Sodium titanium phosphate (NaTi2(PO4)3, NTP) has emerged as a promising electrode material due to its three-dimensional open framework. This study investigates the use of NTP in aqueous dilute Li+/Na+ electrolytes and extends its application to high-concentration K+ electrolytes. X-ray photoelectron spectroscopy, X-ray absorption near-edge structure analysis, and density functional theory calculations revealed that highly electronegative fluorine partially substitutes for oxygen in the NTP lattice, resulting in the formation of Ti-F bonds. The substitution effectively modulates the electronic structure of Ti4+, alters the local coordination environment, and influences the redox dynamics. Enhanced long-term cycling stability and rate performance were demonstrated across aqueous sodium-ion, lithium-ion, and potassium-ion half-cells. Among the investigated systems, the aqueous sodium-ion system exhibited the best electrochemical performance, characterized by a single, well-defined charge–discharge plateau, stable cycling behavior with 88.7% capacity retention after 500 cycles at 1 A g−1, and an initial specific discharge capacity of 121.7 mAh g−1 at 0.2 A g−1. The results establish F-doped NTP as a promising candidate for advanced energy storage applications in aqueous alkali metal-ion batteries.
磷酸钛钠(NaTi2(PO4)3, NTP)由于其三维开放结构而成为一种很有前途的电极材料。本研究研究了NTP在稀Li+/Na+水溶液中的应用,并将其应用于高浓度K+电解质。x射线光电子能谱、x射线吸收近边结构分析和密度泛函理论计算表明,高电负性的氟在NTP晶格中部分取代了氧,导致Ti-F键的形成。取代有效地调节了Ti4+的电子结构,改变了局部配位环境,影响了氧化还原动力学。在钠离子、锂离子和钾离子半电池中证明了增强的长期循环稳定性和速率性能。其中,水溶液钠离子体系表现出最佳的电化学性能,具有单一、清晰的充放电平台,在1 a g−1条件下循环500次后容量保持率为88.7%,在0.2 a g−1条件下初始比放电容量为121.7 mAh g−1。结果表明,f掺杂NTP作为一种有前途的候选材料,可以应用于碱金属离子电池的先进储能。
{"title":"Fluorine-Doped NaTi2(PO4)3 Via Electronic Orbital Modulation and Bandgap Engineering for Aqueous Li/Na/K-Ion Batteries","authors":"Tong Xu, Jiaojiao Yu, Junchao Ma, Hongbo Yu, Junling Che, Qixiang Yin, Yukun Xi, Yanyan Cao, Mangmang Shi, Shuting Wang, Wu Wan, Changxin Li, Rui Chen, Jinniu Zhang, Qiyi Zhao, Wei Ren, Mingliang Hu, Xifei Li","doi":"10.1002/eem2.70043","DOIUrl":"https://doi.org/10.1002/eem2.70043","url":null,"abstract":"<p>Sodium titanium phosphate (NaTi<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub>, NTP) has emerged as a promising electrode material due to its three-dimensional open framework. This study investigates the use of NTP in aqueous dilute Li<sup>+</sup>/Na<sup>+</sup> electrolytes and extends its application to high-concentration K<sup>+</sup> electrolytes. X-ray photoelectron spectroscopy, X-ray absorption near-edge structure analysis, and density functional theory calculations revealed that highly electronegative fluorine partially substitutes for oxygen in the NTP lattice, resulting in the formation of Ti-F bonds. The substitution effectively modulates the electronic structure of Ti<sup>4+</sup>, alters the local coordination environment, and influences the redox dynamics. Enhanced long-term cycling stability and rate performance were demonstrated across aqueous sodium-ion, lithium-ion, and potassium-ion half-cells. Among the investigated systems, the aqueous sodium-ion system exhibited the best electrochemical performance, characterized by a single, well-defined charge–discharge plateau, stable cycling behavior with 88.7% capacity retention after 500 cycles at 1 A g<sup>−1</sup>, and an initial specific discharge capacity of 121.7 mAh g<sup>−1</sup> at 0.2 A g<sup>−1</sup>. The results establish F-doped NTP as a promising candidate for advanced energy storage applications in aqueous alkali metal-ion batteries.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70043","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774162","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}
In the present review, we addressed the synthesis and applications of the magnetic layered double hydroxide nanocomposites in different scientific areas including catalysis, environmental remediation, and biological functions. First, we appraised the varied approaches for the synthesis of layered double hydroxides (LDHs), containing co-precipitation, hydrothermal, sol–gel, ion-exchange, urea hydrolysis, and reconstruction methods. Afterward, we concentrated on the utility of the magnetic LDH-based composites and evaluated their catalytic effectiveness in 4-nitrophenol reduction, coupling reactions, preparation of polycyclic aromatic compounds, and oxidation reactions. Next, the applicability of magnetic LDHs was assessed in the removal of water pollutants and dyes. Ultimately, we discussed the efficiency of magnetic LDH nanocomposites for biological applications like drug delivery. Investigating the obtained results of the reviewed reports demonstrated the auspicious performance of these compounds in all of the above-mentioned fields. Overall, the magnetic LDH-based composites manifested a satisfactory outlook in various scientific areas due to their stability, remarkable flexibility, relatively proper surface area, appropriate adsorption capacity, as well as propitious retrievability and reusability character.
