Li1.3Al0.3Ti1.7(PO4)3 (LATP) is a promising solid-state electrolyte for next-generation solid-state lithium metal batteries, offering high ionic conductivity, superior air stability, and low cost. However, its practical application is hindered by high interface impedance due to rigid solid–solid contact with electrodes and instability when in contact with lithium metal. Here, a hybrid solid–liquid electrolyte is designed, consisting of a porous 3D LATP skeleton infiltrated with carbonate-based organic electrolyte, to ensure sufficient electrolyte wettability. Further, the thermodynamic instability between LATP and Li is solved by magnetron sputtering a layer of ferroelectric Ba0.5Sr0.5TiO3 (BST) onto the LATP surface. This BST interlayer prevents direct contact between LATP and Li metal, enhancing performance by dynamically regulating Li+ deposition, inhibiting dendrite growth, reducing overpotential and interface resistance, and improving Li+ transport. Compared to the LATP-based electrolyte (LATP-LE), the BST-modified hybrid electrolyte (B@LATP-LE) demonstrates largely improved ionic conductivity (0.42 to 1.38 mS cm−1) and outstanding electrochemical performance, achieving stable cycling for over 7000 h in Li||Li cells and superior stability in LiFePO4||Li and LiNi0.8Co0.1Mn0.1O2||Li full cells. This approach offers a cost-effective solution to the interface issues of LATP and provides insights for high-performance lithium metal batteries.
Li1.3Al0.3Ti1.7(PO4)3 (LATP)是一种很有前途的固态电解质,用于下一代固态锂金属电池,具有高离子电导率,优越的空气稳定性和低成本。然而,由于与电极的刚性固-固接触以及与锂金属接触时的不稳定性,其界面阻抗高,阻碍了其实际应用。本文设计了一种混合固液电解质,由多孔的3D LATP骨架渗透碳酸盐基有机电解质组成,以确保足够的电解质润湿性。此外,通过磁控溅射一层铁电Ba0.5Sr0.5TiO3 (BST)到LATP表面,解决了LATP与Li之间的热力学不稳定性。该BST中间层防止了LATP与Li金属的直接接触,通过动态调节Li+沉积、抑制枝晶生长、降低过电位和界面电阻以及改善Li+输运来提高性能。与基于latp的电解质(LATP-LE)相比,bst修饰的混合电解质(B@LATP-LE)的离子电导率大幅提高(0.42至1.38 mS cm−1),电化学性能优异,在Li||锂电池中可稳定循环超过7000 h,在LiFePO4||Li和LiNi0.8Co0.1Mn0.1O2||Li全电池中具有优异的稳定性。这种方法为LATP的接口问题提供了一种经济有效的解决方案,并为高性能锂金属电池提供了见解。
{"title":"A Ba0.5Sr0.5TiO3 Interlayer Enabling Ultra-Stable Performance in Hybrid Solid–Liquid Lithium Metal Batteries","authors":"Zhen Chen, Yang Wang, Kepin Zhu, Ziqi Zhao, Xian-Ao Li, Yixin Wu, Xinwei Dou, Minghua Chen, Chuying Ouyang","doi":"10.1002/eem2.70018","DOIUrl":"https://doi.org/10.1002/eem2.70018","url":null,"abstract":"<p>Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> (LATP) is a promising solid-state electrolyte for next-generation solid-state lithium metal batteries, offering high ionic conductivity, superior air stability, and low cost. However, its practical application is hindered by high interface impedance due to rigid solid–solid contact with electrodes and instability when in contact with lithium metal. Here, a hybrid solid–liquid electrolyte is designed, consisting of a porous 3D LATP skeleton infiltrated with carbonate-based organic electrolyte, to ensure sufficient electrolyte wettability. Further, the thermodynamic instability between LATP and Li is solved by magnetron sputtering a layer of ferroelectric Ba<sub>0.5</sub>Sr<sub>0.5</sub>TiO<sub>3</sub> (BST) onto the LATP surface. This BST interlayer prevents direct contact between LATP and Li metal, enhancing performance by dynamically regulating Li<sup>+</sup> deposition, inhibiting dendrite growth, reducing overpotential and interface resistance, and improving Li<sup>+</sup> transport. Compared to the LATP-based electrolyte (LATP-LE), the BST-modified hybrid electrolyte (B@LATP-LE) demonstrates largely improved ionic conductivity (0.42 to 1.38 mS cm<sup>−1</sup>) and outstanding electrochemical performance, achieving stable cycling for over 7000 h in Li||Li cells and superior stability in LiFePO<sub>4</sub>||Li and LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub>||Li full cells. This approach offers a cost-effective solution to the interface issues of LATP and provides insights for high-performance lithium metal batteries.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70018","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144773948","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Exploring multiple-level encryption technologies and extra safety decoding ways to prevent information leakage is of great significance and interest, but is still challenging. Herein, we propose a novel approach by developing halloysite-based X-ray-activated persistent luminescent hydrogels with self-healing properties, which can emit visible luminescence even after switching off the X-ray irradiation. The afterglow properties can be well regulated by controlling the crystal form of the anchored nanocrystal on the surface of the halloysite nanotube, enabling the “time-lock” encryption. Additionally, the absence or presence of photoluminescence behaviors can also be controlled by changing the crosslinkers in synthesizing hydrogels. Six types of hydrogels were reported by means of condensation reactions, which show diverse emission and afterglow properties. By taking advantage of these features, the hydrogels were programmed as a display panel that exhibits three types of fake information under the wrong decoding tools. Only when the right stimuli are applied at the defined time does the panel give a readable pattern, allowing the encrypted information to be recognized. We believe this work will pave a novel path in developing extra safety information-encryption materials.
