Pub Date : 2025-12-31DOI: 10.1016/j.jmat.2025.101159
Xiali Liang , Jian Wang , Wanbiao Hu
Chemical doping represents a crucial and effective approach for controlling electricity and also many other properties, but the underlying mechanisms connecting dopant-induced structural evolutions to emergent functionalities remain incompletely understood. To address this knowledge gap, the atomic-level mechanism of the enhanced electric polarization in a typical perovskite ferroelectric oxide BiFeO3 (BFO) is unveiled. B-site Mn-dopping, with bringing about atomic-level lattice and charge evolutions, clearly accelerates the local lattice distortion i.e. enhanced Fe/Mn displacement and (Fe/Mn)O6 octahedral rotation. This facilitates large-scale polarization orientation alignment to create the enhanced collective polarity while manifesting an overall ferroelectric polarization of up to ∼160 μC/cm2. Local lattice distortion also promotes the Jahn-Teller effect because of the increasing proportion in Mn3+ (3d4 configuration) that could instigate symmetry-breaking stretching and bending distortions of (Fe/Mn)O6 octahedra with showing improved magnetic moments. Our findings uncover the ferroelectricity-enhanced origination and offer a new paradigm for principally designing ferroelectric functions.
{"title":"Atomic scale octahedral distortion and enhanced collective polarity underlying large polarization in ferroelectric perovskite oxides","authors":"Xiali Liang , Jian Wang , Wanbiao Hu","doi":"10.1016/j.jmat.2025.101159","DOIUrl":"10.1016/j.jmat.2025.101159","url":null,"abstract":"<div><div>Chemical doping represents a crucial and effective approach for controlling electricity and also many other properties, but the underlying mechanisms connecting dopant-induced structural evolutions to emergent functionalities remain incompletely understood. To address this knowledge gap, the atomic-level mechanism of the enhanced electric polarization in a typical perovskite ferroelectric oxide BiFeO<sub>3</sub> (BFO) is unveiled. B-site Mn-dopping, with bringing about atomic-level lattice and charge evolutions, clearly accelerates the local lattice distortion <em>i.e.</em> enhanced Fe/Mn displacement and (Fe/Mn)O<sub>6</sub> octahedral rotation. This facilitates large-scale polarization orientation alignment to create the enhanced collective polarity while manifesting an overall ferroelectric polarization of up to ∼160 μC/cm<sup>2</sup>. Local lattice distortion also promotes the Jahn-Teller effect because of the increasing proportion in Mn<sup>3+</sup> (3d<sup>4</sup> configuration) that could instigate symmetry-breaking stretching and bending distortions of (Fe/Mn)O<sub>6</sub> octahedra with showing improved magnetic moments. Our findings uncover the ferroelectricity-enhanced origination and offer a new paradigm for principally designing ferroelectric functions.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101159"},"PeriodicalIF":9.6,"publicationDate":"2025-12-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894283","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
BiFeO3BaTiO3 lead-free piezoelectric ceramics exhibit superior piezoelectric properties while preserving a high Curie temperature. However, given the inherent Gibbs free energy law of BiFeO3, the system is difficult to avoid heterogeneous phases such as Bi25FeO39 and/or Bi2Fe4O9, which are accompanied by the volatilization of Bi3+ and the change of Fe3+, resulting in low insulating properties and high dielectric loss. These factors hinder the enhancement of polarizability and the overall performance at elevated temperatures and electric field conditions. The present study focuses on a highly leaky 0.75BiFeO3–0.25BaTiO3 ceramic, in which the Fe content is deliberately designed to be both severely excessive and deficient, and is prepared using a one-step low-temperature sintering process. It is noteworthy that the structural stability and defect suppression, even in this challenging system, are achieved via the one-step low-temperature sintering. This samples exhibit a distinctive self-tuning property and an excellent stability over a wide compositional range. First-principles density functional theory calculations and XPS analysis have for the first time confirmed that suppressing oxygen vacancies and Fe3+ valence states can reduce the concentration and mobility of hole carriers, thereby effectively reducing leakage current, with the mechanism shifting from ohmic conduction to space-charge-limited conduction. Even under the extreme compositional conditions of x = ± 5 and a low sintering temperature, the piezoelectric coefficients d33 reach 132 pC/N and 110 pC/N, respectively. These are significantly higher than those of the most stoichiometric 0.75BiFeO3–0.25BaTiO3 counterparts, setting a new performance record.
