Pub Date : 2025-05-30DOI: 10.1016/j.jmat.2025.101089
Sitong Luo , Yujin Wang , Jingxuan Liang , Yuntian Jiang , Zhibo Wei , Yifan Du , Liang Lv , Shuqi Zheng , Weiyu Song
CuGaTe2 is p-type thermoelectric material with high thermoelectric potential. However, its performance is hindered by its intrinsic high resistivity and thermal conductivity. In this study, a synergistic strategy combining band engineering and chemical bonding modulation is employed to simultaneously optimize the electrical and thermal transport properties of CuGaTe2. First-principles calculations reveal that Cd preferentially occupy Ga sites, leading to bandgap narrowing and increasing density of states near Fermi level. Consequently, both carrier concentration and density-of-states effective mass are simultaneously optimized, ultimately power factor reaches 1359 μW·m−1·K−2. Phonon dispersion analysis reveals that Cd doping induces acoustic-optical phonon avoided crossing behavior, decelerating phonon velocity. Combined with the increase of Grüneisen parameter and weakened chemical bonding, which significantly enhances lattice anharmonicity, leading to effectively reduce in lattice thermal conductivity. Microstructural characterization further reveals that CdTe doping leads to the formation of three-dimensional defect network consisting of point defects, dislocations, and stacking faults enhances phonon scattering. Ultimately, lattice thermal conductivity of doped sample is reduced to 0.81 W·m−1·K−1. Consequently, (CuGaTe2)0.9975(2CdTe)0.0025 sample achieves enhanced zT of 1.05 at 823 K. This work provides insights into the synergistic effects of band engineering and chemical bonding modulation, offering pathway for the design of thermoelectric materials.
{"title":"Realizing high thermoelectric performance of CuGaTe2 via CdTe-doping-driven band engineering and chemical bond modulation","authors":"Sitong Luo , Yujin Wang , Jingxuan Liang , Yuntian Jiang , Zhibo Wei , Yifan Du , Liang Lv , Shuqi Zheng , Weiyu Song","doi":"10.1016/j.jmat.2025.101089","DOIUrl":"10.1016/j.jmat.2025.101089","url":null,"abstract":"<div><div>CuGaTe<sub>2</sub> is p-type thermoelectric material with high thermoelectric potential. However, its performance is hindered by its intrinsic high resistivity and thermal conductivity. In this study, a synergistic strategy combining band engineering and chemical bonding modulation is employed to simultaneously optimize the electrical and thermal transport properties of CuGaTe<sub>2</sub>. First-principles calculations reveal that Cd preferentially occupy Ga sites, leading to bandgap narrowing and increasing density of states near Fermi level. Consequently, both carrier concentration and density-of-states effective mass are simultaneously optimized, ultimately power factor reaches 1359 μW·m<sup>−1</sup>·K<sup>−2</sup>. Phonon dispersion analysis reveals that Cd doping induces acoustic-optical phonon avoided crossing behavior, decelerating phonon velocity. Combined with the increase of Grüneisen parameter and weakened chemical bonding, which significantly enhances lattice anharmonicity, leading to effectively reduce in lattice thermal conductivity. Microstructural characterization further reveals that CdTe doping leads to the formation of three-dimensional defect network consisting of point defects, dislocations, and stacking faults enhances phonon scattering. Ultimately, lattice thermal conductivity of doped sample is reduced to 0.81 W·m<sup>−1</sup>·K<sup>−1</sup>. Consequently, (CuGaTe<sub>2</sub>)<sub>0.9975</sub>(2CdTe)<sub>0.0025</sub> sample achieves enhanced <em>zT</em> of 1.05 at 823 K. This work provides insights into the synergistic effects of band engineering and chemical bonding modulation, offering pathway for the design of thermoelectric materials.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 6","pages":"Article 101089"},"PeriodicalIF":8.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144176969","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 : 2025-05-30DOI: 10.1016/j.jmat.2025.101090
Qi Zhao , Zhen Fan , Yi Wang , Qiulin Liu , Xuejuan Dong , Xiaowei Wu , Zhicheng Shan , Hangtian Zhu , Zhiliang Li , Shufang Wang , Huaizhou Zhao
High-strength high-performance p-type (Bi,Sb)2Te3 are of pivotal importance for near-room-temperature thermoelectric conversions, the reliable synthesis and fabrication has been viewed of imperative priority. It is known that the energy-favorable formation of anti-site SbTe’ and vacancy vSb''' acceptor defects from high-temperature syntheses results in additional charge carriers and scattering centers for electrical and phonon transport. However, how p-type (Bi,Sb)2Te3 with minimal lattice defects function remains to be scrutinized. Herein, we present the synergistic enhancements of mechanical robustness and thermoelectric property in crystallographic-defect-suppressed pristine (Bi,Sb)2Te3 through a simple mechanical alloying combined with spark-plasma-sintering (SPS) process. The SbTe’ and vSb''' acceptor defects were efficiently restrained, contributing to markedly increased charge carrier mobilities. A slightly enlarged band gap of 0.24 eV underpinned enhanced thermoelectric performance for pristine Bi0.3Sb1.7Te3 over a wide temperature range, delivering high zT300 K of 1.16 and zTave of 1.21 over 300–473 K. Interestingly, the confined in-situ grain coarsening during SPS with uniform dispersive nanopores readily endowed an ultra-high compressive strength of 206 MPa, surpassing that of reported (Bi,Sb)2Te3 so far. A 7-pair module (coupled with n-Bi2Te3) was fabricated, demonstrating a competitive ΔT over 70 K at Thot = 300 K. Furthermore, a power-generation module coupled with n-Mg3SbBi registered a cutting-edge thermoelectric conversion efficiency of 9.5% at a temperature gradient of 250 K. The strategy eliminates the need of complex processing nor extrinsic doping for pristine (Bi,Sb)2Te3, demonstrating great potentials in thermoelectric power generation and cooling applications.
