs the tumor growth and upregulates FLI1, which reduces the levels of COLs and compromises irradiation‐induced autophagy, leading to considerable therapeutic benefits during radiotherapy. Moreover, the direct interaction between ACSL6 and FLI1 and engagement between FLI1 and COLs indicates the involvement of the ACSL6‐FLI1‐COL axis. Finally, the potently adjusted autophagy flux reduces its otherwise contributive capability in surviving irradiation stress and leads to satisfactory radiosensitization for LC radiotherapy. These results demonstrate that enhanced ACSL6 expression promotes the aggressive performance of irradiated LC through increased FLI1‐COL‐mediated autophagy flux. Thus, the ACSL6‐FLI1‐Col‐autophagy axis may be targeted to enhance the radiosensitivity of LC and improve the management of LC in radiotherapy.
Genomic Amplification of TBC1D31 Promotes Hepatocellular Carcinoma Through Reducing the Rab22A‐Mediated Endolysosomal Trafficking and Degradation of EGFR
Authors: Cao Pengbo , Chen Hongxia , Zhang Ying , Zhang Qi , Shi Mengting , Han Huihui , Wang Xiaowen , Jin Liang , Guo Bingqian , Hao Rongjiao , Zhao Xi , Li Yuanfeng , Gao Chengming , Liu Xinyi , Wang Yahui , Yang Aiqing , Yang Chenning , Si Anfeng , Li Hua , Song Qingfeng , He Fuchu , Zhou Gangqiao 
Published: August 2024

AbstractHepatocellular carcinomas (HCCs) are characterized by a vast spectrum of somatic copy number alterations (CNAs); however, their functional relevance is largely unknown. By performing a genome‐wide survey on prognosis‐associated focal CNAs in 814 HCC patients by an integrative computational framework based on transcriptomic data, genomic amplification is identified at 8q24.13 as a promising candidate. Further evidence is provided that the 8q24.13 amplification‐driven overexpression of Rab GTPase activating protein TBC1D31 exacerbates HCC growth and metastasis both in vitro and in vivo through activating Epidermal growth factor receptor (EGFR) signaling. Mechanistically, TBC1D31 acts as a Rab GTPase activating protein to catalyze GTP hydrolysis for Rab22A and then reduces the Rab22A‐mediated endolysosomal trafficking and degradation of EGFR. Notably, overexpression of TBC1D31 markedly increases the resistance of HCC cells to lenvatinib, whereas inhibition of the TBC1D31‐EGFR axis can reverse this resistance phenotype. This study highlights that TBC1D31 at 8q24.13 is a new critical oncogene, uncovers a novel mechanism of EGFR activation in HCC, and proposes the potential strategies for treating HCC patients with TBC1D31 amplification or overexpression.
Simultaneous Salt Rejection and Heat Localization Via Engineering Macrochannels in Morning Glory‐Shaped 3D Evaporator
Authors: Mao Zhengyi , Han Yicheng , Shen Junda , Zhang Lei , Xie Youneng , Liu Jiahua , Wu Haikun , Yu Zhen , Duan Xiaoguang , Zhang Yaoxin , Lu Jian 
Published: August 2024

AbstractSolar desalination is a promising solution for alleviating water scarcity due to its low‐cost, environmentally friendly, and off‐grid capabilities. However, simultaneous salt rejection and heat localization remain challenging, as the rapid salt convection often results in considerable heat loss. Herein, this challenge is overcome via a facile design: i) isolating high‐temperature and high‐salt zones by rationally designing morning glory‐shaped wick structures and ii) bridging high‐salt zones and bulk water with low‐tortuosity macrochannels across low‐temperature surfaces. The salinity gradient in the macrochannels passively triggers convective flow, facilitating the rapid transfer of salt ions from the high‐salt zone to the bulk water. Meanwhile, the macrochannels are spatially isolated from the high‐temperature zone, preventing heat loss during salt convection and thereby achieving a high evaporation rate (≈3 kg m−2 h−1) and superior salt rejection even in highly concentrated real seawater. This work provides new insights into salt rejection strategies and advances practical applications for sustainable seawater desalination.
Dipole Orientation Engineering in Crosslinking Polymer Blends for High‐Temperature Energy Storage Applications
Authors: Pan Zizhao , Li Li , Jin Fei , Dong Jiufeng , Niu Yujuan , Sun Liang , Tan Li , Liu Yuqi , Wang Qing , Wang Hong 
Published: August 2024

AbstractPolymer dielectrics that perform efficiently under harsh electrification conditions are critical elements of advanced electronic and power systems. However, developing polymer dielectrics capable of reliably withstanding harsh temperatures and electric fields remains a fundamental challenge, requiring a delicate balance in dielectric constant (K), breakdown strength (Eb), and thermal parameters. Here, amide crosslinking networks into cyano polymers is introduced, forming asymmetric dipole pairs with differing dipole moments. This strategy weakens the original electrostatic interactions between dipoles, thereby reducing the dipole orientation barriers of cyano groups, achieving dipole activation while suppressing polarization losses. The resulting styrene‐acrylonitrile/crosslinking styrene‐maleic anhydride (SAN/CSMA) blends exhibit a K of 4.35 and an Eb of 670 MV m−1 simultaneously at 120 °C, and ultrahigh discharged energy densities (Ue) with 90% efficiency of 8.6 and 7.4 J cm−3 at 120 and 150 °C are achieved, respectively, more than ten times that of the original dielectric at the same conditions. The SAN/CSMA blends show excellent cyclic stability in harsh conditions. Combining the results with SAN/CSMA and ABS (acrylonitrile‐butadiene‐styrene copolymer)/CSMA blends, it is demonstrated that this novel strategy can meet the demands of high‐performing dielectric polymers at elevated temperatures.
Porous Structure Enhances the Longitudinal Piezoelectric Coefficient and Electromechanical Coupling Coefficient of Lead‐Free (Ba0.85Ca0.15)(Zr0.1Ti0.9)O3
Authors: Li Zihe , Roscow James , Khanbareh Hamideh , Davies Philip R. , Han Guifang , Qin Jingyu , Haswell Geoff , Wolverson Daniel , Bowen Chris 
Published: August 2024

