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Regulating the Mott–Hubbard Splitting for High-Performance Co-Free Li-Rich Mn-Based Oxide Cathode
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-02-16 DOI: 10.1002/adfm.202423843
Tianyu Wang, Ruoyu Wang, Jicheng Zhang, Guangxue Zhao, Wen Yin, Nian Zhang, Lirong Zheng, Xiangfeng Liu
Co-free Li-rich Mn-based layered oxides attract great attention as next-generation cathodes due to high specific capacity and low cost. However, their practical applications are hindered by the structural damage and poor cycling stability caused by the irreversible oxygen anion redox (OAR). Herein, a distinct strategy for regulating Mott–Hubbard splitting to address the detrimental issues is proposed. Introducing cations with specific electronic properties into the Li layer and transition metal (TM) layer decreases the Mott–Hubbard splitting energy (U) of TM cations, which promotes the electron removal and optimizes the band structure. This causes the antibonding band (M─O)* to rise and reduces its overlap with O2p band, thereby simultaneously enhancing the redox activity of TMs and the reversibility of OAR. The specific capacity, rate capability, and capacity retention are all significantly improved (255 mAh g−1 vs 223 mAh g−1 at 0.1C;197 mAh g−1 vs168 mAh g−1 at 1C;147 mAh g−1 vs115 mAh g−1 at 5 C; 93.2% vs 75.5% at 1C after 400 cycles). The oxygen release and voltage decay are also mitigated (92.4% vs 85.6% at 1C after 400 cycles). Moreover, a quantitative method to estimate U value is established for the first time. These findings provide insights into the intrinsic interaction mechanism of anions and cations redox and provide guidance for designing high-performance cathodes.
{"title":"Regulating the Mott–Hubbard Splitting for High-Performance Co-Free Li-Rich Mn-Based Oxide Cathode","authors":"Tianyu Wang, Ruoyu Wang, Jicheng Zhang, Guangxue Zhao, Wen Yin, Nian Zhang, Lirong Zheng, Xiangfeng Liu","doi":"10.1002/adfm.202423843","DOIUrl":"https://doi.org/10.1002/adfm.202423843","url":null,"abstract":"Co-free Li-rich Mn-based layered oxides attract great attention as next-generation cathodes due to high specific capacity and low cost. However, their practical applications are hindered by the structural damage and poor cycling stability caused by the irreversible oxygen anion redox (OAR). Herein, a distinct strategy for regulating Mott–Hubbard splitting to address the detrimental issues is proposed. Introducing cations with specific electronic properties into the Li layer and transition metal (TM) layer decreases the Mott–Hubbard splitting energy (U) of TM cations, which promotes the electron removal and optimizes the band structure. This causes the antibonding band (M─O)* to rise and reduces its overlap with O2p band, thereby simultaneously enhancing the redox activity of TMs and the reversibility of OAR. The specific capacity, rate capability, and capacity retention are all significantly improved (255 mAh g<sup>−1</sup> vs 223 mAh g<sup>−1</sup> at 0.1C;197 mAh g<sup>−1</sup> vs168 mAh g<sup>−1</sup> at 1C;147 mAh g<sup>−1</sup> vs115 mAh g<sup>−1</sup> at 5 C; 93.2% vs 75.5% at 1C after 400 cycles). The oxygen release and voltage decay are also mitigated (92.4% vs 85.6% at 1C after 400 cycles). Moreover, a quantitative method to estimate U value is established for the first time. These findings provide insights into the intrinsic interaction mechanism of anions and cations redox and provide guidance for designing high-performance cathodes.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"135 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418383","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}
引用次数: 0
Controllable Growth of Monocrystalline MoS2/Polycrystalline ReS2 Lateral Heterojunction for High Quantum Efficiency Photodetector
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-02-16 DOI: 10.1002/adfm.202421508
Jiaxi Li, Jinrong Chen, Yixun He, Jiaying Xiao, Guoqiang Li, Wenliang Wang
Photodetectors (PDs) based on 2D transition metal dichalcogenides (2D TMDCs) heterojunction have become a potential candidate for frontier technology applications such as visible light communication (VLC). However, the conventional 2D TMDCs heterojunction PDs are facing problems with excessive dark current and low photoelectric conversion efficiency, resulting in the performance of PDs not meeting application requirements. Herein, the controllable growth of monocrystalline MoS2/polycrystalline ReS2 lateral heterojunction via a two-step chemical vapor deposition (CVD) method has been proposed. According to the result of density functional theory (DFT) calculation and the characterization of multiple parallel experiments under different conditions, the controllable growth of lateral heterojunction, especially the competition mechanism between lateral epitaxy and vertical stacking is systematically analyzed from different perspectives. Based on the analysis above, a strategy for preparing monocrystalline MoS2/polycrystalline ReS2 lateral heterojunction with a large-scale epitaxy layer and a high-quality lateral structure is provided. Finally, PDs based on the as-grown lateral heterojunction with responsivity and external quantum efficiency (EQE) up to 2.65 A W−1 and 506% are successfully applied to the VLC demonstration. This work provides a potential approach for the design and fabrication of optoelectronic devices with the requirement of high responsivity and photoelectric conversion efficiency.
