bluuebunny/crossref_metadata_2025_split huggingface dataset:
Multifunctional Reconfigurable Electromagnetic Metamaterials Based on Compression‐Torsion Coupling Structures for Transmission Modulations and Holographic Displays
Authors: He Shuchang , Yao Xincheng , Tao Jie , Wang Kai , Tang Haishan , Wang Chengjun , Gao Fei , Wang Zuojia , Song Jizhou 
Published: January 2025

AbstractMechanically controlled reconfigurable electromagnetic metamaterials that can dynamically modulate their electromagnetic properties by simple mechanical compression/stretch hold great potential in wavefront control, tunable filtering, and holographic display. Undesired operating frequency shift and difficult independent controlling of unit cells in existing mechanically controlled reconfigurable metamaterials greatly limit their wide developments. Here, a multifunctional reconfigurable electromagnetic metamaterial based on a compression‐torsion coupling structure with the unit cell featuring a split‐ring resonator, a pair of parallel square frames, and four inclined beams between the frames, is reported. The unit cells can be globally or selectively compressed to induce the uniform or patterned in‐plane rotations of split‐ring resonators, enabling the multifunctionalities of electromagnetic transmission modulation and holographic display, which are not easily accessible by existing mechanically controlled electromagnetic metamaterials based on in‐plane compression and tension schemes. Numerical and experimental studies are carried out to reveal the design and operation of reconfigurable metamaterials enabled by the compression‐torsion coupling structure. Demonstrations of the metamaterials in modulating the transmittance of linearly polarized waves with stable resonant frequencies and multi‐imaged holographic display functions illustrate the versatility and feasibility of compression‐torsion strategy in realizing multifunctional electromagnetic metamaterials.
Polymorphs of the n‐Type Polymer P(NDI2OD‐T2): A Comprehensive Description of the Impact of Processing on Crystalline Morphology and Charge Transport
Authors: Karunasena Chamikara , Thurston Jonathan R. , Chaney Thomas P. , Li Hong , Risko Chad , Coropceanu Veaceslav , Toney Michael F. , Bredas Jean‐Luc 
Published: January 2025

AbstractA systematic study of the polymorphs emerging in P(NDI2OD‐T2) (also commercially known as N2200), a prototypical organic semiconducting n‐type polymer, is presented. Using a tightly integrated experimental and computational approach, detailed atomistic‐level descriptions are provided investigating the three known P(NDI2OD‐T2) polymorphs observed at room temperature as a function of thin‐film processing. Importantly, over the course of the work, a missing link is uncovered, a fourth polymorph referred to here as Form I‐𝜷; this new form is a morphological intermediary observed upon thermal annealing, which evolves from Form I but tends to disappear upon full polymer chain melting. The computationally derived polymorph structures show excellent agreement with experimental X‐ray scattering characterization. The relative stabilities of each polymorph are calculated in terms of both the bulk material and the polymorph‐air interface. An energy landscape is then constructed to qualitatively compare the thermodynamic versus kinetic origins of each polymorph, and the factors driving (supra)assembly and associated transformations among polymorphs using an approach generalizable to other organic semiconducting polymers. Lastly, the relationships among preferential polymorphic crystallinity, relative chain orientations, and directional charge transport properties in P(NDI2OD‐T2) are explored. Overall, this work provides unprecedented insights into complex structure‐processing‐transport relationships in a representative semiconducting organic polymer.
A Multifunctional Surface Modifier Capable of Stabilizing 5.0 V Graphite Cathode via Reinforced Mechanical Strength and Preferential Anion Adsorption
Authors: Li Yuqing , Xiong Weixing , Qu Qunting , Shao Jie , Wang Longfei , Wang Ru , Yan Ying , Zheng Honghe 
Published: January 2025

AbstractWith the ever‐increasing demand for high power and high energy batteries, extensive researches devote to high voltage cathode materials. Graphite cathode‐based dual‐ion batteries (DIBs) possess the unique advantages of high working voltage (≈4.5−5.0) and high power, but still suffer from low coulombic efficiency and poor long‐term stability mainly resulted by the serious oxidative decomposition of electrolytes and significant structural deterioration of graphite cathode. From the perspectives of simultaneously reinforcing the mechanical strength of graphite cathode and suppressing the decomposition of electrolytes via a cathode/electrolyte interphase (CEI), polyacrylic acid (PAA) is adopted as the surface modifier of natural graphite (NG). The mechanical stability of graphite cathode is significantly improved by virtue of the bonding interaction between PAA and binder, which is validated through both theoretical calculation and experimental observation. In addition, PAA contributes to the formation of a LiF‐rich and homogeneous CEI through the preferential adsorption of anions, and effectively mitigates the cointercalation and decomposition of solvent. As the cathode material of DIBs, NG@PAA manifests fast charge/discharge capability and outstanding capacity retention of 73.9% after 8000 cycles. This work provides a surface modification strategy for optimizing the performance of electrode materials from multiple perspectives.
Oriented Cortical‐Bone‐Like Silk Protein Lamellae Effectively Repair Large Segmental Bone Defects in Pigs
Authors: Shuai Yajun , Yang Tao , Zheng Meidan , Zheng Li , Wang Jie , Mao Chuanbin , Yang Mingying 
Published: January 2025