{"title":"Magnetic Layered Double Hydroxide Nanocomposites: Synthesis, Catalytic Performances, Environmental and Biological Applications","authors":"Mohammad Mavvaji, Ahmed M. Senan, Senem Akkoc","doi":"10.1002/eem2.70015","DOIUrl":"https://doi.org/10.1002/eem2.70015","url":null,"abstract":"<p>In the present review, we addressed the synthesis and applications of the magnetic layered double hydroxide nanocomposites in different scientific areas including catalysis, environmental remediation, and biological functions. First, we appraised the varied approaches for the synthesis of layered double hydroxides (LDHs), containing co-precipitation, hydrothermal, sol–gel, ion-exchange, urea hydrolysis, and reconstruction methods. Afterward, we concentrated on the utility of the magnetic LDH-based composites and evaluated their catalytic effectiveness in 4-nitrophenol reduction, coupling reactions, preparation of polycyclic aromatic compounds, and oxidation reactions. Next, the applicability of magnetic LDHs was assessed in the removal of water pollutants and dyes. Ultimately, we discussed the efficiency of magnetic LDH nanocomposites for biological applications like drug delivery. Investigating the obtained results of the reviewed reports demonstrated the auspicious performance of these compounds in all of the above-mentioned fields. Overall, the magnetic LDH-based composites manifested a satisfactory outlook in various scientific areas due to their stability, remarkable flexibility, relatively proper surface area, appropriate adsorption capacity, as well as propitious retrievability and reusability character.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70015","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774161","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}
Integrating phase change materials (PCM) into thermal insulation materials offers a novel approach to aerospace thermal protection. Herein, we used waste biomass as a template; by selecting the appropriate carbonization temperature, we obtained carbon aerogels (CCA) with extremely high porosity (95.8%) and high pore volume. After encapsulating PEG2000, we achieved high enthalpy (137.79 J g−1, 91% of pure PEG2000) and low thermal conductivity (0.137 W (m·K)−1, 45% of pure PEG2000). Thanks to the rich hierarchical nano-micro porous structure of CCA and the high latent heat of PEG2000, CCA/PEG exhibits excellent thermal insulation properties (under a heating temperature of 131 °C, the material takes 1400 s to reach its maximum temperature and can be maintained below 65 °C) and cycle performance. Additionally, irradiation destroyed the structure of CCA/PEG, leading to the degradation of PEG and the formation of other carbonyl-containing compounds, which decreased its latent heat (4.2%) and thermal conductivity (16.1%). However, the irradiation-resistant CCA, acting as a protective layer, minimizes the impact of irradiation on PEG2000. Instead, irradiation enhances the hierarchical porous structure of the material, ultimately improving its thermal insulation performance. CCA/PEG has potential application prospects in thermal protection and aerospace and is a strong competitor for high-efficiency thermal insulation materials.