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引用次数: 0
A Dual-Mode Anode-Free Zinc-Prussian Blue Electrochromic Device 双模无阳极锌普鲁士蓝电致变色装置
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-02-16 DOI: 10.1002/adfm.202423532
Bingkun Huang, Bin Wang, Feifei Zhao, Haizeng Li, William W. Yu
Conventional Prussian blue (PB)-based electrochromic devices (ECDs) suffer from a narrow light modulation range due to their single absorption band. Herein, an anode-free Zn-PB electrochromic device is reported, utilizing a platinum (Pt) layer-modified ITO glass (denoted as Pt/ITO glass) counter electrode with a hybrid electrolyte containing propylene carbonate (PC). This device compensated for the charge released or consumed during the bleaching/coloring process of the PB electrode (i.e., ion-insertion/extraction) through a reversible Zn electrodeposition occurring on the surface of the Pt/ITO glass. The Pt layer ensured a uniformly distributed electric field across the electrode surface, leading to uniform Zn deposition. Concurrently, PC molecules modified the solvation structures of ions, engendering uniform Zn deposition and suppressing the “ion trapping” effect of PB. Meanwhile, PC suppressed water activity by changing the H-bonding network of electrolytes, thereby limiting the formation of by-products, the occurrence of side reactions, and the destruction of the PB structure. As a result, the optimized anode-free Zn-PB ECDs demonstrated high transmittance modulation ability (60.3% at 700 nm) and exceptional cycling durability (71.7% capacity retention and 69.1% of its initial ΔT after 1000 cycles). Finally, a dual-mode electrochromic device is developed with five color states to expand the light modulation range.
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引用次数: 0
Challenges and Strategies for Multi-Electron Reactions in High-Energy Phosphate-Based Cathodes for Sodium-Ion Batteries
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-02-16 DOI: 10.1002/adfm.202420864
Xiaoyin Zhang, Bin Lian, Hujun Shen, Shaoan Cheng, Fujun Li
Sodium-ion batteries (SIBs) have been considered as promising candidates for large-scale energy storage systems and low-speed electric vehicles due to abundant sodium resources and low cost. Phosphate-based cathodes stand out for their high voltages, structural stability, superior safety, etc. However, their large molecular weight limits the overall capacity, compromising the energy density for practical applications. Recent advancements in multi-electron reactions based on transition metal (TM) ions provide a promising pathway to achieve both high energy density and stability. This review discusses the fundamental principles behind the multi-electron reactions of phosphate-based cathodes from the perspectives of electrochemistry and materials science. The key factors, such as the conservation of matter and charge, thermodynamic, and kinetic feasibility, are addressed for activating and regulating the multi-electron reactions, aiming for a high capacity exceeding 170 mAh g−1. The current progress in NASICON-type phosphate cathodes is summarized, and the challenges associated with pyrophosphate and mixed phosphate cathodes are analyzed for multi-electron reactions. Finally, the perspectives on the future development of high-energy phosphate-based cathodes are provided.