{"title":"Halloysite-Based X-Ray-Activated Persistent Luminescent Hydrogels Enable Multiple-Level Encryption and Dual-Locked Camouflage","authors":"Huabiao Chen, Weihua Song, Bo Zhang, Zetong Zhang, Yanmin Yang, Libin Bai, Yonggang Wu, Hailei Zhang","doi":"10.1002/eem2.70034","DOIUrl":"https://doi.org/10.1002/eem2.70034","url":null,"abstract":"<p>Exploring multiple-level encryption technologies and extra safety decoding ways to prevent information leakage is of great significance and interest, but is still challenging. Herein, we propose a novel approach by developing halloysite-based X-ray-activated persistent luminescent hydrogels with self-healing properties, which can emit visible luminescence even after switching off the X-ray irradiation. The afterglow properties can be well regulated by controlling the crystal form of the anchored nanocrystal on the surface of the halloysite nanotube, enabling the “time-lock” encryption. Additionally, the absence or presence of photoluminescence behaviors can also be controlled by changing the crosslinkers in synthesizing hydrogels. Six types of hydrogels were reported by means of condensation reactions, which show diverse emission and afterglow properties. By taking advantage of these features, the hydrogels were programmed as a display panel that exhibits three types of fake information under the wrong decoding tools. Only when the right stimuli are applied at the defined time does the panel give a readable pattern, allowing the encrypted information to be recognized. We believe this work will pave a novel path in developing extra safety information-encryption materials.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70034","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774047","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sangki Lee, Hyungjin Lee, Hyeonjun Lee, Seunghyeop Baek, Netanel Shpigel, Daniel Sharon, Seung-Tae Hong, Munseok S. Chae
Aqueous batteries are an emerging next-generation technology for large-scale energy storage. Among various metal-ion systems, manganese-based batteries have attracted significant interest due to their superior theoretical energy density over zinc-based battery systems. This study demonstrates oxygen vacancy-engineered vanadium oxide (V2O4.85) as a high-performance cathode material for aqueous manganese metal batteries. The V2O4.85 cathode had a discharge capacity of 212.6 mAh g−1 at 0.1 A g−1, retaining 89.5% capacity after 500 cycles. Oxygen vacancies enhanced ion diffusion and reduced migration barriers, facilitating both Mn2+ and H+ ion intercalation. Proton intercalation dominated charge storage, forming Mn(OH)2 layers, whereas Mn2+ contributed to surface-limited reactions. Furthermore, manganese metal batteries had a significantly higher operating voltage than that of aqueous zinc battery systems. Despite challenges with hydrogen evolution reactions at the Mn metal anode, this study underscores the potential of manganese batteries for future energy storage systems.