将相变材料(PCM)集成到隔热材料中,为航空航天热防护提供了一种新的方法。在这里,我们使用废弃生物质作为模板;通过选择合适的炭化温度,获得了具有极高孔隙率(95.8%)和高孔隙体积的碳气凝胶(CCA)。封装PEG2000后,我们获得了高焓(137.79 J g−1,为纯PEG2000的91%)和低导热系数(0.137 W (m·K)−1,为纯PEG2000的45%)。由于CCA具有丰富的分层纳米微孔结构和PEG2000的高潜热,CCA/PEG具有优异的隔热性能(在131℃的加热温度下,材料达到最高温度需要1400 s,并能保持在65℃以下)和循环性能。此外,辐照破坏了CCA/PEG的结构,导致PEG降解并生成其他含羰基化合物,从而降低了其潜热(4.2%)和导热系数(16.1%)。然而,抗辐照CCA作为保护层,将辐照对PEG2000的影响降至最低。相反,辐照增强了材料的分层多孔结构,最终提高了其隔热性能。CCA/PEG在热防护和航空航天领域具有潜在的应用前景,是高效保温材料的有力竞争者。
{"title":"Ultra-Compact Cellular Structured Bio-Carbon Aerogels Supported PCM for Exceptional Thermal Insulation and Radiation Shielding for Space Applications","authors":"Zihao Zhao, Daili Feng, Xinxin Zhang, Yanhui Feng","doi":"10.1002/eem2.70042","DOIUrl":"https://doi.org/10.1002/eem2.70042","url":null,"abstract":"<p>Integrating phase change materials (PCM) into thermal insulation materials offers a novel approach to aerospace thermal protection. Herein, we used waste biomass as a template; by selecting the appropriate carbonization temperature, we obtained carbon aerogels (CCA) with extremely high porosity (95.8%) and high pore volume. After encapsulating PEG2000, we achieved high enthalpy (137.79 J g<sup>−1</sup>, 91% of pure PEG2000) and low thermal conductivity (0.137 W (m·K)<sup>−1</sup>, 45% of pure PEG2000). Thanks to the rich hierarchical nano-micro porous structure of CCA and the high latent heat of PEG2000, CCA/PEG exhibits excellent thermal insulation properties (under a heating temperature of 131 °C, the material takes 1400 s to reach its maximum temperature and can be maintained below 65 °C) and cycle performance. Additionally, irradiation destroyed the structure of CCA/PEG, leading to the degradation of PEG and the formation of other carbonyl-containing compounds, which decreased its latent heat (4.2%) and thermal conductivity (16.1%). However, the irradiation-resistant CCA, acting as a protective layer, minimizes the impact of irradiation on PEG2000. Instead, irradiation enhances the hierarchical porous structure of the material, ultimately improving its thermal insulation performance. CCA/PEG has potential application prospects in thermal protection and aerospace and is a strong competitor for high-efficiency thermal insulation materials.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70042","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774022","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}
Self-powered sensing technologies are increasingly sought for intelligent and autonomous marine environmental monitoring. A Faraday cage-enabled triboelectric nanogenerator (FC-TENG) is developed by incorporating a FeCoCrNiAl alloy powder layer, enabling efficient harvesting of low-frequency mechanical energy. The quasi-enclosed conductive architecture mimics a Faraday cage, effectively confining electrostatic charges and suppressing edge-induced dissipation, thereby enhancing charge retention. Compared to single-metal triboelectric layers, the FC-TENG exhibits 4.86-, 3.57-, and 2.76-fold increases in open-circuit voltage (VOC, 1276.27 V), short-circuit current (ISC, 63.69 μA), and transferred charge (QSC, 29.55 nC), respectively. Its hydrophobic surface further ensures environmental robustness and stable output under humid conditions. With an optimized load resistance of 60 MΩ, the FC-TENG device achieves a peak power of ~4.08 mW and reliably powers LED arrays and environmental sensors, while enabling efficient energy storage across a wide frequency range. Furthermore, a wave-driven FC-TENG system integrated with wireless communication and visual feedback modules enables real-time marine motion monitoring without external power. This work introduces the Faraday cage–inspired triboelectric device based on microspherical alloy powder, offering enhanced charge retention, humidity tolerance, and dual-mode functionality in power generation and marine wave sensing. The proposed strategy provides a robust and scalable architecture for future self-powered systems operating in harsh environments.