{"title":"Challenges and Strategies for Multi-Electron Reactions in High-Energy Phosphate-Based Cathodes for Sodium-Ion Batteries","authors":"Xiaoyin Zhang, Bin Lian, Hujun Shen, Shaoan Cheng, Fujun Li","doi":"10.1002/adfm.202420864","DOIUrl":"https://doi.org/10.1002/adfm.202420864","url":null,"abstract":"Sodium-ion batteries (SIBs) have been considered as promising candidates for large-scale energy storage systems and low-speed electric vehicles due to abundant sodium resources and low cost. Phosphate-based cathodes stand out for their high voltages, structural stability, superior safety, etc. However, their large molecular weight limits the overall capacity, compromising the energy density for practical applications. Recent advancements in multi-electron reactions based on transition metal (TM) ions provide a promising pathway to achieve both high energy density and stability. This review discusses the fundamental principles behind the multi-electron reactions of phosphate-based cathodes from the perspectives of electrochemistry and materials science. The key factors, such as the conservation of matter and charge, thermodynamic, and kinetic feasibility, are addressed for activating and regulating the multi-electron reactions, aiming for a high capacity exceeding 170 mAh g<sup>−1</sup>. The current progress in NASICON-type phosphate cathodes is summarized, and the challenges associated with pyrophosphate and mixed phosphate cathodes are analyzed for multi-electron reactions. Finally, the perspectives on the future development of high-energy phosphate-based cathodes are provided.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"1 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418350","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}
引用次数: 0
Efficient Modulation d/p-Band Center Proximity in Birnessite-Type MnO2 by Cation/Anion Co-Doping for Enhanced Dual-Ion Storage
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-02-16 DOI: 10.1002/adfm.202500137
Yuhui Xu, Gaini Zhang, Xiaoxue Wang, Jianhua Zhang, Haocheng Wen, Dongniu Wang, Yitong Yuan, Qinting Jiang, Huaming Qian, Yukun Xi, Jiaxuan Zuo, Ming Li, Jihu Liu, Huijuan Yang, Yangyang Luo, Jingjing Wang, Wenbin Li, Xifei Li
The wide band gap of δ-MnO<sub>2</sub> and the restricted regulation of the p-band center (<span data-altimg="/cms/asset/b5e1bf62-68ee-4947-a794-bab592dd5611/adfm202500137-math-0001.png"></span><mjx-container ctxtmenu_counter="5" ctxtmenu_oldtabindex="1" jax="CHTML" role="application" sre-explorer- style="font-size: 103%; position: relative;" tabindex="0"><mjx-math aria-hidden="true" location="graphic/adfm202500137-math-0001.png"><mjx-semantics><mjx-mi data-semantic-annotation="clearspeak:simple" data-semantic-font="italic" data-semantic- data-semantic-role="greekletter" data-semantic-speech="epsilon" data-semantic-type="identifier"><mjx-c></mjx-c></mjx-mi></mjx-semantics></mjx-math><mjx-assistive-mml display="inline" unselectable="on"><math altimg="urn:x-wiley:1616301X:media:adfm202500137:adfm202500137-math-0001" display="inline" location="graphic/adfm202500137-math-0001.png" xmlns="http://www.w3.org/1998/Math/MathML"><semantics><mi data-semantic-="" data-semantic-annotation="clearspeak:simple" data-semantic-font="italic" data-semantic-role="greekletter" data-semantic-speech="epsilon" data-semantic-type="identifier">ε</mi>${varepsilon}$</annotation></semantics></math></mjx-assistive-mml></mjx-container><sub>p</sub>) of active oxygen atoms hinder electron conduction and ion diffusion during zinc storage. Heteroatom doping has proven effective in improving zinc storage. However, the regulation of <span data-altimg="/cms/asset/df89cc31-2889-4388-a779-01724ea6bce5/adfm202500137-math-0002.png"></span><mjx-container ctxtmenu_counter="6" ctxtmenu_oldtabindex="1" jax="CHTML" role="application" sre-explorer- style="font-size: 