{"title":"One-step sintering enabled structural stability and defect suppression even in Fe-off-stoichiometric BiFeO3BaTiO3 piezoceramics","authors":"Shiyuan Zhang, Xingyuan Qi, Jinhao Hu, Xianxin Zhang, Mengping Xue, Bo-Ping Zhang","doi":"10.1016/j.jmat.2025.101158","DOIUrl":"10.1016/j.jmat.2025.101158","url":null,"abstract":"<div><div>BiFeO<sub>3</sub><img>BaTiO<sub>3</sub> lead-free piezoelectric ceramics exhibit superior piezoelectric properties while preserving a high Curie temperature. However, given the inherent Gibbs free energy law of BiFeO<sub>3</sub>, the system is difficult to avoid heterogeneous phases such as Bi<sub>25</sub>FeO<sub>39</sub> and/or Bi<sub>2</sub>Fe<sub>4</sub>O<sub>9</sub>, which are accompanied by the volatilization of Bi<sup>3+</sup> and the change of Fe<sup>3+</sup>, resulting in low insulating properties and high dielectric loss. These factors hinder the enhancement of polarizability and the overall performance at elevated temperatures and electric field conditions. The present study focuses on a highly leaky 0.75BiFeO<sub>3</sub>–0.25BaTiO<sub>3</sub> ceramic, in which the Fe content is deliberately designed to be both severely excessive and deficient, and is prepared using a one-step low-temperature sintering process. It is noteworthy that the structural stability and defect suppression, even in this challenging system, are achieved via the one-step low-temperature sintering. This samples exhibit a distinctive self-tuning property and an excellent stability over a wide compositional range. First-principles density functional theory calculations and XPS analysis have for the first time confirmed that suppressing oxygen vacancies and Fe<sup>3+</sup> valence states can reduce the concentration and mobility of hole carriers, thereby effectively reducing leakage current, with the mechanism shifting from ohmic conduction to space-charge-limited conduction. Even under the extreme compositional conditions of <em>x</em> = ± 5 and a low sintering temperature, the piezoelectric coefficients <em>d</em><sub>33</sub> reach 132 pC/N and 110 pC/N, respectively. These are significantly higher than those of the most stoichiometric 0.75BiFeO<sub>3</sub>–0.25BaTiO<sub>3</sub> counterparts, setting a new performance record.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101158"},"PeriodicalIF":9.6,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894284","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-27DOI: 10.1016/j.jmat.2025.101157
Tauqeer Ahmad , Wen Lei , Burhan Ullah , Wen-zhong Lu
A series of (Sr0.4Ce0.4)TiO3 + 4% (in mass) Sr2CeO4 + x% B2O3 (SCTO + 4% SCO + x% B2O3 for 1≤ x ≤ 5) composites were synthesized via solid-state reaction to investigate the effects of Sr2CeO4 and B2O3 additives on their structural evolution and microwave dielectric properties. X-ray diffraction (XRD) and Rietveld refinement confirmed the dominant orthorhombic phase (O-phase), with SCO as a secondary phase, indicating a chemically stable composite system. HRTEM and SAED analyses further confirmed the formation of the O-phase through direct observation of the superlattice reflections. Microstructural evolution demonstrated B2O3-assisted liquid-phase sintering, reducing porosity (0.017 → 0.006) and increasing grain size (3.34 → 6.01 μm) with increasing x% (in mass). Raman spectroscopy verified octahedral tilting and CeO stretching, while B2O3 incorporation modified the TiO6 network via BO3/BO4 interactions. The εr decreased from 113 (SCTO) to 27 at x = 5%, while τf improved from +213 to +12 × 10−6/°C. The reduction in εr arises from a complex interplay of internal factors (ionic polarizability) and external factors (porosity, and density), whereas the variation in τf is governed by compensating effects from Sr2CeO4 and B2O3. Optimal microwave performance was achieved at x = 5%, with Q×f = 43,603 GHz, εr = 27, and τf of +12 × 10−6/°C. The study demonstrates that SCO and B2O3 act as effective modifiers, enhancing densification and dielectric properties in SCTO-based microwave ceramics.