水电池是新兴的下一代大规模储能技术。在各种金属离子系统中,锰基电池由于其优于锌基电池系统的理论能量密度而引起了极大的兴趣。本研究证明了氧空位工程氧化钒(V2O4.85)是一种高性能的锰金属水电池正极材料。V2O4.85阴极在0.1 a g−1下的放电容量为212.6 mAh g−1,循环500次后容量保持89.5%。氧空位增强了离子扩散,降低了迁移障碍,促进了Mn2+和H+离子的嵌入。质子插入主导了电荷存储,形成了Mn(OH)2层,而Mn2+则促进了表面限制反应。此外,锰金属电池的工作电压明显高于锌水电池系统。尽管锰金属阳极的析氢反应存在挑战,但这项研究强调了锰电池在未来储能系统中的潜力。
{"title":"Oxygen Vacancy-Driven High-Performance V2O5 Cathodes for Aqueous Manganese Metal Batteries","authors":"Sangki Lee, Hyungjin Lee, Hyeonjun Lee, Seunghyeop Baek, Netanel Shpigel, Daniel Sharon, Seung-Tae Hong, Munseok S. Chae","doi":"10.1002/eem2.70036","DOIUrl":"https://doi.org/10.1002/eem2.70036","url":null,"abstract":"<p>Aqueous batteries are an emerging next-generation technology for large-scale energy storage. Among various metal-ion systems, manganese-based batteries have attracted significant interest due to their superior theoretical energy density over zinc-based battery systems. This study demonstrates oxygen vacancy-engineered vanadium oxide (V<sub>2</sub>O<sub>4.85</sub>) as a high-performance cathode material for aqueous manganese metal batteries. The V<sub>2</sub>O<sub>4.85</sub> cathode had a discharge capacity of 212.6 mAh g<sup>−1</sup> at 0.1 A g<sup>−1</sup>, retaining 89.5% capacity after 500 cycles. Oxygen vacancies enhanced ion diffusion and reduced migration barriers, facilitating both Mn<sup>2+</sup> and H<sup>+</sup> ion intercalation. Proton intercalation dominated charge storage, forming Mn(OH)<sub>2</sub> layers, whereas Mn<sup>2+</sup> contributed to surface-limited reactions. Furthermore, manganese metal batteries had a significantly higher operating voltage than that of aqueous zinc battery systems. Despite challenges with hydrogen evolution reactions at the Mn metal anode, this study underscores the potential of manganese batteries for future energy storage systems.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70036","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774039","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lithium-sulfur batteries have been developing in recent years and appear to offer an alternative to existing commercial batteries that can potentially replace them in the future. With their exceptional theoretical energy density, lower production costs, and affordable and environmentally friendly abundant raw materials, lithium-sulfur batteries have shown the ability to defeat counterparts in the race for rechargeable energy devices currently being developed. The lithium-sulfur batteries display extraordinary features, but they suffer from sulfur's non-conductivity, the shuttle effect that results from polysulfide dissolution, volumetric sulfur changes during charging, and dendrites at the anode, resulting in a decline in capacity and a short battery life. As a result of rigorous and innovative engineering designs, lithium-sulfur batteries have been developed to overcome their drawbacks and utilize their entire potential during the past decade. This review will pay particular attention to porous carbon-based matrix materials, especially graphene-based nanocomposites that are most commonly used in producing sulfur cathodes. We provide an in-depth perspective on the structural merits of graphene materials, the detailed mechanism by which they interact with sulfur, and essential strategies for designing high-performance cathodes for lithium-sulfur batteries. Finally, we discuss the significant challenges and prospects for developing lithium-sulfur batteries with high energy density and long cycle lives for the next-generation electric vehicles.