AbstractAssembling natural proteins into large, strong, bone‐mimetic scaffolds for repairing bone defects in large‐animal load‐bearing sites remain elusive. Here this challenge is tackled by assembling pure silk fibroin (SF) into 3D scaffolds with cortical‐bone‐like lamellae, superior strength, and biodegradability through freeze‐casting. The unique lamellae promote the attachment, migration, and proliferation of tissue‐regenerative cells (e.g., mesenchymal stem cells [MSCs] and human umbilical vein endothelial cells) around them, and are capable of developing in vitro into cortical‐bone organoids with a high number of MSC‐derived osteoblasts. High‐SF‐content lamellar scaffolds, regardless of MSC inoculation, regenerated more bone than non‐lamellar or low‐SF‐content lamellar scaffolds. They accelerated neovascularization by transforming macrophages from M1 to M2 phenotype, promoting bone regeneration to repair large segmental bone defects (LSBD) in minipigs within three months, even without growth factor supplements. The bone regeneration can be further enhanced by controlling the orientation of the lamella to be parallel to the long axis of bone during implantation. This work demonstrates the power of oriented lamellar bone‐like protein scaffolds in repairing LSBD in large animal models.
Biopolymer‐Derived Carbon Materials for Wearable Electronics
Authors: Jin Jiongke , Ma Haoxuan , Liang Huarun , Zhang Yingying 
Published: January 2025

AbstractAdvanced carbon materials are widely utilized in wearable electronics. Nevertheless, the production of carbon materials from fossil‐based sources raised concerns regarding their non‐renewability, high energy consumption, and the consequent greenhouse gas emissions. Biopolymers, readily available in nature, offer a promising and eco‐friendly alternative as a carbon source, enabling the sustainable production of carbon materials for wearable electronics. This review aims to discuss the carbonization mechanisms, carbonization techniques, and processes, as well as the diverse applications of biopolymer‐derived carbon materials (BioCMs) in wearable electronics. First, the characteristics of four representative biopolymers, including cellulose, lignin, chitin, and silk fibroin, and their carbonization processes are discussed. Then, typical carbonization techniques, including pyrolysis carbonization, laser‐induced carbonization, Joule heating carbonization, hydrothermal transformation, and salt encapsulation carbonization are discussed. The influence of the processes on the morphology and properties of the resultant BioCMs are summarized. Subsequently, applications of BioCMs in wearable devices, including physical sensors, chemical sensors, energy devices, and display devices are discussed. Finally, the challenges currently facing the field and the future opportunities are discussed.
Transforming Adsorbate Surface Dynamics in Aqueous Electrocatalysis: Pathways to Unconstrained Performance
Authors: Do Viet‐Hung , Lee Jong‐Min 
Published: January 2025

AbstractDeveloping highly efficient catalysts to accelerate sluggish electrode reactions is critical for the deployment of sustainable aqueous electrochemical technologies, yet remains a great challenge. Rationally integrating functional components to tailor surface adsorption behaviors and adsorbate dynamics would divert reaction pathways and alleviate energy barriers, eliminating conventional thermodynamic constraints and ultimately optimizing energy flow within electrochemical systems. This approach has, therefore, garnered significant interest, presenting substantial potential for developing highly efficient catalysts that simultaneously enhance activity, selectivity, and stability. The immense promise and rapid evolution of this design strategy, however, do not overshadow the substantial challenges and ambiguities that persist, impeding the realization of significant breakthroughs in electrocatalyst development. This review explores the latest insights into the principles guiding the design of catalytic surfaces that enable favorable adsorbate dynamics within the contexts of hydrogen and oxygen electrochemistry. Innovative approaches for tailoring adsorbate‐surface interactions are discussed, delving into underlying principles that govern these dynamics. Additionally, perspectives on the prevailing challenges are presented and future research directions are proposed. By evaluating the core principles and identifying critical research gaps, this review seeks to inspire rational electrocatalyst design, the discovery of novel reaction mechanisms and concepts, and ultimately, advance the large‐scale implementation of electroconversion technologies.
Combined Electrooxidation and Proline Catalysis for Asymmetric Formal Cross‐Dehydrogenative Coupling of Benzylic Alcohols with Ketones
Authors: Pu Hong‐Ping , Long Chao‐Jiu , Liu Zhe‐Kai , Guan Zhi , He Yan‐Hong 
Published: January 2025