{"title":"Atomic-defect-suppressed pristine p-type Bi0.3Sb1.7Te3 as robust high-performance thermoelectrics for power generation and cooling","authors":"Qi Zhao , Zhen Fan , Yi Wang , Qiulin Liu , Xuejuan Dong , Xiaowei Wu , Zhicheng Shan , Hangtian Zhu , Zhiliang Li , Shufang Wang , Huaizhou Zhao","doi":"10.1016/j.jmat.2025.101090","DOIUrl":"10.1016/j.jmat.2025.101090","url":null,"abstract":"<div><div>High-strength high-performance p-type (Bi,Sb)<sub>2</sub>Te<sub>3</sub> are of pivotal importance for near-room-temperature thermoelectric conversions, the reliable synthesis and fabrication has been viewed of imperative priority. It is known that the energy-favorable formation of anti-site Sb<sub>Te</sub><sup>’</sup> and vacancy v<sub>Sb</sub><sup>'''</sup> acceptor defects from high-temperature syntheses results in additional charge carriers and scattering centers for electrical and phonon transport. However, how p-type (Bi,Sb)<sub>2</sub>Te<sub>3</sub> with minimal lattice defects function remains to be scrutinized. Herein, we present the synergistic enhancements of mechanical robustness and thermoelectric property in crystallographic-defect-suppressed pristine (Bi,Sb)<sub>2</sub>Te<sub>3</sub> through a simple mechanical alloying combined with spark-plasma-sintering (SPS) process. The Sb<sub>Te</sub><sup>’</sup> and v<sub>Sb</sub><sup>'''</sup> acceptor defects were efficiently restrained, contributing to markedly increased charge carrier mobilities. A slightly enlarged band gap of 0.24 eV underpinned enhanced thermoelectric performance for pristine Bi<sub>0.3</sub>Sb<sub>1.7</sub>Te<sub>3</sub> over a wide temperature range, delivering high <em>zT</em><sub>300 K</sub> of 1.16 and <em>zT</em><sub>ave</sub> of 1.21 over 300–473 K. Interestingly, the confined <em>in-situ</em> grain coarsening during SPS with uniform dispersive nanopores readily endowed an ultra-high compressive strength of 206 MPa, surpassing that of reported (Bi,Sb)<sub>2</sub>Te<sub>3</sub> so far. A 7-pair module (coupled with n-Bi<sub>2</sub>Te<sub>3</sub>) was fabricated, demonstrating a competitive Δ<em>T</em> over 70 K at <em>T</em><sub>hot</sub> = 300 K. Furthermore, a power-generation module coupled with n-Mg<sub>3</sub>SbBi registered a cutting-edge thermoelectric conversion efficiency of 9.5% at a temperature gradient of 250 K. The strategy eliminates the need of complex processing nor extrinsic doping for pristine (Bi,Sb)<sub>2</sub>Te<sub>3</sub>, demonstrating great potentials in thermoelectric power generation and cooling applications.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 6","pages":"Article 101090"},"PeriodicalIF":8.4,"publicationDate":"2025-05-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144183760","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 : 2025-05-29DOI: 10.1016/j.jmat.2025.101091
Zhixing Wan , Shuo Wang , Yahao Mu , Ruihua Zhou , Hang Liu , Tingwu Jin , Di Wu , Jianlong Xia , Ce-Wen Nan
Organic cathode materials have garnered significant attention for their potential application in lithium-ion batteries due to their lightweight nature, tunable structures, high energy density, and environmental friendliness. However, the dissolution of organic cathodes in liquid electrolytes often leads to poor cycling stability, which limits their practical application. In this study, a composite cathode was prepared by ball milling the PTCDA/CuS (perylene-3,4,9,10-tetracarboxylic dianhydride, PTCDA) with a sulfide-based electrolyte and carbon nanotubes. By optimizing the component ratios, the assembled all-solid-state batteries (ASSBs) show a high discharge capacity of 210 mA⸱h/g after 200 cycles without any capacity degradation at a current density of 33.0 mA/g. Through comprehensive characterization techniques including X-ray diffraction (XRD), Raman spectroscopy, Fourier-transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS), the coordination of Cu2+ and the formation of sulfur-linked polymers during the charge-discharge processes are elucidated, and the reversibility of the electrochemical reactions has been confirmed. This work highlights the excellent compatibility between organic cathodes and sulfide-based electrolytes, providing a new way for the development of high-performance ASSBs with high energy density and extended lifespan.