{"title":"A Faraday Cage-Inspired Triboelectric Nanogenerator Enabled by Alloy Powder Architecture for Self-Powered Ocean Sensing","authors":"Kequan Xia, Yutao Hao, Penghui Luo, Yu Zhang, Jing Guo, Zhiyuan Zhu","doi":"10.1002/eem2.70040","DOIUrl":"https://doi.org/10.1002/eem2.70040","url":null,"abstract":"<p>Self-powered sensing technologies are increasingly sought for intelligent and autonomous marine environmental monitoring. A Faraday cage-enabled triboelectric nanogenerator (FC-TENG) is developed by incorporating a FeCoCrNiAl alloy powder layer, enabling efficient harvesting of low-frequency mechanical energy. The quasi-enclosed conductive architecture mimics a Faraday cage, effectively confining electrostatic charges and suppressing edge-induced dissipation, thereby enhancing charge retention. Compared to single-metal triboelectric layers, the FC-TENG exhibits 4.86-, 3.57-, and 2.76-fold increases in open-circuit voltage (<i>V</i><sub>OC</sub>, 1276.27 V), short-circuit current (<i>I</i><sub>SC</sub>, 63.69 μA), and transferred charge (<i>Q</i><sub>SC</sub>, 29.55 nC), respectively. Its hydrophobic surface further ensures environmental robustness and stable output under humid conditions. With an optimized load resistance of 60 MΩ, the FC-TENG device achieves a peak power of ~4.08 mW and reliably powers LED arrays and environmental sensors, while enabling efficient energy storage across a wide frequency range. Furthermore, a wave-driven FC-TENG system integrated with wireless communication and visual feedback modules enables real-time marine motion monitoring without external power. This work introduces the Faraday cage–inspired triboelectric device based on microspherical alloy powder, offering enhanced charge retention, humidity tolerance, and dual-mode functionality in power generation and marine wave sensing. The proposed strategy provides a robust and scalable architecture for future self-powered systems operating in harsh environments.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70040","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774025","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}
Water-induced electric generators (WEGs) exhibit tremendous promise as sustainable energy sources harvesting electricity through the interaction between materials and water utilizing the hydrovoltaic effect, an innovative green energy harvesting method. However, existing water-induced electric generator devices predominantly rely on inorganic materials with limited research on naturally available, bio-based materials for hydrovoltaic energy harvesting. This study introduces a novel nutshell-based hydrovoltaic water-induced electric generator for the first time. This low-cost, organic, and efficient renewable energy source can generate a voltage above 600 mV with a power density exceeding 5.96 μW cm−2 utilizing streaming and evaporation potential methodologies, which can be sustained for more than a week. Notably, after further chemical treatments and combining the physical and chemical phenomena, output voltage and maximum current density reach a record high of 1.21 V and 347.2 μA cm−2 respectively, which outperforms most inorganic and organic materials-based water-induced electric generators. By connecting two units in series and parallel, this eco-friendly water-induced electric generator can power an LCD calculator without the assistance of any rectifier. We believe that this novel nutshell-based water-induced electric generator provides a significant advancement in water-induced electric generator technology by offering a sustainable solution for powering electronic devices utilizing agricultural waste.
{"title":"Hydrovoltaic Energy Harvesting From Nut Shells","authors":"Nazmul Hossain, Roozbeh Abbasi, Weinan Zhao, Xiaoye Zhao, Aiping Yu, Norman Zhou","doi":"10.1002/eem2.70017","DOIUrl":"https://doi.org/10.1002/eem2.70017","url":null,"abstract":"<p>Water-induced electric generators (WEGs) exhibit tremendous promise as sustainable energy sources harvesting electricity through the interaction between materials and water utilizing the hydrovoltaic effect, an innovative green energy harvesting method. However, existing water-induced electric generator devices predominantly rely on inorganic materials with limited research on naturally available, bio-based materials for hydrovoltaic energy harvesting. This study introduces a novel nutshell-based hydrovoltaic water-induced electric generator for the first time. This low-cost, organic, and efficient renewable energy source can generate a voltage above 600 mV with a power density exceeding 5.96 μW cm<sup>−2</sup> utilizing streaming and evaporation potential methodologies, which can be sustained for more than a week. Notably, after further chemical treatments and combining the physical and chemical phenomena, output voltage and maximum current density reach a record high of 1.21 V and 347.2 μA cm<sup>−2</sup> respectively, which outperforms most inorganic and organic materials-based water-induced electric generators. By connecting two units in series and parallel, this eco-friendly water-induced electric generator can power an LCD calculator without the assistance of any rectifier. We believe that this novel nutshell-based water-induced electric generator provides a significant advancement in water-induced electric generator technology by offering a sustainable solution for powering electronic devices utilizing agricultural waste.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70017","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774024","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}
Sang Yoon Park, Se Jin Choi, Jae Chan Kim, Daniel J. Joe, Han Eol Lee
Electrocardiogram (ECG) sensor is emerging as an essential medical device for diagnosing various cardiovascular diseases in modern people. Conventional ECG sensors have investigated by several researchers, but they still have significant issues of discomfort in wearing, easy swelling, poor electrical conductivity, and signal inaccuracy. Here, we demonstrate a hydrogel nanocomposite-based ECG sensor patches, monolithically integrated with a hydrogel-based biocompatible electrode and an electromagnetic interference (EMI) shielding layer in a single unit. The developed device with low impedance (20 kΩ) exhibited excellent mechanical properties including adhesion force (35.8 N m−1), multiple detachability (5 times), stretching/twisting stability and self-healing characteristic. The ECG sensor displayed superior long-term humidity stability for 30 days, showing superior biocompatibility. Finally, the ECG patch with high EMI shielding property monitored human vital signal and pulse rate changes in real-time.