AbstractThis article presents a method for asymmetric formal cross‐dehydrogenative coupling of benzylic alcohols with ketones through combined electrooxidation and organocatalysis. Employing inexpensive and environmentally friendly proline as a chiral organocatalyst, various benzylic alcohols and simple ketones serve as substrates to directly obtain diverse chiral β‐hydroxycarbonyl compounds with moderate to good yields (up to 85%) and excellent stereoselectivity (up to 99% ee and 99:1 dr). The reaction proceeds under mild conditions at room temperature in air, without oxidants or additives, demonstrating robust functional group tolerance and atom efficiency. Hydrogen gas released at the cathode is the sole byproduct. Using L‐ or D‐proline allows straightforward access to both chiral configurations of β‐hydroxycarbonyl compounds.
Visible Light‐Promoted Cascade Sulfonylation‐Cyclization‐Aromatization of Tertiary Enamides to Access Multi‐Substituted Pyridines and 1,2‐Dihydropyridines
Authors: Xu Xin‐Ming , Wang Jiping , Chen Sen , Chen Xiaoxu , Chen Jinchun , Liu Qian , Wang Zu‐Li , Tian Miao , Sun Kai 
Published: January 2025

AbstractFunctionalized pyridines and 1,2‐dihydropyridines are crucial organic entities in natural products, organic materials, drugs and catalysts. Despite progress, a facile and eco‐friendly synthesis remains desirable so far. In this context, we disclose a novel visible light‐promoted radical cascade sulfonylation‐cyclization‐aromatization of N‐propargyl enamides with selenosulfonates. This approach avoids the use of metal‐ or photocatalyst, bases and external oxidants, marking a significant advance in sustainable and green chemistry accords. Utilizing this protocol, we successfully synthesized a diverse range of sulfonated 1,2‐dihydropyridines and pyridines, featuring good functional group compatibility, simple operation and mild condition.
Optimal Neutron Spectrum Database for In‐reactor 238Pu Production
Authors: Pan Qingquan , Liu Xiaojing , Cai Yun 
Published: January 2025

AbstractPlutonium‐238 (238Pu) is a scarce heat‐source radioisotope used in nuclear batteries, which is produced by in‐reactor irradiation of Americium‐241 (241Am) or Neptunium‐237 (237Np). Optimizing the neutron spectrum can improve the production efficiency of 238Pu, but currently, it is still a lack of knowledge about the optimal neutron spectrum for 238Pu production. Genetic algorithms and burnup algorithms are combined to identify optimal neutron spectra for 238Pu production under various irradiation times and flux levels, and build an optimal neutron spectrum database, which answers the questions “What is the optimal neutron spectrum for 238Pu production?” and “What is the maximum efficiency for 238Pu production” once and for all. This database can be referred to for determining the optimal neutron spectrum, guiding the neutron spectrum regulation process to improve the yield of 238Pu. Moreover, these results find that the production method of in‐reactor irradiation 237Np not only has a higher yield but also achieves a higher purity of 238Pu than that of in‐reactor irradiation 241Am, which conflicts with the traditional experiences, providing with previously unknown insights and helping break through the efficiency limit of traditional methods, maximizing 238Pu production.
Unlocking Interpretable Prediction of Battery Random Discharge Capacity With Domain Adaptative Physics Constraint
Authors: Che Yunhong , Guo Jia , Zheng Yusheng , Stroe Daniel‐Ioan , Liu Wenxue , Hu Xiaosong , Teodorescu Remus 
Published: January 2025