{"title":"Recent Developments and Prospects on Functional Graphene-Based Nanocomposites as Potential Sulfur Hosts for Next-Generation Lithium-Sulfur Batteries","authors":"Mohan Raj Krishnan, Chandra Sekhar Bongu, Edreese Housni Alsharaeh","doi":"10.1002/eem2.70032","DOIUrl":"https://doi.org/10.1002/eem2.70032","url":null,"abstract":"<p>Lithium-sulfur batteries have been developing in recent years and appear to offer an alternative to existing commercial batteries that can potentially replace them in the future. With their exceptional theoretical energy density, lower production costs, and affordable and environmentally friendly abundant raw materials, lithium-sulfur batteries have shown the ability to defeat counterparts in the race for rechargeable energy devices currently being developed. The lithium-sulfur batteries display extraordinary features, but they suffer from sulfur's non-conductivity, the shuttle effect that results from polysulfide dissolution, volumetric sulfur changes during charging, and dendrites at the anode, resulting in a decline in capacity and a short battery life. As a result of rigorous and innovative engineering designs, lithium-sulfur batteries have been developed to overcome their drawbacks and utilize their entire potential during the past decade. This review will pay particular attention to porous carbon-based matrix materials, especially graphene-based nanocomposites that are most commonly used in producing sulfur cathodes. We provide an in-depth perspective on the structural merits of graphene materials, the detailed mechanism by which they interact with sulfur, and essential strategies for designing high-performance cathodes for lithium-sulfur batteries. Finally, we discuss the significant challenges and prospects for developing lithium-sulfur batteries with high energy density and long cycle lives for the next-generation electric vehicles.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70032","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774099","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhihua Lin, Frederik Bettels, Taoran Li, Sreeja K. Satheesh, Haiwei Wu, Fei Ding, Chaofeng Zhang, Yuping Liu, Hui Ying Yang, Lin Zhang
Localized high-concentration electrolytes offer a potential solution for achieving uniform lithium deposition and a stable solid-electrolyte interface in Lithium metal batteries. However, the use of highly concentrated salts or structure-loaded diluents can result in significantly higher production costs and increased environmental burdens. Herein, a novel localized high-concentration electrolyte is developed, comprising ultra-low content (2% by mass) triethylammonium chloride as an electrolyte additive. The stable Lewis acid structure of the triethylammonium chloride molecule allows for the adsorption of numerous solvent molecules and TFSI− anions, intensifying the electrostatic interactions between lithium ions and anions. The chloride ions introduced by TC, along with TFSI− anions, integrate into the solvent sheath, forming a LiCl-rich inorganic SEI and enhancing the electrochemical performance of the lithium metal anode. The improved Li||Li cell shows excellent cycling stability for over 500 h at 1 mA cm2 with a 27 mV overpotential. This work provides insights into the impact of electrolyte additives on the electrode-electrolyte interface and Li-ion solvation, crucial for safer lithium metal battery development.
局部高浓度电解质为实现锂金属电池中均匀的锂沉积和稳定的固体-电解质界面提供了一个潜在的解决方案。然而,使用高浓度盐或结构负载稀释剂会导致生产成本显著提高,并增加环境负担。本文开发了一种新型局部高浓度电解质,其包含超低含量(质量比为2%)三乙基氯化铵作为电解质添加剂。三乙基氯化铵分子稳定的Lewis酸结构允许吸附大量溶剂分子和TFSI -阴离子,增强锂离子与阴离子之间的静电相互作用。TC引入的氯离子与TFSI -阴离子一起整合到溶剂鞘中,形成富licl的无机SEI,提高了锂金属阳极的电化学性能。改进的Li||锂电池在1 mA cm2和27 mV过电位下表现出超过500 h的优异循环稳定性。这项工作为电解质添加剂对电极-电解质界面和锂离子溶剂化的影响提供了见解,这对于更安全的锂金属电池的开发至关重要。
{"title":"Ultra-Low Content Triethylammonium Chloride Facilitates Localized High-Concentration Electrolytes and Formation of Inorganic Solid Electrolyte Interface","authors":"Zhihua Lin, Frederik Bettels, Taoran Li, Sreeja K. Satheesh, Haiwei Wu, Fei Ding, Chaofeng Zhang, Yuping Liu, Hui Ying Yang, Lin Zhang","doi":"10.1002/eem2.70029","DOIUrl":"https://doi.org/10.1002/eem2.70029","url":null,"abstract":"<p>Localized high-concentration electrolytes offer a potential solution for achieving uniform lithium deposition and a stable solid-electrolyte interface in Lithium metal batteries. However, the use of highly concentrated salts or structure-loaded diluents can result in significantly higher production costs and increased environmental burdens. Herein, a novel localized high-concentration electrolyte is developed, comprising ultra-low content (2% by mass) triethylammonium chloride as an electrolyte additive. The stable Lewis acid structure of the triethylammonium chloride molecule allows for the adsorption of numerous solvent molecules and TFSI<sup>−</sup> anions, intensifying the electrostatic interactions between lithium ions and anions. The chloride ions introduced by TC, along with TFSI<sup>−</sup> anions, integrate into the solvent sheath, forming a LiCl-rich inorganic SEI and enhancing the electrochemical performance of the lithium metal anode. The improved Li||Li cell shows excellent cycling stability for over 500 h at 1 mA cm<sup>2</sup> with a 27 mV overpotential. This work provides insights into the impact of electrolyte additives on the electrode-electrolyte interface and Li-ion solvation, crucial for safer lithium metal battery development.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70029","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144773902","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Getachew M.B., Tien M.N., Do Y.K., Dong W.K., Jungdon S., and Yongku K. Highly Ion-Conductive 3D Hybrid Solid Polymer Electrolyte Using Al-Doped Li7La3Zr2O12 Embedded Electrospun 3D Nanowebs for Ambient-Temperature All-Solid Lithium Polymer Batteries. Energy Environ. Mater. 2025, 8, 3. https://doi.org/10.1002/eem2.12860
In Experimental Section, the text “Detailed information related to the synthesis of active electrodes, physicochemical characterization, and electrochemical evaluation of bifunctional electrodes towards UOR and supercapacitor application is provided in Supporting Information” was incorrect. The corrected version is listed below.