{"title":"PTCDA/CuS cathode enabling stable sulfide-based all-solid-state batteries","authors":"Zhixing Wan , Shuo Wang , Yahao Mu , Ruihua Zhou , Hang Liu , Tingwu Jin , Di Wu , Jianlong Xia , Ce-Wen Nan","doi":"10.1016/j.jmat.2025.101091","DOIUrl":"10.1016/j.jmat.2025.101091","url":null,"abstract":"<div><div>Organic cathode materials have garnered significant attention for their potential application in lithium-ion batteries due to their lightweight nature, tunable structures, high energy density, and environmental friendliness. However, the dissolution of organic cathodes in liquid electrolytes often leads to poor cycling stability, which limits their practical application. In this study, a composite cathode was prepared by ball milling the PTCDA/CuS (perylene-3,4,9,10-tetracarboxylic dianhydride, PTCDA) with a sulfide-based electrolyte and carbon nanotubes. By optimizing the component ratios, the assembled all-solid-state batteries (ASSBs) show a high discharge capacity of 210 mA⸱h/g after 200 cycles without any capacity degradation at a current density of 33.0 mA/g. Through comprehensive characterization techniques including X-ray diffraction (XRD), Raman spectroscopy, Fourier-transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS), the coordination of Cu<sup>2+</sup> and the formation of sulfur-linked polymers during the charge-discharge processes are elucidated, and the reversibility of the electrochemical reactions has been confirmed. This work highlights the excellent compatibility between organic cathodes and sulfide-based electrolytes, providing a new way for the development of high-performance ASSBs with high energy density and extended lifespan.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"12 1","pages":"Article 101091"},"PeriodicalIF":9.6,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144176964","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 : 2025-05-24DOI: 10.1016/j.jmat.2025.101077
Cangjin Li, Manwen Yao, Xi Yao, Chunyu Li
For multilayer ceramic capacitors, co-sintering of ceramics with inner electrodes is a crucial issue. This requires ceramic materials to have a low sintering temperature. In response to this criterion, a hybrid processing technology is proposed in this study. This technology involves mixing of calcined ceramic powders with sol solutions to obtain composite powders. Eventually, sintering temperature of the obtained composite material is reduced from 1300 °C to 1120 °C. This is originated from the introduction of more specific surface areas and more oxygen vacancies by sol solutions, leading to an enhancement of chemical reaction activity. The ceramic powders and the sol solutions used in this work are (Pb0.94La0.04)(Zr0.51Sn0.47Hf0.01Ti0.01)O3 and (Pb0.97La0.02)(Zr0.6Sn0.4)O3, respectively. Such composition design helps improve the dielectric constant and polarization intensity. While in the meantime, because of the strong interfacial resistance caused by sol solutions, interfacial insulation as well as electrical breakdown strength can be significantly improved. Consequently, a high energy storage density up to 12.4 J/cm3 and an efficiency of 92.4% is obtained in this work. Overall, this technology is applicable to a wide range of ceramic material systems, and provides an innovative design and manufacture of ceramics.