{"title":"Low-loss (Sr,Ce)TiO3Sr2CeO4B2O3 ceramics composite featuring balanced microwave dielectric properties for miniaturized wireless communication applications","authors":"Tauqeer Ahmad , Wen Lei , Burhan Ullah , Wen-zhong Lu","doi":"10.1016/j.jmat.2025.101157","DOIUrl":"10.1016/j.jmat.2025.101157","url":null,"abstract":"<div><div>A series of (Sr<sub>0.4</sub>Ce<sub>0.4</sub>)TiO<sub>3</sub> + 4% (in mass) Sr<sub>2</sub>CeO<sub>4</sub> + <em>x</em>% B<sub>2</sub>O<sub>3</sub> (SCTO + 4% SCO + <em>x</em>% B<sub>2</sub>O<sub>3</sub> for 1≤ <em>x</em> ≤ 5) composites were synthesized <em>via</em> solid-state reaction to investigate the effects of Sr<sub>2</sub>CeO<sub>4</sub> and B<sub>2</sub>O<sub>3</sub> additives on their structural evolution and microwave dielectric properties. X-ray diffraction (XRD) and Rietveld refinement confirmed the dominant orthorhombic phase (O-phase), with SCO as a secondary phase, indicating a chemically stable composite system. HRTEM and SAED analyses further confirmed the formation of the O-phase through direct observation of the superlattice reflections. Microstructural evolution demonstrated B<sub>2</sub>O<sub>3</sub>-assisted liquid-phase sintering, reducing porosity (0.017 → 0.006) and increasing grain size (3.34 → 6.01 μm) with increasing <em>x</em>% (in mass). Raman spectroscopy verified octahedral tilting and Ce<img>O stretching, while B<sub>2</sub>O<sub>3</sub> incorporation modified the TiO<sub>6</sub> network <em>via</em> BO<sub>3</sub>/BO<sub>4</sub> interactions. The <em>ε</em><sub>r</sub> decreased from 113 (SCTO) to 27 at <em>x</em> = 5%, while <em>τ</em><sub>f</sub> improved from +213 to +12 × 10<sup>−6</sup>/°C. The reduction in <em>ε</em><sub>r</sub> arises from a complex interplay of internal factors (ionic polarizability) and external factors (porosity, and density), whereas the variation in <em>τ</em><sub>f</sub> is governed by compensating effects from Sr<sub>2</sub>CeO<sub>4</sub> and B<sub>2</sub>O<sub>3</sub>. Optimal microwave performance was achieved at <em>x</em> = 5%, with <em>Q×f</em> = 43,603 GHz, <em>ε</em><sub>r</sub> = 27, and <em>τ</em><sub>f</sub> of +12 × 10<sup>−6</sup>/°C. The study demonstrates that SCO and B<sub>2</sub>O<sub>3</sub> act as effective modifiers, enhancing densification and dielectric properties in SCTO-based microwave ceramics.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101157"},"PeriodicalIF":9.6,"publicationDate":"2025-12-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145844897","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-26DOI: 10.1016/j.jmat.2025.101156
Ying Wang , Bo Yang , Hanqing Yu , Dingxin Shuai , Xiuqiong Hu , Ying Zhang , Jiyue Hou , Yiyong Zhang
Lithium-sulfur batteries (LSBs) exhibit high energy density and high theoretical specific capacity, approximately one order of magnitude higher than traditional lithium-ion batteries. However, the shuttling effect of lithium polysulfides (LiPSs) generated during the charge-discharge process severely compromises battery performance and hinders commercialization. In this paper, a 3D porous carbon gel sulfur host, M@rGO–PCG (M = Ni, Co), composed of transition metal particles and redox graphene, was fabricated through gelation and freeze-drying techniques. This material enhances the conductivity of the cathode, buffers the volume expansion of the electrode, and further accelerates the catalytic conversion of LiPSs. The assembled Ni@rGO–PCG/S and Co@rGO–PCG/S batteries deliver initial discharge specific capacities of 1390.0 mA⋅h⋅g−1 and 1603.6 mA⋅h⋅g−1 at a current rate of 0.1C, respectively. The findings provide valuable insights into the synergistic suppression of the shuttling effect through multiple functions.