心电图传感器正逐渐成为现代人诊断各种心血管疾病的必备医疗设备。传统的心电传感器已经被一些研究人员研究过,但它们仍然存在佩戴不舒服、容易肿胀、导电性差和信号不准确等显著问题。在这里,我们展示了一种基于水凝胶纳米复合材料的ECG传感器贴片,该贴片与基于水凝胶的生物相容性电极和电磁干扰(EMI)屏蔽层单片集成在一个单元中。所开发的低阻抗器件(20 kΩ)具有优异的机械性能,包括附着力(35.8 N m−1)、多次可拆卸性(5次)、拉伸/扭转稳定性和自修复特性。该心电传感器具有30天的长期湿度稳定性,具有良好的生物相容性。最后,采用高电磁干扰屏蔽性能的心电贴片实时监测人体生命信号和脉搏率变化。
{"title":"Self-Healable and Conductive Hydrogel Nanocomposite with High Environmental Stability for Electromagnetic-Interference-Free Electrocardiography Patches","authors":"Sang Yoon Park, Se Jin Choi, Jae Chan Kim, Daniel J. Joe, Han Eol Lee","doi":"10.1002/eem2.70039","DOIUrl":"https://doi.org/10.1002/eem2.70039","url":null,"abstract":"<p>Electrocardiogram (ECG) sensor is emerging as an essential medical device for diagnosing various cardiovascular diseases in modern people. Conventional ECG sensors have investigated by several researchers, but they still have significant issues of discomfort in wearing, easy swelling, poor electrical conductivity, and signal inaccuracy. Here, we demonstrate a hydrogel nanocomposite-based ECG sensor patches, monolithically integrated with a hydrogel-based biocompatible electrode and an electromagnetic interference (EMI) shielding layer in a single unit. The developed device with low impedance (20 kΩ) exhibited excellent mechanical properties including adhesion force (35.8 N m<sup>−1</sup>), multiple detachability (5 times), stretching/twisting stability and self-healing characteristic. The ECG sensor displayed superior long-term humidity stability for 30 days, showing superior biocompatibility. Finally, the ECG patch with high EMI shielding property monitored human vital signal and pulse rate changes in real-time.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70039","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774010","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-Selenium (Li-Se) batteries have emerged as one of the most promising candidates for next-generation energy storage systems owing to superior electronic conductivity, impressive volumetric capacity, and enhanced compatibility with carbonate electrolyte of selenium, comparable to sulfur. Despite these advantages, the development of Li-Se batteries is impeded by several intrinsic challenges, including volume expansion during the discharge process and the consequent sluggish reaction kinetics that undermine their electrochemical performance. In this study, MIL-91(Al) is used as an electrode additive to accelerate the one-step mutual solid–solid conversion reaction between Se and Li2Se in the carbonate-based electrolyte. By doing so, uncontrollable deposition of Li2Se is effectively mitigated, enhancing the electrochemical performance of the system. Thus, the use of MIL-91(Al) results in reduced internal resistance and faster Li-ion transfer rate, as analyzed by SPEIS and GITT. Ab initio calculations and molecular dynamics simulations further reveal that Li2Se anchors to closely situated dangling oxygens of the phosphonate group of the organic linker of MIL-91(Al), inducing relaxation of the Li-Se-Li angle and stabilizing the overall structure. Accordingly, the MIL-91(Al)-containing Li-Se cells demonstrate a high specific capacity of approximately 530 mAh g−1 at 1C (675 mA g−1) after 100 cycles and retaining a specific capacity of 320 mAh/g even under high current rate (20C) after 200 cycles. This research underlines the importance of the use of electrocatalyst/electroadsorbent materials to enhance the redox kinetics of the conversion reactions between Se and Li2Se, thus paving the way for the development of high-performance Li-Se batteries.