{"title":"A hybrid processing technology for fabricating lead zirconate-based ceramics with high energy storage density, high efficiency, and low sintering temperature","authors":"Cangjin Li, Manwen Yao, Xi Yao, Chunyu Li","doi":"10.1016/j.jmat.2025.101077","DOIUrl":"10.1016/j.jmat.2025.101077","url":null,"abstract":"<div><div>For multilayer ceramic capacitors, co-sintering of ceramics with inner electrodes is a crucial issue. This requires ceramic materials to have a low sintering temperature. In response to this criterion, a hybrid processing technology is proposed in this study. This technology involves mixing of calcined ceramic powders with sol solutions to obtain composite powders. Eventually, sintering temperature of the obtained composite material is reduced from 1300 °C to 1120 °C. This is originated from the introduction of more specific surface areas and more oxygen vacancies by sol solutions, leading to an enhancement of chemical reaction activity. The ceramic powders and the sol solutions used in this work are (Pb<sub>0.94</sub>La<sub>0.04</sub>)(Zr<sub>0.51</sub>Sn<sub>0.47</sub>Hf<sub>0.01</sub>Ti<sub>0.01</sub>)O<sub>3</sub> and (Pb<sub>0.97</sub>La<sub>0.02</sub>)(Zr<sub>0.6</sub>Sn<sub>0.4</sub>)O<sub>3</sub>, respectively. Such composition design helps improve the dielectric constant and polarization intensity. While in the meantime, because of the strong interfacial resistance caused by sol solutions, interfacial insulation as well as electrical breakdown strength can be significantly improved. Consequently, a high energy storage density up to 12.4 J/cm<sup>3</sup> and an efficiency of 92.4% is obtained in this work. Overall, this technology is applicable to a wide range of ceramic material systems, and provides an innovative design and manufacture of ceramics.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 6","pages":"Article 101077"},"PeriodicalIF":8.4,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144130452","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}
In this study, the inequivalent substitution of Ca2+ by Li+ in the Ca3Co2SiV2O12 compound was designed to modulate its sintering characteristics and microwave dielectric properties. The corresponding Ca3–xLi2xCo2SiV2O12 (CCSV-xLi, 0.01≤ x ≤ 0.07) ceramics were prepared via the conventional solid-state phase method, which could be densely sintered at a temperature below 1140 °C. Rietveld refinement results suggested that all the doped Li occupied the Ca-site as x ≤ 0.05 while superfluous Li positioned at the Co-site of CCSV when x = 0.07. This atomic occupancy had a remarkable effect on the degree of “rattling effect” and thus modulated the relative permittivity of ceramics, constantly increasing at x = 0.01–0.05 and slightly decreasing at x = 0.07. Raman spectra revealed that Q×f value was closely related to Raman shift and FWHM. Also, the Q×f value was partly influenced by oxygen vacancy concentration. The τf demonstrated an opposite tendency to the bond valence of the A-site and was affected by the “rattling effect”. The CCSV-0.05Li ceramic sintered at 1120 °C possessed excellent microwave dielectric properties: εr = 12.17, Q×f = 56,220 GHz, and τf = −8.5 × 10−6 °C−1.
{"title":"Modulation in sintering characteristics and microwave dielectric properties of Ca3Co2SiV2O12 via Li+ inequivalent substitution","authors":"Zhenli Tao, Jiamao Li, Junxian Wang, Yuxuan Ren, Yunfeng Guo, Qinghe Yang, Zhihao Yuan, Rui Tian, Wenbo Wang","doi":"10.1016/j.jmat.2025.101074","DOIUrl":"10.1016/j.jmat.2025.101074","url":null,"abstract":"<div><div>In this study, the inequivalent substitution of Ca<sup>2+</sup> by Li<sup>+</sup> in the Ca<sub>3</sub>Co<sub>2</sub>SiV<sub>2</sub>O<sub>12</sub> compound was designed to modulate its sintering characteristics and microwave dielectric properties. The corresponding Ca<sub>3–<em>x</em></sub>Li<sub>2<em>x</em></sub>Co<sub>2</sub>SiV<sub>2</sub>O<sub>12</sub> (CCSV-<em>x</em>Li, 0.01≤ <em>x</em> ≤ 0.07) ceramics were prepared <em>via</em> the conventional solid-state phase method, which could be densely sintered at a temperature below 1140 °C. Rietveld refinement results suggested that all the doped Li occupied the Ca-site as <em>x</em> ≤ 0.05 while superfluous Li positioned at the Co-site of CCSV when <em>x</em> = 0.07. This atomic occupancy had a remarkable effect on the degree of “rattling effect” and thus modulated the relative permittivity of ceramics, constantly increasing at <em>x</em> = 0.01–0.05 and slightly decreasing at <em>x</em> = 0.07. Raman spectra revealed that <em>Q</em>×<em>f</em> value was closely related to Raman shift and FWHM. Also, the <em>Q</em>×<em>f</em> value was partly influenced by oxygen vacancy concentration. The <em>τ</em><sub>f</sub> demonstrated an opposite tendency to the bond valence of the A-site and was affected by the “rattling effect”. The CCSV-0.05Li ceramic sintered at 1120 °C possessed excellent microwave dielectric properties: <em>ε</em><sub>r</sub> = 12.17, <em>Q</em>×<em>f</em> = 56,220 GHz, and <em>τ</em><sub>f</sub> = −8.5 × 10<sup>−6</sup> °C<sup>−1</sup>.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 6","pages":"Article 101074"},"PeriodicalIF":8.4,"publicationDate":"2025-05-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933325","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 : 2025-05-10DOI: 10.1016/j.jmat.2025.101076