{"title":"3D porous carbon gel composite with transition metal particles for anchoring-diffusion-conversion of polysulfides for lithium–sulfur batteries","authors":"Ying Wang , Bo Yang , Hanqing Yu , Dingxin Shuai , Xiuqiong Hu , Ying Zhang , Jiyue Hou , Yiyong Zhang","doi":"10.1016/j.jmat.2025.101156","DOIUrl":"10.1016/j.jmat.2025.101156","url":null,"abstract":"<div><div>Lithium-sulfur batteries (LSBs) exhibit high energy density and high theoretical specific capacity, approximately one order of magnitude higher than traditional lithium-ion batteries. However, the shuttling effect of lithium polysulfides (LiPSs) generated during the charge-discharge process severely compromises battery performance and hinders commercialization. In this paper, a 3D porous carbon gel sulfur host, M@rGO–PCG (M = Ni, Co), composed of transition metal particles and redox graphene, was fabricated through gelation and freeze-drying techniques. This material enhances the conductivity of the cathode, buffers the volume expansion of the electrode, and further accelerates the catalytic conversion of LiPSs. The assembled Ni@rGO–PCG/S and Co@rGO–PCG/S batteries deliver initial discharge specific capacities of 1390.0 mA⋅h⋅g<sup>−1</sup> and 1603.6 mA⋅h⋅g<sup>−1</sup> at a current rate of 0.1C, respectively. The findings provide valuable insights into the synergistic suppression of the shuttling effect through multiple functions.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101156"},"PeriodicalIF":9.6,"publicationDate":"2025-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145844898","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-22DOI: 10.1016/j.jmat.2025.101155
Thi Sinh Vo , Truong Sinh Nguyen , Seung-Hyun Lee , Kyunghoon Kim
Flexible and transparent strain sensors with high sensitivity were fabricated by embedding hybrid networks of carbon nanotubes (CNTs) and carbon (C) nanoparticles into micro-mesh polydimethylsiloxane (PDMS) substrates. The resulting devices exhibited optical transmittance above 70% and haze below 7%, ensuring unobtrusive integration on skin. Systematic variation of CNT:C ratios (0:1, 1:1, 2:1, 3:1) revealed that the 2:1 hybrid achieved optimal performance, combining uniform dispersion, strong interfacial adhesion, and robust conductive pathways. The optimized device (S2-PDMS) demonstrated a maximum gauge factor of 465.35 at 32.5% strain, and reliable cycling stability for repeatability of stretching, bending, and twisting deformations. Mechanical tests confirmed high tensile strength (2.63 MPa) and durability under repeated deformation, outperforming polyethylene terephthalate (PET)-based counterparts. The sensor also exhibited response times in the range of ∼158–557 ms and recovery times between ∼110 ms and 697 ms, depending on the type and complexity of the human motion. As such, the sensors successfully monitored diverse human motions, subtle muscle activity, and vocal vibrations, and enabled wireless data transmission via Bluetooth, underscoring their potential for real-time health monitoring, human–machine interfaces, and Internet of Things-enabled wearable electronics.
{"title":"Mesh-channel-integrated transparent devices with hybrid conductive networks for enhanced electromechanical sensing","authors":"Thi Sinh Vo , Truong Sinh Nguyen , Seung-Hyun Lee , Kyunghoon Kim","doi":"10.1016/j.jmat.2025.101155","DOIUrl":"10.1016/j.jmat.2025.101155","url":null,"abstract":"<div><div>Flexible and transparent strain sensors with high sensitivity were fabricated by embedding hybrid networks of carbon nanotubes (CNTs) and carbon (C) nanoparticles into micro-mesh polydimethylsiloxane (PDMS) substrates. The resulting devices exhibited optical transmittance above 70% and haze below 7%, ensuring unobtrusive integration on skin. Systematic variation of CNT:C ratios (0:1, 1:1, 2:1, 3:1) revealed that the 2:1 hybrid achieved optimal performance, combining uniform dispersion, strong interfacial adhesion, and robust conductive pathways. The optimized device (S2-PDMS) demonstrated a maximum gauge factor of 465.35 at 32.5% strain, and reliable cycling stability for repeatability of stretching, bending, and twisting deformations. Mechanical tests confirmed high tensile strength (2.63 MPa) and durability under repeated deformation, outperforming polyethylene terephthalate (PET)-based counterparts. The sensor also exhibited response times in the range of ∼158–557 ms and recovery times between ∼110 ms and 697 ms, depending on the type and complexity of the human motion. As such, the sensors successfully monitored diverse human motions, subtle muscle activity, and vocal vibrations, and enabled wireless data transmission <em>via</em> Bluetooth, underscoring their potential for real-time health monitoring, human–machine interfaces, and Internet of Things-enabled wearable electronics.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101155"},"PeriodicalIF":9.6,"publicationDate":"2025-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145813852","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-17DOI: 10.1016/j.jmat.2025.101153
Xingkun Ning, Yongmao Ran, Jiaying Han, Linjie Gao, Shufang Wang
Transparent thermoelectric CdO thin films exhibit critical flexibility and thermoelectric performance that require focused research to advance flexible transparent self-powered devices. Here, we demonstrate the superior flexibility of freestanding single-crystalline CdO membranes. These membranes achieve a notable room-temperature power factor of 1.48 μW·cm−1·K−2 and exhibit superior optical transmittance exceeding 94% in the 550–800 nm range. Crucially, freestanding CdO exhibits exceptional mechanical robustness, retaining >90% electrical conductivity after 1000 bending cycles (radius: 11.5 mm). Microstructure analyses confirm polycrystalline CdO films suffer from grain boundary cracking under bending due to stress concentration, but single-crystal CdO membranes—without grain boundaries to concentrate stress—exhibit better flexibility and resistance to cracking. Furthermore, curvature-induced strain boosts the power factor by 12.8%, providing a curvature-controlled strain engineering strategy to optimize flexible thermoelectric performance. This work establishes freestanding CdO as a highly efficient and flexible thermoelectric material and suggests a fundamental strategy for designing robust smart materials for transparent, self-powered flexible electronics.