Corrected to read: “Detailed information on the fabrication of electrodes and solid electrolytes, along with the physicochemical characterization and electrochemical evaluation of the solid electrolytes for all-solid-state lithium polymer battery applications, is provided in the Supporting Information.”
{"title":"Correction to “Highly Ion-Conductive 3D Hybrid Solid Polymer Electrolyte Using Al-Doped Li7La3Zr2O12 Embedded Electrospun 3D Nanowebs for Ambient-Temperature All-Solid Lithium Polymer Batteries”","authors":"","doi":"10.1002/eem2.70035","DOIUrl":"https://doi.org/10.1002/eem2.70035","url":null,"abstract":"<p>Getachew M.B., Tien M.N., Do Y.K., Dong W.K., Jungdon S., and Yongku K. Highly Ion-Conductive 3D Hybrid Solid Polymer Electrolyte Using Al-Doped Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> Embedded Electrospun 3D Nanowebs for Ambient-Temperature All-Solid Lithium Polymer Batteries. <i>Energy Environ. Mater</i>. 2025, 8, 3. https://doi.org/10.1002/eem2.12860</p><p>In Experimental Section, the text “Detailed information related to the synthesis of active electrodes, physicochemical characterization, and electrochemical evaluation of bifunctional electrodes towards UOR and supercapacitor application is provided in Supporting Information” was incorrect. The corrected version is listed below.</p><p>Corrected to read: “Detailed information on the fabrication of electrodes and solid electrolytes, along with the physicochemical characterization and electrochemical evaluation of the solid electrolytes for all-solid-state lithium polymer battery applications, is provided in the Supporting Information.”</p><p>We apologize for this error.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70035","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144773901","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Enhancing the stability of piezoelectric properties is essential for ensuring the reliability of high-temperature piezoelectric sensors. In this study, we have synthesized AlN piezoelectric crystals as representative materials and employed first-principles methods to investigate their temperature-dependent piezoelectric properties. By integrating the effects of lattice expansion and electron–phonon interactions, we accurately constructed the crystal structure of AlN across a wide temperature range and successfully predicted its piezoelectric behavior. Theoretical analysis reveals that ion polarization driven by lattice distortion and elastic softening of chemical bonds maintains the overall structural integrity of defect-free AlN single crystals, resulting in a stable piezoelectric coefficient d33 with a deviation of only 8.55% at temperatures up to 1300 K. However, experimental results indicate that the stability of the piezoelectric performance of the grown AlN crystals is disrupted at temperatures above 870 K. This temperature limitation is attributed to point defects within AlN crystals, particularly those caused by oxygen-substituted nitrogen (ON). These findings provide valuable guidance for enhancing the piezoelectric temperature stability of AlN crystals through optimized experimental conditions, such as oxygen atmosphere treatment and defect modification during crystal growth.