103%; position: relative;" tabindex="0"><mjx-math aria-hidden="true" location="graphic/adfm202500137-math-0002.png"><mjx-semantics><mjx-mi data-semantic-annotation="clearspeak:simple" data-semantic-font="italic" data-semantic- data-semantic-role="greekletter" data-semantic-speech="epsilon" data-semantic-type="identifier"><mjx-c></mjx-c></mjx-mi></mjx-semantics></mjx-math><mjx-assistive-mml display="inline" unselectable="on"><math altimg="urn:x-wiley:1616301X:media:adfm202500137:adfm202500137-math-0002" display="inline" location="graphic/adfm202500137-math-0002.png" xmlns="http://www.w3.org/1998/Math/MathML"><semantics><mi data-semantic-="" data-semantic-annotation="clearspeak:simple" data-semantic-font="italic" data-semantic-role="greekletter" data-semantic-speech="epsilon" data-semantic-type="identifier">ε</mi>${varepsilon}$</annotation></semantics></math></mjx-assistive-mml></mjx-container><sub>p</sub> solely through cation doping is comparatively constrained. Herein, a cation/anion co-doping strategy is proposed to simultaneously adjust the <span data-altimg="/cms/asset/fc49dfe1-0743-4baa-8432-a30900c9f157/adfm202500137-math-0003.png"></span><mjx-container ctxtmenu_counter="7" ctxtmenu_oldtabindex="1" jax="CHTML" role="application" sre-explorer- style="font-size: 103%; position: relative;" tabindex="0"><mjx-math aria-hidden="true
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引用次数: 0
Mom and Baby Wellness with a Smart Lactation Pad: A Wearable Sensor-Embedded Lactation Pad for on-Body Quantification of Glucose in Breast Milk
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-02-16 DOI: 10.1002/adfm.202420973
Abdulrahman Al-Shami, Haozheng Ma, Melissa Banks, Farbod Amirghasemi, Mona A Mohamed, Ali Soleimani, Sina Khazaee Nejad, Victor Ong, Alessandro Tasso, Alara Berkmen, Maral P. S. Mousavi
Wearable sensors are transforming healthcare by facilitating rapid, non-invasive, on-body biochemical analysis in biofluids such as sweat, tears, saliva, and blood, providing real-time insights into health conditions. Despite extensive academic and industrial efforts in developing wearable devices, very few are tailored to meet women's health needs. None are specifically designed for measurements in human breast milk. Beyond being the optimal source of infant nutrition, milk serves as a rich biofluid containing potential biomarkers reflecting a mother's health as well. Analyzing the composition of milk offers valuable information for the health of the infant, and the mother. This work pioneers a wearable sensor embedded in a lactation pad for on-body sampling of breast milk and continuous analysis of glucose levels in breast milk. Lactation pads are worn by most lactating individuals to absorb milk leakage during the day, and keep the cloth dry. In this work, by integrating microfluidic channels and electrochemical sensors in the lactation pad, milk sampling and analysis becomes part of an existing daily routine for the mother, posing no additional burden for milk sampling and analysis. The electrochemical sensors are developed using laser-induced carbonization of polyimide thin films, allowing for development of flexible, low-cost, and high-surface area electrodes. Glucose sensing is done via an enzymatic membrane composed of glucose oxidase, glutaraldehyde, bovine serum albumin, and Nafion to achieve enhanced enzyme protection and extended biosensor shelf life and operation in milk. Notably, the wearable device demonstrates high accuracy (96.8 to 104.1%) in measurement of glucose in whole undiluted human milk, collected 1st, 6th, and 12th months postpartum. This innovative smart lactation pad empowers mothers to track their babies' glucose intake and potentially identify early signs of health concerns.