锂硒(Li-Se)电池已成为下一代储能系统最有前途的候选者之一,因为它具有卓越的电子导电性,令人印象深刻的体积容量,以及与硒的碳酸盐电解质的相容性增强,可与硫相媲美。尽管有这些优势,但锂硒电池的发展受到一些内在挑战的阻碍,包括放电过程中的体积膨胀以及由此产生的反应动力学缓慢,从而破坏了它们的电化学性能。本研究采用MIL-91(Al)作为电极添加剂,在碳酸盐基电解质中加速Se与Li2Se之间的一步固固互转化反应。通过这样做,有效地减轻了Li2Se的不可控沉积,提高了体系的电化学性能。因此,根据SPEIS和git的分析,MIL-91(Al)的使用导致内阻降低和锂离子传输速率加快。从头计算和分子动力学模拟进一步表明,Li2Se锚定在MIL-91(Al)有机连接体的膦酸基团上,诱导Li-Se-Li角的松弛,从而稳定了整体结构。因此,MIL-91(Al)含Li-Se电池在1C (675 mA g - 1)循环100次后显示出约530 mAh g - 1的高比容量,并且在200次循环后即使在高电流(20℃)下也保持320 mAh/g的比容量。这项研究强调了使用电催化剂/电吸附材料来增强Se和Li2Se之间转化反应的氧化还原动力学的重要性,从而为高性能Li-Se电池的发展铺平了道路。
{"title":"MIL-91(Al) to Boost Solid–Solid Conversion Reactions in Li-Se Batteries","authors":"Tutku Mutlu-Cetinkaya, Pieter Dobbelaere, Wim Temmerman, Wenqing Lu, Vanessa Pimenta, Veronique Van Speybroeck, Rezan Demir-Cakan","doi":"10.1002/eem2.70038","DOIUrl":"https://doi.org/10.1002/eem2.70038","url":null,"abstract":"<p>Lithium-Selenium (Li-Se) batteries have emerged as one of the most promising candidates for next-generation energy storage systems owing to superior electronic conductivity, impressive volumetric capacity, and enhanced compatibility with carbonate electrolyte of selenium, comparable to sulfur. Despite these advantages, the development of Li-Se batteries is impeded by several intrinsic challenges, including volume expansion during the discharge process and the consequent sluggish reaction kinetics that undermine their electrochemical performance. In this study, MIL-91(Al) is used as an electrode additive to accelerate the one-step mutual solid–solid conversion reaction between Se and Li<sub>2</sub>Se in the carbonate-based electrolyte. By doing so, uncontrollable deposition of Li<sub>2</sub>Se is effectively mitigated, enhancing the electrochemical performance of the system. Thus, the use of MIL-91(Al) results in reduced internal resistance and faster Li-ion transfer rate, as analyzed by SPEIS and GITT. Ab initio calculations and molecular dynamics simulations further reveal that Li<sub>2</sub>Se anchors to closely situated dangling oxygens of the phosphonate group of the organic linker of MIL-91(Al), inducing relaxation of the Li-Se-Li angle and stabilizing the overall structure. Accordingly, the MIL-91(Al)-containing Li-Se cells demonstrate a high specific capacity of approximately 530 mAh g<sup>−1</sup> at 1C (675 mA g<sup>−1</sup>) after 100 cycles and retaining a specific capacity of 320 mAh/g even under high current rate (20C) after 200 cycles. This research underlines the importance of the use of electrocatalyst/electroadsorbent materials to enhance the redox kinetics of the conversion reactions between Se and Li<sub>2</sub>Se, thus paving the way for the development of high-performance Li-Se batteries.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70038","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774060","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}
Mattia Longo, Matteo Gandolfo, Nuria Abigail Plebani, Cecilia Andrea Calderon, Matteo Destro, Daniela Fontana, Silvia Bodoardo, Julia Amici
Gel polymer electrolytes (GPEs) present the best compromise between mechanical and electrochemical properties, as well as an improvement of the cell safety in the framework of Li metal batteries production. However, the polymerization mechanism typically employed relies on the presence of an initiator, and is hindered by oxygen, thus impeding the industrial scale-up of the GPEs production. In this work, an UV-mediated thiol-ene polymerization, employing polyethylene glycol diacrylate (PEGDA) as oligomer, was carried out in a liquid electrolyte solution (1 M LiTFSI in EC/DEC) to obtain a self-standing GPE. A comparative study between two different thiol-containing crosslinkers (trimethylolpropane tris(3-mercaptopropionate) - T3 and pentaerythritol tetrakis(3-mercaptopropionate) - T4) was carried out, studying the effects of the crosslinking environment and the GPE production methods on the cell performances. All the produced GPEs present an excellent room temperature ionic conductivity above 1 mS cm−1, as well as a wide electrochemical stability window up to 4.59 V. When cycled at a current density of C/10 for more than 250 cycles, all of the tested cells showed a stable cycling profile and a specific capacity >100 mAh g−1, indicating the suitability of such processes for up-scaling.