{"title":"Unveiling Temperature-Dependent Behavior of AlN Piezoelectric Single Crystal: Insights at the Atomic Scale","authors":"Yajing Fan, Lili Li, Linyu Bai, Qingzhi Song, Zijian Liu, Yanlu Li, Guodong Wang, Xiulan Duan, Lei Zhang, Fapeng Yu, Xiufeng Cheng, Xian Zhao","doi":"10.1002/eem2.70027","DOIUrl":"https://doi.org/10.1002/eem2.70027","url":null,"abstract":"<p>Enhancing the stability of piezoelectric properties is essential for ensuring the reliability of high-temperature piezoelectric sensors. In this study, we have synthesized AlN piezoelectric crystals as representative materials and employed first-principles methods to investigate their temperature-dependent piezoelectric properties. By integrating the effects of lattice expansion and electron–phonon interactions, we accurately constructed the crystal structure of AlN across a wide temperature range and successfully predicted its piezoelectric behavior. Theoretical analysis reveals that ion polarization driven by lattice distortion and elastic softening of chemical bonds maintains the overall structural integrity of defect-free AlN single crystals, resulting in a stable piezoelectric coefficient <i>d</i><sub>33</sub> with a deviation of only 8.55% at temperatures up to 1300 K. However, experimental results indicate that the stability of the piezoelectric performance of the grown AlN crystals is disrupted at temperatures above 870 K. This temperature limitation is attributed to point defects within AlN crystals, particularly those caused by oxygen-substituted nitrogen (O<sub>N</sub>). These findings provide valuable guidance for enhancing the piezoelectric temperature stability of AlN crystals through optimized experimental conditions, such as oxygen atmosphere treatment and defect modification during crystal growth.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70027","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774090","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Riyadh Abdekadir Khellouf, Vipin Cyriac, Constantin Bubulinca, Vladimir Sedlarik
The advancement of electric double-layer capacitors capable of operating beyond standard conditions is vital for meeting the demands of modern electronic applications. To realize this, huge efforts have been devoted to the development of biopolymer-based electrolytes. This study explores the potential application of a plasticized biopolymer-based electrolyte in electric double-layer capacitor systems at ambient and elevated temperatures. A plasticized Na CMC/PEO/LiClO4 electrolyte is successfully synthesized via a solution-casting approach. Fourier-transform infrared spectroscopy and X-ray diffraction verify the material's chemical and amorphous structure, respectively. The sample was designated as R20, with a salt concentration of 20 wt. % exhibits good electrochemical properties, including a high ionic conductivity of 3.73 × 10−4 S cm−1 and a wide electrochemical stability window of 3.2 V. The sample is placed into an electric double-layer capacitor cell and subjected to cyclic voltammetry and galvanostatic charge–discharge analyses at both room and high temperatures. The cyclic voltammetry test demonstrates that the electric double-layer capacitor achieves a specific capacitance (Cp) of 38 F g−1 at ambient temperature, which increases to 60 F g−1 at 60 °C. Additionally, the electric double-layer capacitor cell maintains consistent performance, demonstrating stable power and energy densities of 25 W kg−1 and 6 Wh kg−1, respectively, under both ambient and elevated temperatures.
能够在标准条件下工作的双电层电容器的进步对于满足现代电子应用的需求至关重要。为了实现这一点,生物聚合物电解质的开发已经投入了巨大的努力。本研究探讨了一种基于生物聚合物的塑化电解质在环境和高温下双电层电容器系统中的潜在应用。采用溶液浇铸法制备了Na CMC/PEO/LiClO4增塑电解质。傅里叶变换红外光谱和x射线衍射分别验证了材料的化学结构和非晶结构。样品编号为R20,盐浓度为20 wt。%具有良好的电化学性能,包括3.73 × 10−4 S cm−1的高离子电导率和3.2 V的宽电化学稳定窗口。将样品放入双层电容电池中,在室温和高温下进行循环伏安法和恒流充放电分析。循环伏安法测试表明,双电层电容器在环境温度下的比电容(Cp)为38 F g−1,在60℃时增加到60 F g−1。此外,电双层电容器电池保持稳定的性能,在环境和高温下分别表现出25 W kg - 1和6 Wh kg - 1的稳定功率和能量密度。
{"title":"Deciphering the Role of LiClO4 Salt on Electrochemical Properties of Plasticized Biopolymer Electrolytes for Superior EDLC Efficiency at Elevated Temperatures","authors":"Riyadh Abdekadir Khellouf, Vipin Cyriac, Constantin Bubulinca, Vladimir Sedlarik","doi":"10.1002/eem2.70023","DOIUrl":"https://doi.org/10.1002/eem2.70023","url":null,"abstract":"<p>The advancement of electric double-layer capacitors capable of operating beyond standard conditions is vital for meeting the demands of modern electronic applications. To realize this, huge efforts have been devoted to the development of biopolymer-based electrolytes. This study explores the potential application of a plasticized biopolymer-based electrolyte in electric