可穿戴传感器可对汗液、泪液、唾液和血液等生物流体进行快速、无创、体外生化分析,实时了解健康状况,从而改变医疗保健。尽管学术界和工业界在开发可穿戴设备方面做出了大量努力,但专为满足女性健康需求而设计的设备却寥寥无几。没有一款是专门为测量母乳而设计的。母乳不仅是婴儿营养的最佳来源,还是一种丰富的生物流体,含有反映母亲健康状况的潜在生物标志物。分析母乳的成分可为婴儿和母亲的健康提供有价值的信息。这项研究首创了一种嵌入哺乳垫的可穿戴传感器,用于对母乳进行体外采样,并对母乳中的葡萄糖水平进行连续分析。大多数哺乳期妇女都会佩戴授乳垫,以吸收白天渗漏的乳汁,并保持布料干燥。在这项工作中,通过在哺乳垫中集成微流控通道和电化学传感器,母乳采样和分析成为母亲现有日常工作的一部分,不会给母乳采样和分析带来额外负担。电化学传感器是利用聚酰亚胺薄膜的激光诱导碳化技术开发的,从而实现了柔性、低成本和高表面积电极的开发。葡萄糖传感是通过由葡萄糖氧化酶、戊二醛、牛血清白蛋白和 Nafion 组成的酶膜实现的,以加强酶保护,延长生物传感器在牛奶中的保质期和工作时间。值得注意的是,该可穿戴设备在产后第 1、6 和 12 个月收集的未稀释母乳中测量葡萄糖的准确度很高(96.8% 至 104.1%)。这款创新型智能哺乳垫使母亲们能够跟踪婴儿的葡萄糖摄入量,并有可能发现健康问题的早期征兆。
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引用次数: 0
Advancing Organic Photovoltaics: the Role of Dipole Distance and Acidity in Perylene-Diimide Electron Transport Layers 推进有机光伏技术:过二亚胺电子传输层中偶极距离和酸度的作用
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-02-16 DOI: 10.1002/adfm.202420588
Wanqing Zhang, Xiaoman Ding, Jie Lv, Xiaokang Sun, Dingqin Hu, Guangye Zhang, Chuanlin Gao, Yizebang Xue, Yufei Zhong, Gang Li, Hanlin Hu
The electronic transport layer (ETL) based on perylene-diimide (PDI) has been widely demonstrated for efficient organic solar cells (OSCs). However, the effect of ETL materials on interfacial traps and energy losses remains understudied. This study investigates the effects of dipole distance on PDINN interface defects using three specifically designed weak acidic materials with varying carboxyl and hydroxyl group amounts. Among these, 3,5-dihydroxybenzoic acid (2OH), with moderate pH and high dipole distance, enhanced intermolecular forces with PDINN. This interaction boosted π–π stacking, enhanced ohmic contact with the active layer and Ag electrode. The P-2OH film exhibited a higher and more uniform potential distribution, suppressing charge recombination at the interface, reducing the trap density to 2.12 × 1016 cm3, and reducing the non-radiative loss ∆E3 from 0.236 to 0.174 eV. Consequently, the energy loss decreased from 0.553 to 0.484 meV for the PM6: BTP-ec9/P-2OH device. Notably, a decent PCE of 19.1% is achieved for P-2OH (10 nm), and it impressively remains a power conversion efficiency (PCE) of 16.4% when thickness of P-2OH up to 50 nm. This work underscores the importance of hydroxyl and carboxyl groups in regulating the ETL to minimize energy loss and offers insights for developing thickness-insensitive interlayers for high-performance OSCs.