Peng Yan , Mingming Si , Yongping Liu, Yu Ren, Jie Min, Xu Wang, Qi Ding, Weizhong Jiang, Yuchi Fan, Wan Jiang
Cold-sintered ceramics typically exhibit inferior mechanical properties compared to high-temperature sintered counterparts. We demonstrate that introducing large internal stress through highly concentrated nanodiamonds (NDs) significantly enhances cold-sintered α-quartz composites to structural ceramic levels. At 500 MPa cold-sintering pressure, uniformly dispersed NDs generate 1.2 GPa local prestress via Young's modulus difference, while pressure-modulated internal stress is evidenced by dielectric property changes. The optimized composite achieves fracture toughness of (3.65 ± 0.21) MPa·m1/2 (180% increase) and Vickers hardness of 10.6 GPa (80% increase), matching some high-temperature-sintered ceramics. Toughening arises from prestress-driven crack deflection and crack tip bridging, while hardness enhancement stems from NDs' rigid constraint and high-pressure-induced dislocations in silica matrix. Compressive strength increases by 90% and fatigue life exceeds 1000 cycles, attributed to internal stress-strengthened grain boundaries and improved toughness. This work presents a transformative strategy for developing damage-resistant ceramics, meriting further exploration of scalability and engineering applications.
{"title":"Hard, strong, and tough cold-sintered α-quartz composites as high-performance structural ceramics","authors":"Peng Yan , Mingming Si , Yongping Liu, Yu Ren, Jie Min, Xu Wang, Qi Ding, Weizhong Jiang, Yuchi Fan, Wan Jiang","doi":"10.1016/j.jmat.2025.101076","DOIUrl":"10.1016/j.jmat.2025.101076","url":null,"abstract":"<div><div>Cold-sintered ceramics typically exhibit inferior mechanical properties compared to high-temperature sintered counterparts. We demonstrate that introducing large internal stress through highly concentrated nanodiamonds (NDs) significantly enhances cold-sintered α-quartz composites to structural ceramic levels. At 500 MPa cold-sintering pressure, uniformly dispersed NDs generate 1.2 GPa local prestress <em>via</em> Young's modulus difference, while pressure-modulated internal stress is evidenced by dielectric property changes. The optimized composite achieves fracture toughness of (3.65 ± 0.21) MPa·m<sup>1</sup>/<sup>2</sup> (180% increase) and Vickers hardness of 10.6 GPa (80% increase), matching some high-temperature-sintered ceramics. Toughening arises from prestress-driven crack deflection and crack tip bridging, while hardness enhancement stems from NDs' rigid constraint and high-pressure-induced dislocations in silica matrix. Compressive strength increases by 90% and fatigue life exceeds 1000 cycles, attributed to internal stress-strengthened grain boundaries and improved toughness. This work presents a transformative strategy for developing damage-resistant ceramics, meriting further exploration of scalability and engineering applications.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 6","pages":"Article 101076"},"PeriodicalIF":8.4,"publicationDate":"2025-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143930994","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 : 2025-05-09DOI: 10.1016/j.jmat.2025.101075
Qijun Yang , Siwei Dai , Changfan Ju , Keyu Bao , Binjian Zeng , Shuaizhi Zheng , Jiajia Liao , Jiangang Guo , Sirui Zhang , Yichun Zhou , Min Liao
High-scalability HfO2-based ferroelectric thin films are promising for application in fast, energy-efficient, and high-density non-volatile memories. This ferroelectricity is believed to originate from the metastable orthorhombic phase, which is difficult to obtain. Post-metallization annealing with a top electrode capping layer is a useful method for stabilizing the ferroelectric orthorhombic phase. However, direct physical evidence of the top electrode role is lacking. In this study, we visualized the dynamic process of the phase transition in Hf0.5Zr0.5O2 (HZO) thin films with TiN and Pt top electrodes during the heating and cooling processes through in-situ scanning transmission electron microscopy (STEM). The TiN top electrode stabilized the orthorhombic phase, whereas the Pt top electrode induced a phase transition to the monoclinic phase. Subsequently, we elucidated the phase transition mechanism in HZO thin films using the kinetic effect and revealed that it was related to the concentration of oxygen vacancies induced by the top electrode. This study provides valuable insights into the stabilization of the orthorhombic phase in HfO2-based ferroelectric thin films and contributes to the elucidation of the phase transition mechanism of HfO2-based ferroelectric thin films.