double-layer capacitor systems at ambient and elevated temperatures. A plasticized Na CMC/PEO/LiClO<sub>4</sub> electrolyte is successfully synthesized via a solution-casting approach. Fourier-transform infrared spectroscopy and X-ray diffraction verify the material's chemical and amorphous structure, respectively. The sample was designated as R20, with a salt concentration of 20 wt. % exhibits good electrochemical properties, including a high ionic conductivity of 3.73 × 10<sup>−4</sup> S cm<sup>−1</sup> and a wide electrochemical stability window of 3.2 V. The sample is placed into an electric double-layer capacitor cell and subjected to cyclic voltammetry and galvanostatic charge–discharge analyses at both room and high temperatures. The cyclic voltammetry test demonstrates that the electric double-layer capacitor achieves a specific capacitance (<i>C</i><sub>p</sub>) of 38 F g<sup>−1</sup> at ambient temperature, which increases to 60 F g<sup>−1</sup> at 60 °C. Additionally, the electric double-layer capacitor cell maintains consistent performance, demonstrating stable power and energy densities of 25 W kg<sup>−1</sup> and 6 Wh kg<sup>−1</sup>, respectively, under both ambient and elevated temperatures.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70023","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774091","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The efficiency of carbon dioxide (CO2) adsorption in carbonaceous materials is primarily influenced by their microporosity and thermodynamic affinity for CO2. However, achieving optimal heteroatom doping and precise micropore engineering through advanced activation techniques remains a significant challenge. We introduce a solvent-free one-pot method using polythiophene, melamine, and KOH to prepare highly microporous, heteroatom-co-doped carbons (NSC). This approach leverages sulfur from polythiophene, nitrogen from melamine, and the activation agent KOH to enhance CO2 capture performance. Our results demonstrate that the optimized sample, NSC-800, achieves a CO2 adsorption capacity of 280.5 mg g−1 at 273 K and 1 bar, attributed to its high nitrogen (6.5 at.%) and sulfur (3.4 at.%) contents, a specific surface area of 2888 m2 g−1, and a micropore volume of 1.685 cm3 g−1. The moderate isosteric heat of adsorption (27.7 kJ mol−1) indicates a primarily physisorption-driven mechanism, as confirmed by close alignment with the pseudo-first-order polynomial model (R2 > 0.99) across temperatures of 303–323 K. This study reveals that NSC-800 also displays efficient regeneration after ten cycles of CO2 adsorption–desorption under flue gas conditions (15% CO2 and 85% N2 at 313 K), highlighting its potential as a regenerable, energy-efficient adsorbent for practical CO2 capture applications.
碳质材料对CO2的吸附效率主要受其微孔隙度和对CO2的热力学亲和性的影响。然而,通过先进的活化技术实现最佳的杂原子掺杂和精确的微孔工程仍然是一个重大挑战。介绍了一种用聚噻吩、三聚氰胺和KOH制备高微孔杂原子共掺杂碳(NSC)的无溶剂一锅法。该方法利用聚噻吩中的硫、三聚氰胺中的氮和活化剂KOH来提高CO2捕获性能。结果表明,优化后的样品NSC-800在273 K和1 bar条件下的CO2吸附量为280.5 mg g - 1,这主要归功于其高氮(6.5% at.%)和高硫(3.4 at.%)含量、2888 m2 g - 1的比表面积和1.685 cm3 g - 1的微孔体积。中等等等吸附热(27.7 kJ mol−1)表明主要是物理吸附驱动的机制,在303-323 K范围内与伪一阶多项式模型(R2 > 0.99)非常接近。该研究表明,NSC-800在烟气条件下(313 K下,15% CO2和85% N2)进行10次CO2吸附-解吸循环后也显示出高效的再生能力,突出了其作为可再生、节能吸附剂的潜力,可用于实际的CO2捕获应用。
{"title":"Hierarchically Porous Heteroatom-co-Doped Carbons for Enhanced Carbon Dioxide Capture","authors":"Choong-Hee Kim, Seul-Yi Lee, Soo-Jin Park","doi":"10.1002/eem2.70026","DOIUrl":"https://doi.org/10.1002/eem2.70026","url":null,"abstract":"<p>The efficiency of carbon dioxide (CO<sub>2</sub>) adsorption in carbonaceous materials is primarily influenced by their microporosity and thermodynamic affinity for CO<sub>2</sub>. However, achieving optimal heteroatom doping and precise micropore engineering through advanced activation techniques remains a significant challenge. We introduce a solvent-free one-pot method using polythiophene, melamine, and KOH to prepare highly microporous, heteroatom-<i>co</i>-doped carbons (NSC). This approach leverages sulfur from polythiophene, nitrogen from melamine, and the activation agent KOH to enhance CO<sub>2</sub> capture performance. Our results demonstrate that the optimized sample, NSC-800, achieves a CO<sub>2</sub> adsorption capacity of 280.5 mg g<sup>−1</sup> at 273 K and 1 bar, attributed to its high nitrogen (6.5 at.%) and sulfur (3.4 at.%) contents, a specific surface area of 2888 m<sup>2</sup> g<sup>−1</sup>, and a micropore volume of 1.685 cm<sup>3</sup> g<sup>−1</sup>. The moderate isosteric heat of adsorption (27.7 kJ mol<sup>−1</sup>) indicates a primarily physisorption-driven mechanism, as confirmed by close alignment with the pseudo-first-order polynomial model (<i>R</i><sup>2</sup> > 0.99) across temperatures of 303–323 K. This study reveals that NSC-800 also displays efficient regeneration after ten cycles of CO<sub>2</sub> adsorption–desorption under flue gas conditions (15% CO<sub>2</sub> and 85% N<sub>2</sub> at 313 K), highlighting its potential as a regenerable, energy-efficient adsorbent for practical CO<sub>2</sub> capture applications.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 6","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70026","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145272992","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Alba Fombona-Pascual, Sergio Pinilla, Irene Hormigos, Jesús Palma, Julio J. Lado