基于过二亚胺(PDI)的电子传输层(ETL)已被广泛用于高效有机太阳能电池(OSC)。然而,ETL 材料对界面陷阱和能量损失的影响仍未得到充分研究。本研究使用三种专门设计的、羧基和羟基含量不同的弱酸性材料,研究偶极距离对 PDINN 界面缺陷的影响。其中,3,5-二羟基苯甲酸(2OH)具有适中的 pH 值和较高的偶极距离,可增强与 PDINN 的分子间作用力。这种相互作用促进了 π-π 堆叠,增强了与活性层和银电极的欧姆接触。P-2OH 薄膜显示出更高更均匀的电位分布,抑制了界面上的电荷重组,将陷阱密度降低到 2.12 × 1016 cm3,并将非辐射损耗 ∆E3 从 0.236 eV 降低到 0.174 eV。因此,PM6: BTP-ec9/P-2OH 器件的能量损失从 0.553 meV 降至 0.484 meV。值得注意的是,P-2OH(10 nm)的功率转换效率(PCE)达到了 19.1%,当 P-2OH 厚度达到 50 nm 时,功率转换效率(PCE)仍然高达 16.4%,令人印象深刻。这项研究强调了羟基和羧基在调节 ETL 以尽量减少能量损失方面的重要性,并为开发对厚度不敏感的高性能 OSC 夹层提供了启示。
{"title":"Advancing Organic Photovoltaics: the Role of Dipole Distance and Acidity in Perylene-Diimide Electron Transport Layers","authors":"Wanqing Zhang, Xiaoman Ding, Jie Lv, Xiaokang Sun, Dingqin Hu, Guangye Zhang, Chuanlin Gao, Yizebang Xue, Yufei Zhong, Gang Li, Hanlin Hu","doi":"10.1002/adfm.202420588","DOIUrl":"https://doi.org/10.1002/adfm.202420588","url":null,"abstract":"The electronic transport layer (ETL) based on perylene-diimide (PDI) has been widely demonstrated for efficient organic solar cells (OSCs). However, the effect of ETL materials on interfacial traps and energy losses remains understudied. This study investigates the effects of dipole distance on PDINN interface defects using three specifically designed weak acidic materials with varying carboxyl and hydroxyl group amounts. Among these, 3,5-dihydroxybenzoic acid (2OH), with moderate pH and high dipole distance, enhanced intermolecular forces with PDINN. This interaction boosted π–π stacking, enhanced ohmic contact with the active layer and Ag electrode. The P-2OH film exhibited a higher and more uniform potential distribution, suppressing charge recombination at the interface, reducing the trap density to 2.12 × 10<sup>16</sup> cm<sup>3</sup>, and reducing the non-radiative loss ∆E<sub>3</sub> from 0.236 to 0.174 eV. Consequently, the energy loss decreased from 0.553 to 0.484 meV for the PM6: BTP-ec9/P-2OH device. Notably, a decent PCE of 19.1% is achieved for P-2OH (10 nm), and it impressively remains a power conversion efficiency (PCE) of 16.4% when thickness of P-2OH up to 50 nm. This work underscores the importance of hydroxyl and carboxyl groups in regulating the ETL to minimize energy loss and offers insights for developing thickness-insensitive interlayers for high-performance OSCs.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"113 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143417958","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}
引用次数: 0
AI-Enabled Adaptive Eutectogel Skin for Effective Motion Monitoring with Low Signal Artifacts
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-02-16 DOI: 10.1002/adfm.202424965
Yexi Jin, Ruolin Wang, Dahong Tang, Yuhang Qian, Xingwen Zhou, Hao Shen, Jing Zhang, Yizhu Liu, Nan Wang, Baijie Cheng, Liguo Chen
Interfacial gel compliance is essential for the stable monitoring of physiological electrical signals. Current gel materials often fail to maintain stable operation at the skin interface, which is subject to constant change, due to an inadequate balance of viscoelastic properties. In this study, a dynamic adaptive gel network involving metal coordination with hierarchical hydrogen bonding is developed. The multilayered supramolecular structure has enabled the polymer chains to generate new physical entanglements upon dissociation. This dynamic cross-linking allows the eutectogel to sustain stable viscosity and elasticity across a broad frequency range (10−7–340 Hz). Furthermore, the metal-based eutectogel exhibits enhanced stretchability (1800%), good electrical conductivity (125 mS m−1), a wide operating temperature range (−70–100 °C), and strong interfacial adhesion. This adaptive eutectogel offers superior stability in the acquisition of electrical signals when compared with standard commercial gels. Viable application of the resultant strain sensors is demonstrated in human–machine interaction (HMI) and virtual reality (VR) haptic interaction. In addition, a convolutional neural network (CNN) algorithm is employed to develop an intelligent system for evaluating motion states using surface electromyography (sEMG) signals, achieving an accuracy of 94.1%.