AbstractThe introduction of porosity into ferroelectric ceramics can decrease the effective permittivity, thereby enhancing the open circuit voltage and electrical energy generated by the direct piezoelectric effect. However, the decrease in the longitudinal piezoelectric coefficient (d33) with increasing porosity levels currently limiting the range of pore fractions that can be employed. By introducing aligned lamellar pores into (Ba0.85Ca0.15)(Zr0.1Ti0.9)O3, this paper demonstrates an unusual 22–41% enhancement in the d33 compared to its dense counterpart. This unique combination of high d33 and a low permittivity leads to a significantly improved voltage coefficient (g33), energy harvesting figure of merit (FoM33) and electromechanical coupling coefficient (). The underlying mechanism for the improved properties is demonstrated to be a synergy between the low defect concentration and high internal polarizing field within the porous lamellar structure. This work provides insights into the design of porous ferroelectrics for applications related to sensors, energy harvesters, and actuators.
Microneedle‐Delivered PDA@Exo for Multifaceted Osteoarthritis Treatment via PI3K‐Akt‐mTOR Pathway
Authors: Li Zihua , Lu Hengli , Fan Limin , Ma Xiaoyi , Duan Zhengwei , Zhang Yiwei , Fu Yuesong , Wang Sen , Guan Yonghao , Yang Dong , Chen Qingjing , Xu Tianyang , Yang Yunfeng 
Published: August 2024

AbstractOsteoarthritis (OA) is marked by cartilage deterioration, subchondral bone changes, and an inflammatory microenvironment. The study introduces the Microneedle‐Delivered Polydopamine‐Exosome (PDA@Exo MN), a therapeutic that not only preserves cartilage and promotes bone regeneration but also improves localized drug delivery through enhanced penetration capabilities. PDA@Exo MN shows strong reactive oxygen species (ROS) scavenging abilities and high biocompatibility, fostering osteogenesis and balancing anabolic and catabolic processes in cartilage. It directs macrophage polarization from M0 to the anti‐inflammatory M2 phenotype. RNA sequencing of treated chondrocytes demonstrates restored cellular function and activated antioxidant responses, with modulated inflammatory pathways. The PI3K‐AKT‐mTOR pathway's activation, essential for PDA@Exo's effects, is confirmed via bioinformatics and Western blot. In vivo assessments robustly validate that PDA@Exo MN prevents cartilage degradation and OA progression, supported by histological assessments and micro‐CT analysis, highlighting its disease‐modifying impact. The excellent biocompatibility of PDA@Exo MN, verified through histological (H&E) and blood tests showing no organ damage, underscores its safety and efficacy for OA therapy, making it a novel and multifunctional nanomedical approach in orthopedics, characterized by organ‐friendliness and biosecurity.
Fine‐Tuning the Microstructure and Photophysical Characteristics of Fluorescent Conjugated Copolymers Using Photoalignment and Liquid‐Crystal Ordering
Authors: Shi Yuping , Landfester Katharina , Morris Stephen M. 
Published: August 2024

AbstractReplicating the microstructural basis and the near 100% excitation energy transfer efficiency in naturally occurring light‐harvesting complexes (LHCs) remains challenging in synthetic energy‐harvesting devices. Biological photosynthesis regulates active ensembles of light‐absorbing and funneling chlorophylls in proteins in response to fluctuating sunlight. Here, use of long‐range liquid crystal (LC) ordering to tailor chain orientation and packing structure in liquid crystalline conjugated polymer (LCCP) layers for bio‐mimicry of certain structural basis and light‐harvesting properties of LHCs is reported. It is found that long‐range orientational ordering in an LC phase of poly(9,9‐dioctylfluorene‐co‐benzothiadiazole) (F8BT) copolymer stabilizes a small fraction of randomly‐oriented F8BT nanocrystals dispersed in an amorphous matrix of F8BT chains, resembling a self‐doped host–guest system whereby excitation energy funneling and photoluminescence quantum efficiencies are enhanced significantly by triggering 3D donor‐to‐acceptor Förster resonance energy transfer (FRET) and dominant intrachain emission in the nano‐crystal acceptor. Further, photoalignment of nematic F8BT layers is combined with LC orientational ordering to fabricate large‐area‐extended monodomains exhibiting >60% crystallinity and ≈20 nm‐long interchain packing order. Remarkably, these monodomains demonstrate strong linearly polarized emission, whilst also promoting a new band‐edge absorption species and an extra emissive interchain excited state as compared to the non‐aligned films.