凝胶聚合物电解质(GPEs)在机械性能和电化学性能之间表现出最佳的折衷,并且在锂金属电池生产的框架中提高了电池的安全性。然而,通常采用的聚合机制依赖于引发剂的存在,并且受到氧气的阻碍,从而阻碍了gpe生产的工业规模扩大。在这项工作中,采用聚乙二醇二丙烯酸酯(PEGDA)作为低聚物,在液体电解质溶液(1 M LiTFSI In EC/DEC)中进行了紫外线介导的硫醇烯聚合,获得了独立的GPE。对三甲基丙烷三(3-巯基丙酸酯)- T3和季戊四醇四(3-巯基丙酸酯)- T4两种不同的含硫交联剂进行了比较研究,研究了交联环境和GPE生产方法对电池性能的影响。所有制备的gpe均具有优异的室温离子电导率,高于1 mS cm−1,以及高达4.59 V的宽电化学稳定窗口。当以C/10的电流密度循环超过250次时,所有测试的电池都显示出稳定的循环曲线和100 mAh g - 1的比容量,表明这种工艺适合扩大规模。
{"title":"Comparative Study of Photopolymerized Gel Polymer Electrolytes Obtained via Thiol-Ene Click Reaction for Li Metal Batteries","authors":"Mattia Longo, Matteo Gandolfo, Nuria Abigail Plebani, Cecilia Andrea Calderon, Matteo Destro, Daniela Fontana, Silvia Bodoardo, Julia Amici","doi":"10.1002/eem2.70028","DOIUrl":"https://doi.org/10.1002/eem2.70028","url":null,"abstract":"<p>Gel polymer electrolytes (GPEs) present the best compromise between mechanical and electrochemical properties, as well as an improvement of the cell safety in the framework of Li metal batteries production. However, the polymerization mechanism typically employed relies on the presence of an initiator, and is hindered by oxygen, thus impeding the industrial scale-up of the GPEs production. In this work, an UV-mediated thiol-ene polymerization, employing polyethylene glycol diacrylate (PEGDA) as oligomer, was carried out in a liquid electrolyte solution (1 M LiTFSI in EC/DEC) to obtain a self-standing GPE. A comparative study between two different thiol-containing crosslinkers (trimethylolpropane tris(3-mercaptopropionate) - T3 and pentaerythritol tetrakis(3-mercaptopropionate) - T4) was carried out, studying the effects of the crosslinking environment and the GPE production methods on the cell performances. All the produced GPEs present an excellent room temperature ionic conductivity above 1 mS cm<sup>−1</sup>, as well as a wide electrochemical stability window up to 4.59 V. When cycled at a current density of C/10 for more than 250 cycles, all of the tested cells showed a stable cycling profile and a specific capacity >100 mAh g<sup>−1</sup>, indicating the suitability of such processes for up-scaling.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70028","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774107","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}
Elastic strain constitutes a decisive factor in determining the recoverable deformability of thermoelectric materials. Plastic deformation for microstructure engineering has been demonstrated as a viable approach to enhance the elastic strain. However, this approach is highly dependent on the material's plasticity, which is rather limited by the rigidity for the majority of inorganic semiconducting thermoelectric materials. Thermocouple materials, as metallic thermoelectric materials, possess a favorable plasticity, motivating this work to focus on the elastic bendability of a metallic thermoelectric generator that is composed of K-type thermocouple components, namely p-type Ni90Cr10 and n-type Ni95Al2Mn2Si. The cold-rolling process enables a large elastic modulus and a high yield strength, thanks to the texturized direction along <111>, and dense dislocations and refined grains, respectively, eventually resulting in a 400% increase in the elastic strain. Such superior elasticity ensures the preservation of the initial transport properties for the rolled films even after being bent 100 000 times within a radius of ~8 mm. A power output of ~414 μW is achieved in a ten-leg flexible thermoelectric device, suggesting its substantial potential for powering wearable electronics.