{"title":"Direct observation of phase transition in Hf0.5Zr0.5O2 thin films affected by top electrodes using in-situ STEM heating","authors":"Qijun Yang , Siwei Dai , Changfan Ju , Keyu Bao , Binjian Zeng , Shuaizhi Zheng , Jiajia Liao , Jiangang Guo , Sirui Zhang , Yichun Zhou , Min Liao","doi":"10.1016/j.jmat.2025.101075","DOIUrl":"10.1016/j.jmat.2025.101075","url":null,"abstract":"<div><div>High-scalability HfO<sub>2</sub>-based ferroelectric thin films are promising for application in fast, energy-efficient, and high-density non-volatile memories. This ferroelectricity is believed to originate from the metastable orthorhombic phase, which is difficult to obtain. Post-metallization annealing with a top electrode capping layer is a useful method for stabilizing the ferroelectric orthorhombic phase. However, direct physical evidence of the top electrode role is lacking. In this study, we visualized the dynamic process of the phase transition in Hf<sub>0.5</sub>Zr<sub>0.5</sub>O<sub>2</sub> (HZO) thin films with TiN and Pt top electrodes during the heating and cooling processes through <em>in-situ</em> scanning transmission electron microscopy (STEM). The TiN top electrode stabilized the orthorhombic phase, whereas the Pt top electrode induced a phase transition to the monoclinic phase. Subsequently, we elucidated the phase transition mechanism in HZO thin films using the kinetic effect and revealed that it was related to the concentration of oxygen vacancies induced by the top electrode. This study provides valuable insights into the stabilization of the orthorhombic phase in HfO<sub>2</sub>-based ferroelectric thin films and contributes to the elucidation of the phase transition mechanism of HfO<sub>2</sub>-based ferroelectric thin films.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 5","pages":"Article 101075"},"PeriodicalIF":8.4,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143926349","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 : 2025-05-09DOI: 10.1016/j.jmat.2025.101069
Zhan Zeng , Jin Cheng , Xinwei Xu , Hongye Wang , Yani Lu , Liang Sun , Naichao Chen , Xiaoyu Li , Boshen Zhang , Hong Wang
As electronic devices become increasingly miniaturized and demand greater integration, traditional packaging technologies face substantial challenges in meeting the needs for high-frequency performance and system reliability. Ceramic materials, known for their excellent dielectric properties and thermal stability, are promising candidates for advanced packaging applications. However, conventional high-temperature densification processes, which often exceed 1000 °C, restrict their compatibility with temperature-sensitive components in modern electronic systems. To overcome this limitation, we propose a novel approach to densify Al2O3H3BO3 ceramic at room temperature under low uniaxial stress. It is found that a H3BO3 facilitates plastic deformation in the medium of deionized water, enhancing the densification of Al2O3H3BO3 ceramics even at minimal uniaxial stress. The resulting material exhibits a high relative density of over 96% and possesses excellent microwave dielectric properties (relative permittivity : 2.84–5.37; values: 12,924–69,000 GHz; resonant frequency values: −156.94 10−6 °C−1 to −73.42 10−6 °C−1) and thermal conductivity ( values: 1.96–5.96 W·m−1·K−1). After co-firing with a silicon wafer, the ceramic maintains its structural integrity, with no observable atomic diffusion at the ceramic-silicon interface, rendering it a potential candidate for advanced packaging and integration technologies.