界面凝胶顺应性对于稳定监测生理电信号至关重要。目前的凝胶材料由于粘弹性能平衡不足,往往无法在不断变化的皮肤界面保持稳定运行。本研究开发了一种动态自适应凝胶网络,涉及金属配位与分层氢键。多层超分子结构使聚合物链在解离时产生新的物理纠缠。这种动态交联使得共晶凝胶能够在较宽的频率范围(10-7-340 Hz)内保持稳定的粘度和弹性。此外,这种金属基共晶凝胶还具有更强的拉伸性(1800%)、良好的导电性(125 mS m-1)、更宽的工作温度范围(-70-100 °C)和更强的界面粘附性。与标准商用凝胶相比,这种自适应共晶凝胶在采集电信号时具有更高的稳定性。在人机交互(HMI)和虚拟现实(VR)触觉交互中展示了所产生的应变传感器的可行应用。此外,还采用卷积神经网络 (CNN) 算法开发了一个智能系统,利用表面肌电图 (sEMG) 信号评估运动状态,准确率达到 94.1%。
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引用次数: 0
In Situ Reconstruction and Anion Blocking Interphase Strategy for High-Performance Silicon-Based Anodes in Liquid and Solid-State Batteries 液态和固态电池中高性能硅基阳极的原位重构和阴离子阻断相间策略
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-02-16 DOI: 10.1002/adfm.202424137
Kun Tian, Wan Zhang, Jin Zeng, Yuanhao Gao, Xu Guang, Hao Luo, Mi Lu, Xiaodan Li
The silicon (Si) is one of the most promising anodes for next-generation lithium-ion batteries, but addressing the interfacial side reactions caused by volume expansion remains a key challenge. In this study, a composite of nano-Si with covered and interstitial LaF3 (Si@LaF3) is synthesized via a low-cost and scaleable ball milling process. Upon lithiation, the LaF3 layer on the nano-Si surface in situ reconstructs into an interface containing LiF and La. The LiF interface promotes the uniform formation of LiF-rich solid electrolyte interphase (SEI), and La grains can block the penetration of electrolyte anions into an electrode, inducing the stable and thin SEI on the Si@LaF3 anode. Additionally, the interstitial LaF3 particles facilitate the migration of Li+ into Si and reduce local expansion stress in the Si anode by alleviated electrochemical sintering. Compared to micron- and nano-Si anodes, the Si@LaF3 anode demonstrates higher specific capacity and superior cycling stability. The Si@LaF3||-LiFePO4 full battery retains a specific capacity of 125.1 mAh g−1 after 200 cycles at 0.35 C, while the Si@LaF3/graphite anode in all-solid-state battery maintains a capacity of 491 mAh g−1 after 100 cycles at 0.1 A g−1. This study provides new insights on the commercialization of Si-based anodes and solid-state batteries.