AbstractTracking the battery discharge capacity is significant, yet challenging due to complicated degradation patterns as well as varying or even random usage scenarios. This work proposes a physics‐constrained domain adaptation framework to predict the capacities during random discharge with non‐destructive mechanism diagnosis using early or random discharging information. By imposing the impedance as physical constraints in a domain adaptative layer, the interpretability and generalization of the model can be improved as the physics‐constrained layer provides physical insights into the battery mechanism characteristics, enabling onboard and non‐destructive diagnosis without complex tests. The learned impedances in the physics‐constrained layer are well‐fitted to the real ones, suggesting accurate physical insights and, therefore, good interpretability of the trained model. Furthermore, apart from capacity prediction, the aging mechanisms of the cell can be interpreted through the learned physics from this deep learning framework without impedance measurement. Such interpretation has also been validated experimentally through post‐mortem analysis. This work provides an example of grey‐box modeling of complex dynamic systems where deep learning models can provide certain physical details to increase the model's interpretability.
Advancing Thermoelectrics in Lead‐Free Rhombohedral GeTe via Interfacial Engineering With MXene
Authors: Xu Fang , Liu Bo , Ang Ran 
Published: January 2025

AbstractLead‐containing GeTe‐based thermoelectric (TE) materials exhibit outstanding performance, but the toxicity of lead (Pb) limits their practical applications. Lead‐free GeTe‐based TE materials present a promising alternative for environmentally sustainable and scalable applications. Here, Bi doping is used to reduce the majority carrier concentration in GeTe, combined with uniform incorporation of nanoscale layered MXene via high‐energy ball milling. This approach significantly enhances the structural symmetry of GeTe, while MXene further reduces carrier concentration and improves carrier mobility. Consequently, the Ge0.93Bi0.07Te‐0.6 mass% MXene sample achieves an impressive average power factor of ≈28.40 µW m−1 K−2 across 303–603 K. Moreover, point defects, multilayer nanostructures, and grain boundaries reduce thermal conductivity to ≈1.04 W m−1 K−1 at 603 K. A maximum ZTmax of ≈2.1 at 603 K, an average ZTavg of ≈1.1, and a Vickers microhardness of ≈ 236.75 Hv are obtained. In particular, a high power density of ≈1.54 W cm−2 and a maximum conversion efficiency of ≈7.5% at a temperature difference of 300 K are achieved in a 7‐pair TE module. These outcomes represent the highest performance levels for lead‐free GeTe‐based materials. This work uncovers a straightforward method to enhance the structural symmetry of GeTe‐based compounds, providing insights for advancing lead‐free TE technologies.
A Multi‐Component Reaction of Hexafluoro‐1,4‐naphthoquinone with N‐Heterocycles and Active Methylene Compounds: A Straightforward Approach to Polyfluorinated Zwitterions
Authors: Kudryavtseva Ekaterina N. , Lichitsky Boris V. , Tretyakov Evgeny V. 
Published: January 2025

AbstractFor the first time, multi‐component condensation of hexafluoro‐1,4‐naphthoquinone with nitrogen‐containing heterocycles and active methylene compounds was studied. It was shown that the aforementioned process leads to the formation of a previously undescribed type of zwitterionic derivatives. Based on the results, a general one‐step method for preparation of polyfluorinated pyridine‐containing betaines was developed. Advantages of the proposed synthetic protocol are atom economy, readily available starting materials and simple isolation of target products without chromatographic purification. The obtained zwitterions were utilized as precursors for the preparation of new fluorinated polycyclic compounds: pyrido[1,2‐a]indole‐6,11‐diones and naphtho[2,3‐b]furan‐4,9‐diones.
Soluble Covalent Organic Frameworks as Efficient Lithiophilic Modulator for High‐Performance Lithium Metal Batteries
Authors: Xu Shen , Naren Tuoya , Zhao Yanwei , Gu Qianfeng , Wai Lau Ting , Lee Chun‐Sing , Chen Fu‐Rong , Yin Jun , Chen Libao , Zhang Qichun 
Published: January 2025

AbstractLithium metal batteries (LMBs) are regarded as the potential alternative of lithium‐ion batteries due to their ultrahigh theoretical specific capacity (3860 mAh g−1). However, severe instability and safety problems caused by the dendrite growth and inevitable side reactions have hindered the commercialization of LMBs. To solve them, in this contribution, a design strategy of soluble lithiophilic covalent organic frameworks (COFs) is proposed. By introducing polyethylene glycol as the side chains, two COFs (CityU‐28 and CityU‐29) not only become soluble for the facile coating technique, but also can facilitate the lithium‐ion migration in batteries. Furthermore, when coated on the lithium anode of LMB, both COFs can act as artificial solid electrolyte interphase to prevent dendrite growth thus enabling the long‐term stability of the cells. Notably, the symmetric CityU‐29@Li cell can work for more than 5000 h at a current density of 2 mA cm−2 and an areal capacity of 1 mAh cm−2. A remarkable capacity retention of 78.9 % after 1500 cycles and a Coulombic efficiency of about 99.9 % at 1.0 C can also be realized in CityU‐29@Li||LiFePO4 full cell. This work could provide a universal design strategy for soluble COFs and enlighten their application in diverse scenarios, especially energy‐related fields.
Exceptional Battery‐level Safety of High Energy Density Lithium‐Ion Batteries through Non‐Flammable and Low‐Exothermic Localize High Concentration Electrolytes
Authors: Qiu Huamin , Jia Hao , Zhou Yifan , Wang Jun , Zhao Wenguang , Xu Kaiyang , Li Zimu , Song Shuqin , Wang Yi 
Published: January 2025