{"title":"Room-temperature densified Al2O3-H3BO3 ceramics with excellent microwave dielectric properties and thermal conductivity for chip packaging","authors":"Zhan Zeng , Jin Cheng , Xinwei Xu , Hongye Wang , Yani Lu , Liang Sun , Naichao Chen , Xiaoyu Li , Boshen Zhang , Hong Wang","doi":"10.1016/j.jmat.2025.101069","DOIUrl":"10.1016/j.jmat.2025.101069","url":null,"abstract":"<div><div>As electronic devices become increasingly miniaturized and demand greater integration, traditional packaging technologies face substantial challenges in meeting the needs for high-frequency performance and system reliability. Ceramic materials, known for their excellent dielectric properties and thermal stability, are promising candidates for advanced packaging applications. However, conventional high-temperature densification processes, which often exceed 1000 °C, restrict their compatibility with temperature-sensitive components in modern electronic systems. To overcome this limitation, we propose a novel approach to densify Al<sub>2</sub>O<sub>3</sub><img>H<sub>3</sub>BO<sub>3</sub> ceramic at room temperature under low uniaxial stress. It is found that a H<sub>3</sub>BO<sub>3</sub> facilitates plastic deformation in the medium of deionized water, enhancing the densification of Al<sub>2</sub>O<sub>3</sub><img>H<sub>3</sub>BO<sub>3</sub> ceramics even at minimal uniaxial stress. The resulting material exhibits a high relative density of over 96% and possesses excellent microwave dielectric properties (relative permittivity <span><math><msub><mi>ε</mi><mi>r</mi></msub></math></span>: 2.84–5.37; <span><math><mrow><mi>Q</mi><mo>×</mo><mi>f</mi></mrow></math></span> values: 12,924–69,000 GHz; resonant frequency <span><math><msub><mi>τ</mi><mi>f</mi></msub></math></span> values: −156.94 10<sup>−6</sup> °C<sup>−1</sup> to −73.42 10<sup>−6</sup> °C<sup>−1</sup>) and thermal conductivity (<span><math><mrow><mi>λ</mi></mrow></math></span> values: 1.96–5.96 W·m<sup>−1</sup>·K<sup>−1</sup>). After co-firing with a silicon wafer, the ceramic maintains its structural integrity, with no observable atomic diffusion at the ceramic-silicon interface, rendering it a potential candidate for advanced packaging and integration technologies.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 6","pages":"Article 101069"},"PeriodicalIF":8.4,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143926348","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}
Massive energy is consumed to cool buildings for comfortable life in hot climates due to indoor air-conditioning, which necessitates the passive daytime radiative cooling of buildings. Given the high ambient temperature, it is essential to increase the thermal resistance of building walls through paints and enhance their durability to dust and aerosol contamination. In this work, a multifunctional composite paint, mainly consisting of inorganic pigments and mesoporous silica aerogel (SA), is proposed for passive radiative cooling, low thermal conductivity, and surface self-cleaning. In comparison with ordinary paint, the SA microparticles-infused composite paint can enhance the reflectance (ρVIS-NIR) to the solar irradiance by up to 15% in the visible and near-infrared ranges (0.3–2.5 μm). It also maintains the radiative cooling property with about 0.96 emissivity (εLWIR) in the atmospheric transparency windows (8–13 μm) for thermal radiation to dissipate into the cold outer space. Even after long-term outdoor exposure to harsh environmental conditions, SA-infused white paint can still maintain its spectral and wetting properties, achieving daytime cooling with 7.4 °C lower than the ambient temperature. Moreover, the SA infusion enables the paint to reduce the thermal conductivity by 50% and provide much better thermal insulation, while SA renders the paint surface hydrophobic and self-cleaning.
{"title":"Multifunctional silica aerogel-infused paint for self-cleaning and radiative cooling","authors":"Adil Al-Mahdouri , Aikifa Raza , Abdulrahman Al-Hashmi , Youbo Zhao , Krishna Mohan , Khalid Askar , TieJun Zhang","doi":"10.1016/j.jmat.2025.101070","DOIUrl":"10.1016/j.jmat.2025.101070","url":null,"abstract":"<div><div>Massive energy is consumed to cool buildings for comfortable life in hot climates due to indoor air-conditioning, which necessitates the passive daytime radiative cooling of buildings. Given the high ambient temperature, it is essential to increase the thermal resistance of building walls through paints and enhance their durability to dust and aerosol contamination. In this work, a multifunctional composite paint, mainly consisting of inorganic pigments and mesoporous silica aerogel (SA), is proposed for passive radiative cooling, low thermal conductivity, and surface self-cleaning. In comparison with ordinary paint, the SA microparticles-infused composite paint can enhance the reflectance (<em>ρ</em><sub>VIS-NIR</sub>) to the solar irradiance by up to 15% in the visible and near-infrared ranges (0.3–2.5 μm). It also maintains the radiative cooling property with about 0.96 emissivity (<em>ε</em><sub>LWIR</sub>) in the atmospheric transparency windows (8–13 μm) for thermal radiation to dissipate into the cold outer space. Even after long-term outdoor exposure to harsh environmental conditions, SA-infused white paint can still maintain its spectral and wetting properties, achieving daytime cooling with 7.4 °C lower than the ambient temperature. Moreover, the SA infusion enables the paint to reduce the thermal conductivity by 50% and provide much better thermal insulation, while SA renders the paint surface hydrophobic and self-cleaning.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 6","pages":"Article 101070"},"PeriodicalIF":8.4,"publicationDate":"2025-05-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143901374","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 : 2025-05-02DOI: 10.1016/j.jmat.2025.101071
Kui Xue , Min Xing , Tiantian Chen , Bingyun Xi , Haifeng Zhang , Kuicai Ye , Jiayin Feng , Wenhao Qian , Jiajun Qiu , Xuanyong Liu
For alveolar bone defects, magnesium membrane with the mechanical properties of shielding fibrocyte growth and sustainable release of Mg2+ is an excellent choice for guide bone regeneration (GBR) surgery. However, insufficient osteogenesis and bacterial infection have hindered its application. In this study, MgGa-LDH coating was successfully prepared, which delayed the degradation rate of the Mg membranes and greatly reduced the amount of hydrogen evolution. A weakly alkaline microenvironment (pH = 8.5) containing appropriate concentrations of Mg2+ and Ga3+ was successfully constructed, effectively promoting the adhesion and proliferation of MC3T3-E1 cells. It also upregulated the expression of alkaline phosphatase and collagen, which were conducive to the formation of mineralized nodules, and promoted the osteogenic differentiation of rat bone marrow mesenchymal stem cells in vitro. In addition, Ga3+ released from the coating and the generated alkaline microenvironment showed good antibacterial properties against S. aureus and E. coli. The MgGa-LDH coating can effectively reduce the degradation rate of Mg membranes and mitigate inflammation. The MgGa-LDH coating modified Mg membrane promoted new bone formation in cranial defect animal models. This bone-promoting Mg2+ and Ga3+ releasing platform and weak alkaline microenvironment creation system paves the way for the application of Mg membranes in the field of GBR.