{"title":"Remarkable flexibility and curvature-tunable thermoelectric properties in transparent freestanding single-crystalline CdO membranes","authors":"Xingkun Ning, Yongmao Ran, Jiaying Han, Linjie Gao, Shufang Wang","doi":"10.1016/j.jmat.2025.101153","DOIUrl":"10.1016/j.jmat.2025.101153","url":null,"abstract":"<div><div>Transparent thermoelectric CdO thin films exhibit critical flexibility and thermoelectric performance that require focused research to advance flexible transparent self-powered devices. Here, we demonstrate the superior flexibility of freestanding single-crystalline CdO membranes. These membranes achieve a notable room-temperature power factor of 1.48 μW·cm<sup>−1</sup>·K<sup>−2</sup> and exhibit superior optical transmittance exceeding 94% in the 550–800 nm range. Crucially, freestanding CdO exhibits exceptional mechanical robustness, retaining >90% electrical conductivity after 1000 bending cycles (radius: 11.5 mm). Microstructure analyses confirm polycrystalline CdO films suffer from grain boundary cracking under bending due to stress concentration, but single-crystal CdO membranes—without grain boundaries to concentrate stress—exhibit better flexibility and resistance to cracking. Furthermore, curvature-induced strain boosts the power factor by 12.8%, providing a curvature-controlled strain engineering strategy to optimize flexible thermoelectric performance. This work establishes freestanding CdO as a highly efficient and flexible thermoelectric material and suggests a fundamental strategy for designing robust smart materials for transparent, self-powered flexible electronics.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101153"},"PeriodicalIF":9.6,"publicationDate":"2025-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145784654","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-15DOI: 10.1016/j.jmat.2025.101151
Shuoyan Liu , Jiufeng Dong , Liang Sun , Zizhao Pan , Yujuan Niu , Yani Lu , Yuqi Liu , Hong Wang
Aromatic polyimide (PI) with high glass transition temperature (Tg) shows promise as a polymer dielectric for energy storage, but its rigid aromatic structure and electron delocalization cause significant conduction loss, degrading energy storage performance and breakdown strength (Eb) under high temperatures. Herein, we introduce a novel semi-alicyclic fluorinated polyimide (H-FPI) designed via a molecular engineering strategy that synergistically integrates bandgap and topological conformation modulation. Specifically, the alicyclic group elevates the lowest unoccupied molecular orbital (LUMO) while strong electron-withdrawing trifluoromethyl (CF3) substitution depresses the highest occupied molecular orbital (HOMO), creating a wide bandgap (4.2 eV). Concurrently, the chair-conformation alicyclic backbone and sterically bulky CF3 groups synergistically disrupt molecular planarity, reducing π-orbital overlap to suppress charge transfer while restricting chain mobility to yield a high Tg of 272 °C. Remarkably, H-FPI film delivers a high energy density of 6.02 J/cm3 with a superior breakdown strength of 626 MV/m at 200 °C, surpassing commercial PI and fluorinated polyimide (FPI) by 1261% and 55%, respectively. Furthermore, H-FPI film exhibits exceptional capacitor charge-discharge cyclability, enhanced mechanical robustness, and excellent thermal stability. This work establishes a new molecular design paradigm for organic capacitors in electrified transportation and smart grid systems requiring high-temperature working reliability.