AbstractThe poor safety performance of high energy density lithium‐ion batteries (LIBs) is drawing increasing public concern. To enhance the safety performance on the battery level, it is indispensable to design safe electrolytes that are both non‐flammable and low exothermic under abusive conditions. By rational design, a safe localize high concentration electrolyte (LHCE) with non‐flammability and extremely low exothermicity is formulated. Compared with conventional LiPF6‐organocabonate electrolytes and previous LHCEs, the heat generated by the reaction between the safe LHCE and fully charged electrodes under abusive conditions is significantly reduced. Because of the non‐flammability and low‐exothermicity of the safe LHCE, high energy density LIB (1800 mAh Gr||LiNi0.7Mn0.2Co0.1O2, fully charged to 4.3 V) with the safe LHCE successfully passes the nail penetration test. Because of the excellent interphasial properties of the safe LHCE, the cycle life and the rate capability of high energy density LIBs are significantly improved when the safe LHCE is adopted. This work sheds light on the design principles of electrolytes for achieving battery‐level safety.
Asymmetric Functionalization Harnessing Radical‐Mediated Functional‐Group Migration
Authors: Chen Fushan , Cao Zhu , Zhu Chen 
Published: January 2025

AbstractAlong with the renaissance of radical chemistry, the past decade has witnessed rapid development in radical‐mediated rearrangement reactions. A wide diversity of radical approaches harnessing functional‐group migration (FGM) have been devised to enhance both synthetic efficiency and molecular complexity. However, the application of FGM reactions to construct stereogenic centers remains underexplored owing to the inherent challenges of asymmetric radical reactions. In this Minireview, we summarize the emerging area of asymmetric functionalization involving radical‐mediated FGM reactions. Enantioselectivity can be regulated by chiral substrates, auxiliaries or reagents, or achieved through asymmetric transition‐metal catalysis. This synthetic strategy demonstrates its superiority in the production of valuable complex molecules that are otherwise difficult to obtain by conventional methods.
The First Kleinman‐type Second‐Harmonic Generation Circular Dichroism On/Off Switchable Ferroelectrics
Authors: Peng Hang , Qin Yan , Chen Xiao‐Gang , Song Xian‐Jiang , Xiong Ren‐Gen , Liao Wei‐Qiang 
Published: January 2025

AbstractChiral ferroelectrics have recently received considerable interest due to their unique chiroptical properties. They can adopt Kleinman symmetry second‐harmonic generation (SHG)‐active chiral‐polar point groups in the ferroelectric phase while Kleinman symmetry SHG‐inactive chiral‐nonpolar point groups in the paraelectric phase, providing a great opportunity to realize on/off switching of SHG circular dichroism (SHG‐CD) response. However, the SHG‐CD effect was rarely explored in chiral ferroelectrics, and the on/off switchable SHG‐CD has never been reported. Herein, we report the first crown ether‐based chiral ferroelectrics (R/S‐CS)Ca(18‐crown‐6) (CS=camphor‐10‐sulfonic acid), which undergo a 422F2 type ferroelectric phase transition at around 336 K from Kleinman symmetry SHG‐active point group 2 to Kleinman symmetry SHG‐inactive point group 422. Notably, they exhibit obvious SHG‐CD responses with an anisotropy factor of up to 0.31. More importantly, the SHG‐CD response can be switched between SHG‐CD active (SHG‐CD on) and inactive (SHG‐CD off) states during the ferroelectric phase transition, which is unprecedented. To the best of our knowledge, this is the first example of Kleinman‐type SHG‐CD on/off switchable ferroelectric. Our findings open up a new way to switch SHG‐CD response based on chiral ferroelectrics, which would greatly inspire the further exploration of switchable SHG‐CD effects in chiral ferroelectrics.