{"title":"In Situ Reconstruction and Anion Blocking Interphase Strategy for High-Performance Silicon-Based Anodes in Liquid and Solid-State Batteries","authors":"Kun Tian, Wan Zhang, Jin Zeng, Yuanhao Gao, Xu Guang, Hao Luo, Mi Lu, Xiaodan Li","doi":"10.1002/adfm.202424137","DOIUrl":"https://doi.org/10.1002/adfm.202424137","url":null,"abstract":"The silicon (Si) is one of the most promising anodes for next-generation lithium-ion batteries, but addressing the interfacial side reactions caused by volume expansion remains a key challenge. In this study, a composite of nano-Si with covered and interstitial LaF<sub>3</sub> (Si@LaF<sub>3</sub>) is synthesized via a low-cost and scaleable ball milling process. Upon lithiation, the LaF<sub>3</sub> layer on the nano-Si surface in situ reconstructs into an interface containing LiF and La. The LiF interface promotes the uniform formation of LiF-rich solid electrolyte interphase (SEI), and La grains can block the penetration of electrolyte anions into an electrode, inducing the stable and thin SEI on the Si@LaF<sub>3</sub> anode. Additionally, the interstitial LaF<sub>3</sub> particles facilitate the migration of Li<sup>+</sup> into Si and reduce local expansion stress in the Si anode by alleviated electrochemical sintering. Compared to micron- and nano-Si anodes, the Si@LaF<sub>3</sub> anode demonstrates higher specific capacity and superior cycling stability. The Si@LaF<sub>3</sub>||-LiFePO<sub>4</sub> full battery retains a specific capacity of 125.1 mAh g<sup>−1</sup> after 200 cycles at 0.35 C, while the Si@LaF<sub>3</sub>/graphite anode in all-solid-state battery maintains a capacity of 491 mAh g<sup>−1</sup> after 100 cycles at 0.1 A g<sup>−1</sup>. This study provides new insights on the commercialization of Si-based anodes and solid-state batteries.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"11 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418397","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}
引用次数: 0
Effect of Strain Rate on Phase Transition and Microstructural Evolution in Ferroelectric PMN-PT Single Crystals Through Nanoindentation
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-02-16 DOI: 10.1002/adfm.202425763
Guian Man, Yixuan Jiang, Xingzhe Wang
Controlling domain switching and phase transitions in ferroelectric materials under external fields is crucial for advanced device applications. However, the mechanism and kinetics governing mechanically induced phase transitions in relaxor ferroelectric Pb(Mg1/3Nb2/3)O3-PbTiO3 remain some unclear understanding, especially under variable strain rates. To investigate this, localized mechanical stress is applied using nanoindentation to PMN-PT single crystals. With the aid of Raman spectroscopy and high-resolution transmission electron microscopy, irreversible phase transition pathways from the Rhombohedral to Tetragonal phase (R→T) are identified. The variation is also observed in the phase transition behavior with the strain rate during nanoindentation. Interestingly, the coexistence of the R and T phases within the indentation region suggests that an uneven force application via nanoindentation can induce morphotropic phase boundaries (MPBs). Further assessments of the phase-transformation dynamics are conducted using the phase-field method, which simulated the domain evolution process in PMN-PT under various indentation strain rates. These findings provide new insights into how mechanical forces can modulate the microstructural evolution within relaxor ferroelectric materials, enhancing the understanding of this fascinating phenomenon.
{"title":"Effect of Strain Rate on Phase Transition and Microstructural Evolution in Ferroelectric PMN-PT Single Crystals Through Nanoindentation","authors":"Guian Man, Yixuan Jiang, Xingzhe Wang","doi":"10.1002/adfm.202425763","DOIUrl":"https://doi.org/10.1002/adfm.202425763","url":null,"abstract":"Controlling domain switching and phase transitions in ferroelectric materials under external fields is crucial for advanced device applications. However, the mechanism and kinetics governing mechanically induced phase transitions in relaxor ferroelectric Pb(Mg<sub>1/3</sub>Nb<sub>2/3</sub>)O<sub>3</sub>-PbTiO<sub>3</sub> remain some unclear understanding, especially under variable strain rates. To investigate this, localized mechanical stress is applied using nanoindentation to PMN-PT single crystals. With the aid of Raman spectroscopy and high-resolution transmission electron microscopy, irreversible phase transition pathways from the Rhombohedral to Tetragonal phase (R→T) are identified. The variation is also observed in the phase transition behavior with the strain rate during nanoindentation. Interestingly, the coexistence of the R and T phases within the indentation region suggests that an uneven force application via nanoindentation can induce morphotropic phase boundaries (MPBs). Further assessments of the phase-transformation dynamics are conducted using the phase-field method, which simulated the domain evolution process in PMN-PT under various indentation strain rates. These findings provide new insights into how mechanical forces can modulate the microstructural evolution within relaxor ferroelectric materials, enhancing the understanding of this fascinating phenomenon.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"80 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143417964","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}
引用次数: 0
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Advanced Functional Materials
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