{"title":"Semi-alicyclic fluorinated polyimide with ultrahigh energy density enabled by bandgap-topology co-engineering","authors":"Shuoyan Liu , Jiufeng Dong , Liang Sun , Zizhao Pan , Yujuan Niu , Yani Lu , Yuqi Liu , Hong Wang","doi":"10.1016/j.jmat.2025.101151","DOIUrl":"10.1016/j.jmat.2025.101151","url":null,"abstract":"<div><div>Aromatic polyimide (PI) with high glass transition temperature (<em>T</em><sub>g</sub>) shows promise as a polymer dielectric for energy storage, but its rigid aromatic structure and electron delocalization cause significant conduction loss, degrading energy storage performance and breakdown strength (<em>E</em><sub>b</sub>) under high temperatures. Herein, we introduce a novel semi-alicyclic fluorinated polyimide (H-FPI) designed <em>via</em> a molecular engineering strategy that synergistically integrates bandgap and topological conformation modulation. Specifically, the alicyclic group elevates the lowest unoccupied molecular orbital (LUMO) while strong electron-withdrawing trifluoromethyl (<img>CF<sub>3</sub>) substitution depresses the highest occupied molecular orbital (HOMO), creating a wide bandgap (4.2 eV). Concurrently, the chair-conformation alicyclic backbone and sterically bulky <img>CF<sub>3</sub> groups synergistically disrupt molecular planarity, reducing π-orbital overlap to suppress charge transfer while restricting chain mobility to yield a high <em>T</em><sub>g</sub> of 272 °C. Remarkably, H-FPI film delivers a high energy density of 6.02 J/cm<sup>3</sup> with a superior breakdown strength of 626 MV/m at 200 °C, surpassing commercial PI and fluorinated polyimide (FPI) by 1261% and 55%, respectively. Furthermore, H-FPI film exhibits exceptional capacitor charge-discharge cyclability, enhanced mechanical robustness, and excellent thermal stability. This work establishes a new molecular design paradigm for organic capacitors in electrified transportation and smart grid systems requiring high-temperature working reliability.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101151"},"PeriodicalIF":9.6,"publicationDate":"2025-12-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145760216","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-15DOI: 10.1016/j.jmat.2025.101154
Xuewen Jiang , Wei Wang , Aiwen Xie , Ziyi Tang , Ao Tian , Xin Gao , Xiaokuo Er , Liqiang Liu , Ruzhong Zuo
The development of high-performance lead-free energy storage capacitors is crucial for sustainable technologies, yet hindered in NaNbO3-based antiferroelectric (AFE) ceramics because of significant polarization hysteresis from field-induced AFE-ferroelectric (FE) phase transitions. This hysteresis fundamentally limits the simultaneous optimization of recoverable energy density (Wrec) and efficiency (η). Herein, we demonstrate that lamellar nanodomain engineering via compositional design in a (0.87–x)NaNbO3–0.13Bi0.5Na0.5TiO3–xBi(Mg0.5Ti0.5)O3 system effectively overcomes this bottleneck. The optimized composition (x = 0.05) delivers exceptional energy storage performance with a Wrec of ∼8.2 J/cm3, a η of ∼88.9%, and a power density of ∼207 MW/cm3. Analysis on multiscale structure evolution reveals that this compositional tuning induces a phase transformation from AFE P to AFE R symmetry, accompanied by an enhanced local structural disorder. Critically, the formation of lamellar AFE R-phase nanodomains with width ranging from 2 nm to 6 nm drives a quasi-linear polarization response with minimal hysteresis. Concurrently, the refined grain size improves the ceramic resistivity, substantially enhancing dielectric breakdown strength. These synergistic effects collectively yield outstanding energy storage properties, demonstrating that engineering lamellar AFE R-phase nanodomains is an efficient strategy to optimize overall energy storage performance of NaNbO3-based materials.