Water scarcity, driven by climate change and population growth, necessitates innovative desalination technologies. Conventional methods for brackish water desalination are limited by high-energy demands, especially in the low salinity range, prompting the exploration of electrochemical approaches like faradaic deionization. Sodium-manganese oxides, traditionally used in sodium-ion batteries, show promise as faradaic deionization electrode materials due to their abundance, low toxicity, and cost-effectiveness. However, capacity fading during cycling, often caused by structural changes, volume expansion, or chemical transformations, remains a critical challenge. This study investigates the impact of morphology and crystal structure on the electrochemical performance of commercial and synthesized sodium-manganese oxides for faradaic deionization applications. Structural and electrochemical characterization in three-electrode cells with low-concentration electrolytes provided insights into the charge storage mechanisms. Rocking-chair full flow cell experiments demonstrated that the mixed-phase sodium-manganese oxide exhibited superior desalination performance, achieving a high salt removal capacity of 54.5 mg g−1 and a mean value in the salt removal rate of 1.49 mg g−1 min−1. Notably, mixed-phase sodium-manganese oxide maintained 98% capacity retention over 870 cycles, one of the longest reported cycling experiments in this field, effectively mitigating the Jahn-Teller effect. These findings highlight the crucial role of sodium-manganese oxide structure and morphology in electrochemical performance, positioning mixed-phase sodium-manganese oxide as a strong candidate for sustainable water treatment technologies.
{"title":"Sodium-Manganese Oxides in Faradaic Desalination: Achieving Long-Cycling Stability Through Morphological and Structural Optimization","authors":"Alba Fombona-Pascual, Sergio Pinilla, Irene Hormigos, Jesús Palma, Julio J. Lado","doi":"10.1002/eem2.70022","DOIUrl":"https://doi.org/10.1002/eem2.70022","url":null,"abstract":"<p>Water scarcity, driven by climate change and population growth, necessitates innovative desalination technologies. Conventional methods for brackish water desalination are limited by high-energy demands, especially in the low salinity range, prompting the exploration of electrochemical approaches like faradaic deionization. Sodium-manganese oxides, traditionally used in sodium-ion batteries, show promise as faradaic deionization electrode materials due to their abundance, low toxicity, and cost-effectiveness. However, capacity fading during cycling, often caused by structural changes, volume expansion, or chemical transformations, remains a critical challenge. This study investigates the impact of morphology and crystal structure on the electrochemical performance of commercial and synthesized sodium-manganese oxides for faradaic deionization applications. Structural and electrochemical characterization in three-electrode cells with low-concentration electrolytes provided insights into the charge storage mechanisms. Rocking-chair full flow cell experiments demonstrated that the mixed-phase sodium-manganese oxide exhibited superior desalination performance, achieving a high salt removal capacity of 54.5 mg g<sup>−1</sup> and a mean value in the salt removal rate of 1.49 mg g<sup>−1</sup> min<sup>−1</sup>. Notably, mixed-phase sodium-manganese oxide maintained 98% capacity retention over 870 cycles, one of the longest reported cycling experiments in this field, effectively mitigating the Jahn-Teller effect. These findings highlight the crucial role of sodium-manganese oxide structure and morphology in electrochemical performance, positioning mixed-phase sodium-manganese oxide as a strong candidate for sustainable water treatment technologies.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70022","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774114","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}