{"title":"Texturization and Dense Dislocations Boost Elastic Bendability of Metallic Thermoelectric Generator","authors":"Xinyi Shen, Wenjun Ding, Zimin Fan, Erchao Meng, Wen Li, Yanzhong Pei","doi":"10.1002/eem2.70031","DOIUrl":"https://doi.org/10.1002/eem2.70031","url":null,"abstract":"<p>Elastic strain constitutes a decisive factor in determining the recoverable deformability of thermoelectric materials. Plastic deformation for microstructure engineering has been demonstrated as a viable approach to enhance the elastic strain. However, this approach is highly dependent on the material's plasticity, which is rather limited by the rigidity for the majority of inorganic semiconducting thermoelectric materials. Thermocouple materials, as metallic thermoelectric materials, possess a favorable plasticity, motivating this work to focus on the elastic bendability of a metallic thermoelectric generator that is composed of K-type thermocouple components, namely p-type Ni<sub>90</sub>Cr<sub>10</sub> and n-type Ni<sub>95</sub>Al<sub>2</sub>Mn<sub>2</sub>Si. The cold-rolling process enables a large elastic modulus and a high yield strength, thanks to the texturized direction along <111>, and dense dislocations and refined grains, respectively, eventually resulting in a 400% increase in the elastic strain. Such superior elasticity ensures the preservation of the initial transport properties for the rolled films even after being bent 100 000 times within a radius of ~8 mm. A power output of ~414 μW is achieved in a ten-leg flexible thermoelectric device, suggesting its substantial potential for powering wearable electronics.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70031","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144773971","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}
Jae-Moon Jeong, Jingyao Dai, Luiz Acauan, Kwang Il Jeong, Jeonyoon Lee, Carina Xiaochen Li, Hyunsoo Hong, Brian L. Wardle, Seong Su Kim
Bipolar plates (BPs) are essential multifunctional components in vanadium redox flow batteries (VRFBs) that require excellent electrical conductivity, low permeability, and strong solid support for the stack. However, conventional BPs are based on graphite sheets, which provide mechanical properties and corrosion resistance but have limitations in terms of electrical conductivity. Although carbon nanotubes (CNTs) have excellent properties, CNT composites with low CNT volume fractions (10–20%) have increased electrolyte permeability and limited electrical conductivity improvement, resulting in low durability and efficiency for VRFBs. This study proposes a novel concept of horizontally aligned CNT nanocomposite bipolar plate (HACN-BP) to address these issues. The HACN-BPs feature an optimized conduction path with a CNT volume fraction of 59%, resulting in reduced manufacturing time while demonstrating superior conductivity and permeability compared to conventional BPs. Furthermore, integrated HACN-BP mitigates ohmic loss that occurs in the BPs, thereby mitigating the potential drop by 40%. Therefore, the utilization of HACN-BP shows superior performance compared to recent studies, a substantial improvement of more than 6% in energy efficiency and 14% in capacity over conventional BP.
{"title":"Aligned Carbon Nanotube Polymer Nanocomposite Bipolar Plates Technology for Vanadium Redox Flow Batteries","authors":"Jae-Moon Jeong, Jingyao Dai, Luiz Acauan, Kwang Il Jeong, Jeonyoon Lee, Carina Xiaochen Li, Hyunsoo Hong, Brian L. Wardle, Seong Su Kim","doi":"10.1002/eem2.70030","DOIUrl":"https://doi.org/10.1002/eem2.70030","url":null,"abstract":"<p>Bipolar plates (BPs) are essential multifunctional components in vanadium redox flow batteries (VRFBs) that require excellent electrical conductivity, low permeability, and strong solid support for the stack. However, conventional BPs are based on graphite sheets, which provide mechanical properties and corrosion resistance but have limitations in terms of electrical conductivity. Although carbon nanotubes (CNTs) have excellent properties, CNT composites with low CNT volume fractions (10–20%) have increased electrolyte permeability and limited electrical conductivity improvement, resulting in low durability and efficiency for VRFBs. This study proposes a novel concept of horizontally aligned CNT nanocomposite bipolar plate (HACN-BP) to address these issues. The HACN-BPs feature an optimized conduction path with a CNT volume fraction of 59%, resulting in reduced manufacturing time while demonstrating superior conductivity and permeability compared to conventional BPs. Furthermore, integrated HACN-BP mitigates ohmic loss that occurs in the BPs, thereby mitigating the potential drop by 40%. Therefore, the utilization of HACN-BP shows superior performance compared to recent studies, a substantial improvement of more than 6% in energy efficiency and 14% in capacity over conventional BP.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"8 5","pages":""},"PeriodicalIF":14.1,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.70030","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144773970","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}