{"title":"Boosting energy storage in lead-free NaNbO3-based antiferroelectric ceramics through lamellar nanodomain engineering","authors":"Xuewen Jiang , Wei Wang , Aiwen Xie , Ziyi Tang , Ao Tian , Xin Gao , Xiaokuo Er , Liqiang Liu , Ruzhong Zuo","doi":"10.1016/j.jmat.2025.101154","DOIUrl":"10.1016/j.jmat.2025.101154","url":null,"abstract":"<div><div>The development of high-performance lead-free energy storage capacitors is crucial for sustainable technologies, yet hindered in NaNbO<sub>3</sub>-based antiferroelectric (AFE) ceramics because of significant polarization hysteresis from field-induced AFE-ferroelectric (FE) phase transitions. This hysteresis fundamentally limits the simultaneous optimization of recoverable energy density (<em>W</em><sub>rec</sub>) and efficiency (<em>η</em>). Herein, we demonstrate that lamellar nanodomain engineering <em>via</em> compositional design in a (0.87–<em>x</em>)NaNbO<sub>3</sub>–0.13Bi<sub>0.5</sub>Na<sub>0.5</sub>TiO<sub>3</sub>–<em>x</em>Bi(Mg<sub>0.5</sub>Ti<sub>0.5</sub>)O<sub>3</sub> system effectively overcomes this bottleneck. The optimized composition (<em>x</em> = 0.05) delivers exceptional energy storage performance with a <em>W</em><sub>rec</sub> of ∼8.2 J/cm<sup>3</sup>, a <em>η</em> of ∼88.9%, and a power density of ∼207 MW/cm<sup>3</sup>. Analysis on multiscale structure evolution reveals that this compositional tuning induces a phase transformation from AFE <em>P</em> to AFE <em>R</em> symmetry, accompanied by an enhanced local structural disorder. Critically, the formation of lamellar AFE <em>R</em>-phase nanodomains with width ranging from 2 nm to 6 nm drives a quasi-linear polarization response with minimal hysteresis. Concurrently, the refined grain size improves the ceramic resistivity, substantially enhancing dielectric breakdown strength. These synergistic effects collectively yield outstanding energy storage properties, demonstrating that engineering lamellar AFE <em>R</em>-phase nanodomains is an efficient strategy to optimize overall energy storage performance of NaNbO<sub>3</sub>-based materials.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101154"},"PeriodicalIF":9.6,"publicationDate":"2025-12-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145760357","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-15DOI: 10.1016/j.jmat.2025.101152
Zexia Zhang , Yi Jia , Qian Lv , Ruitao Lv , Feiyu Kang
Polymer/Si hybrid solar cells have attracted much research interest in virtue of their simple device structure and combination of flexibility and stability. Metal grid by thermal evaporation is usually used as the top electrode, which gives rise to a tradeoff between the efficient coverage and the decreased light absorption, in addition to the costly metal deposition in high vacuum. Carbon nanotube (CNT) networks possess both good conductivity and high light transmittance, thus is a promising candidate for the top electrode. Although it is significant to prepare and apply large-area and high-quality CNT films with high transparency and low sheet resistances into kinds of solar cells, CNTs have not been studied as transparent electrodes in polymer/Si hybrid solar cells to the best of our knowledge. In this work, large-area and continuous CNT networks with 86% transmittance at 550 nm are synthesized and used as transparent window electrodes in the hybrid heterojunction solar cells composed of a conjugate polymer poly(3,4-ethylenedioxy-thiophene):poly(styrenesulfonate) (PEDOT:PSS) and micro-textured n-type crystalline silicon wafers. Directly laminating the pristine CNT film onto the PEDOT:PSS/Si surface can lead to a power conversion efficiency (PCE) of 3.9%. After purification of CNT networks, the performance is improved up to 7.0%, due to the efficient carrier transportation and light harvesting of CNT electrodes. The results indicate that the flexible and transparent CNT networks have great potential for realizing metal grid-free hybrid polymer/Si solar cells.
{"title":"Carbon nanotube networks as efficient transparent electrode for polymer/silicon hybrid solar cells","authors":"Zexia Zhang , Yi Jia , Qian Lv , Ruitao Lv , Feiyu Kang","doi":"10.1016/j.jmat.2025.101152","DOIUrl":"10.1016/j.jmat.2025.101152","url":null,"abstract":"<div><div>Polymer/Si hybrid solar cells have attracted much research interest in virtue of their simple device structure and combination of flexibility and stability. Metal grid by thermal evaporation is usually used as the top electrode, which gives rise to a tradeoff between the efficient coverage and the decreased light absorption, in addition to the costly metal deposition in high vacuum. Carbon nanotube (CNT) networks possess both good conductivity and high light transmittance, thus is a promising candidate for the top electrode. Although it is significant to prepare and apply large-area and high-quality CNT films with high transparency and low sheet resistances into kinds of solar cells, CNTs have not been studied as transparent electrodes in polymer/Si hybrid solar cells to the best of our knowledge. In this work, large-area and continuous CNT networks with 86% transmittance at 550 nm are synthesized and used as transparent window electrodes in the hybrid heterojunction solar cells composed of a conjugate polymer poly(3,4-ethylenedioxy-thiophene):poly(styrenesulfonate) (PEDOT:PSS) and micro-textured n-type crystalline silicon wafers. Directly laminating the pristine CNT film onto the PEDOT:PSS/Si surface can lead to a power conversion efficiency (PCE) of 3.9%. After purification of CNT networks, the performance is improved up to 7.0%, due to the efficient carrier transportation and light harvesting of CNT electrodes. The results indicate that the flexible and transparent CNT networks have great potential for realizing metal grid-free hybrid polymer/Si solar cells.