对于牙槽骨缺损，具有屏蔽纤维细胞生长和Mg2+持续释放的力学性能的镁膜是引导骨再生（GBR）手术的理想选择。然而，成骨不足和细菌感染阻碍了其应用。本研究成功制备了Mg- ga - ldh涂层，延缓了Mg膜的降解速度，大大降低了析氢量。成功构建了适宜浓度Mg2+和Ga3+的弱碱性微环境（pH =8.5），可有效促进MC3T3-E1细胞的粘附和增殖。上调碱性磷酸酶和胶原蛋白的表达，有利于矿化结节的形成，促进体外培养大鼠骨髓间充质干细胞成骨分化。此外，涂层释放的Ga3+和生成的碱性微环境对金黄色葡萄球菌具有良好的抗菌性能。Mg- ga - ldh涂层可以有效降低Mg膜的降解率，减轻炎症反应。Mg- ga - ldh涂层修饰Mg膜促进颅骨缺损动物模型新骨形成。该促骨Mg2+和Ga3+释放平台和弱碱性微环境创建系统为Mg膜在GBR领域的应用铺平了道路。
{"title":"MgGa layered double hydroxides coating endow magnesium with antibacterial and osteogenic properties for guided-bone regeneration application","authors":"Kui Xue , Min Xing , Tiantian Chen , Bingyun Xi , Haifeng Zhang , Kuicai Ye , Jiayin Feng , Wenhao Qian , Jiajun Qiu , Xuanyong Liu","doi":"10.1016/j.jmat.2025.101071","DOIUrl":"10.1016/j.jmat.2025.101071","url":null,"abstract":"<div><div>For alveolar bone defects, magnesium membrane with the mechanical properties of shielding fibrocyte growth and sustainable release of Mg<sup>2+</sup> is an excellent choice for guide bone regeneration (GBR) surgery. However, insufficient osteogenesis and bacterial infection have hindered its application. In this study, Mg<img>Ga-LDH coating was successfully prepared, which delayed the degradation rate of the Mg membranes and greatly reduced the amount of hydrogen evolution. A weakly alkaline microenvironment (pH = 8.5) containing appropriate concentrations of Mg<sup>2+</sup> and Ga<sup>3+</sup> was successfully constructed, effectively promoting the adhesion and proliferation of MC3T3-E1 cells. It also upregulated the expression of alkaline phosphatase and collagen, which were conducive to the formation of mineralized nodules, and promoted the osteogenic differentiation of rat bone marrow mesenchymal stem cells <em>in vitro</em>. In addition, Ga<sup>3+</sup> released from the coating and the generated alkaline microenvironment showed good antibacterial properties against <em>S. aureus</em> and <em>E. coli</em>. The Mg<img>Ga-LDH coating can effectively reduce the degradation rate of Mg membranes and mitigate inflammation. The Mg<img>Ga-LDH coating modified Mg membrane promoted new bone formation in cranial defect animal models. This bone-promoting Mg<sup>2+</sup> and Ga<sup>3+</sup> releasing platform and weak alkaline microenvironment creation system paves the way for the application of Mg membranes in the field of GBR.</div></div>","PeriodicalId":16173,"journal":{"name":"Journal of Materiomics","volume":"11 6","pages":"Article 101071"},"PeriodicalIF":8.4,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897620","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}
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