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101152"},"PeriodicalIF":9.6,"publicationDate":"2025-12-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145760356","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-10DOI: 10.1016/j.jmat.2025.101150
Qing Li , Wei Deng , Tian-Ci Ma , Changhao Zhao , Mupeng Zheng , Lei Zhao , Qiong Wu , Chaofeng Wu , Fang-Zhou Yao , Wen Gong , Dragan Damjanovic , Mao-Hua Zhang
Complex lead-based perovskites with the general formula Pb(Bx'B1-x")O3, represent an important class of antiferroelectrics beyond the prototypical PbZrO3 and NaNbO3. Depending on the combination of B-site species and the degree of cationic ordering, these materials exhibit a wide range of ferroic behaviors, spanning from antiferroelectric to (relaxor) ferroelectric responses. In this study, we investigate (Pb1-xBax)(Yb1/2Nb1/2)O3 polycrystals synthesized via a two-step processing route. Despite displaying antiferroelectric, ferroelectric, or nearly linear dielectric behavior at room temperature, all compositions exhibit double polarization hysteresis loops in proximity to a lower-temperature dielectric anomaly. This dielectric anomaly originates from the competition between antipolar and nanoscale polar regions, and shifts towards lower temperature with increasing Ba content, reflecting the suppression of long-range antiferroelectric ordering. Notably, a composition-invariant temperature scale, T∗, is identified and associated with the onset of static correlations among nanoscale polar entities, consistent with behavior reported in other complex Pb-based relaxor ferroelectrics. Superlattice reflections arising from antiparallel Pb2+ displacements persist above T∗, suggesting an intricate cation-ordering landscape requiring further investigation. These findings underscore the coexistence and competition of polar and antipolar instabilities in complex lead-based perovskites, and their pronounced sensitivity to chemical substitution, thermal fluctuations, and external electric fields.
{"title":"Temperature-dependent field-induced phase transition behavior in Pb(Yb1/2Nb1/2)O3-based antiferroelectrics","authors":"Qing Li , Wei Deng , Tian-Ci Ma , Changhao Zhao , Mupeng Zheng , Lei Zhao , Qiong Wu , Chaofeng Wu , Fang-Zhou Yao , Wen Gong , Dragan Damjanovic , Mao-Hua Zhang","doi":"10.1016/j.jmat.2025.101150","DOIUrl":"10.1016/j.jmat.2025.101150","url":null,"abstract":"<div><div>Complex lead-based perovskites with the general formula Pb(B<sub><em>x</em></sub>'B<sub>1-<em>x</em></sub>\")O<sub>3</sub>, represent an important class of antiferroelectrics beyond the prototypical PbZrO<sub>3</sub> and NaNbO<sub>3</sub>. Depending on the combination of B-site species and the degree of cationic ordering, these materials exhibit a wide range of ferroic behaviors, spanning from antiferroelectric to (relaxor) ferroelectric responses. In this study, we investigate (Pb<sub>1-<em>x</em></sub>Ba<sub><em>x</em></sub>)(Yb<sub>1/2</sub>Nb<sub>1/2</sub>)O<sub>3</sub> polycrystals synthesized <em>via</em> a two-step processing route. Despite displaying antiferroelectric, ferroelectric, or nearly linear dielectric behavior at room temperature, all compositions exhibit double polarization hysteresis loops in proximity to a lower-temperature dielectric anomaly. This dielectric anomaly originates from the competition between antipolar and nanoscale polar regions, and shifts towards lower temperature with increasing Ba content, reflecting the suppression of long-range antiferroelectric ordering. Notably, a composition-invariant temperature scale, <em>T</em>∗, is identified and associated with the onset of static correlations among nanoscale polar entities, consistent with behavior reported in other complex Pb-based relaxor ferroelectrics. Superlattice reflections arising from antiparallel Pb<sup>2+</sup> displacements persist above <em>T</em>∗, suggesting an intricate cation-ordering landscape requiring further investigation. These findings underscore the coexistence and competition of polar and antipolar instabilities in complex lead-based perovskites, and their pronounced sensitivity to chemical substitution, thermal fluctuations, and external electric fields.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 2","pages":"Article 101150"},"PeriodicalIF":9.6,"publicationDate":"2025-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728764","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
扫码关注我们
求助内容：
应助结果提醒方式：
京公网安备 11010802042870号