Tao Sun, Meng Qi, Qing-Xiu Li, Hang-Fei Li, Zhi-Peng Feng, Run-Ze Xu, You Zhou, Yu Wen, Gui-Jun Li, Ye Zhou, Su-Ting Han
Gait is among the most dependable, accurate, and secure methods of biometric identification. However, high power consumption and low computing capability are two major obstacles on wearable sensors-based gait recognition system. In this work, an integrated system is reported combining a triboelectric nanogenerator (TENG), a memristor (Ag/HfOx/Pt), and perovskite-based multicolor LEDs (PMCLED) for the visualization and recognition of foot patterns through signal-on-none and multi-wavelength on-device preprocessing. The flexible TENG acts as a sensory receptor, generating voltage based on the duration and intensity of pressure, which in turn promotes voltage-triggered synaptic plasticity in the memristor. The PMCLED, with its threshold switching and multi-wavelength emission characteristics, enables nonlinear filtering and amplification of the synaptic signal from the memristor, resulting in a simplified system design and reduced background noise. Additionally, the effectiveness of on-device preprocessing is validated based on a 5 × 5 array of integrated devices and software-built neural network for foot pattern visualization and recognition. The proposed system is able to recognize the on-device preprocessed images with high accuracy, indicating great potentials in both healthcare monitoring and human-machine interaction.
步态是最可靠、准确和安全的生物识别方法之一。然而，高功耗和低计算能力是基于可穿戴传感器的步态识别系统的两大障碍。在这项工作中，报告了一种集成系统，该系统结合了三电纳米发电机（TENG）、忆阻器（Ag/HfOx/Pt）和基于过氧化物的多色发光二极管（PMCLED），通过无信号和多波长设备预处理实现脚型的可视化和识别。柔性 TENG 可充当感觉受体，根据压力的持续时间和强度产生电压，进而促进忆阻器中电压触发的突触可塑性。PMCLED 具有阈值开关和多波长发射特性，能够对来自忆阻器的突触信号进行非线性过滤和放大，从而简化了系统设计并降低了背景噪声。此外，基于 5 × 5 集成器件阵列和用于脚型可视化和识别的软件内置神经网络，验证了器件上预处理的有效性。所提议的系统能够高精度地识别设备上预处理的图像，这表明该系统在医疗保健监测和人机交互方面具有巨大潜力。
{"title":"Integration of Sensory Memory Process Display System for Gait Recognition","authors":"Tao Sun, Meng Qi, Qing-Xiu Li, Hang-Fei Li, Zhi-Peng Feng, Run-Ze Xu, You Zhou, Yu Wen, Gui-Jun Li, Ye Zhou, Su-Ting Han","doi":"10.1002/adfm.202416619","DOIUrl":"https://doi.org/10.1002/adfm.202416619","url":null,"abstract":"Gait is among the most dependable, accurate, and secure methods of biometric identification. However, high power consumption and low computing capability are two major obstacles on wearable sensors-based gait recognition system. In this work, an integrated system is reported combining a triboelectric nanogenerator (TENG), a memristor (Ag/HfO<sub>x</sub>/Pt), and perovskite-based multicolor LEDs (PMCLED) for the visualization and recognition of foot patterns through signal-on-none and multi-wavelength on-device preprocessing. The flexible TENG acts as a sensory receptor, generating voltage based on the duration and intensity of pressure, which in turn promotes voltage-triggered synaptic plasticity in the memristor. The PMCLED, with its threshold switching and multi-wavelength emission characteristics, enables nonlinear filtering and amplification of the synaptic signal from the memristor, resulting in a simplified system design and reduced background noise. Additionally, the effectiveness of on-device preprocessing is validated based on a 5 × 5 array of integrated devices and software-built neural network for foot pattern visualization and recognition. The proposed system is able to recognize the on-device preprocessed images with high accuracy, indicating great potentials in both healthcare monitoring and human-machine interaction.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665574","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}
Stimuli-responsive materials have been applied for sensor devices because they can transform and amplify various target stimuli into observable signals. Much effort has been devoted to exploring effective molecular designs for obtaining stimuli-responsive behaviors by taking advantage of the unique optoelectronic properties of π-conjugated molecules involving various elements. This study focuses on the modulation of the electronic state of the π-conjugated scaffolds by the oxidation number change of the hypervalent antimony. This study demonstrate that the strength of the intramolecular interaction between hypervalent antimony and the π-conjugated framework can be tuned with ligand structure, substituent effect, and oxidation number shifts of hypervalent antimony. In particular, the color changes represented by hypsochromic and bathochromic wavelength shifts of optical bands are achieved by the oxidative reaction of hypervalent antimony in the solid state. Significantly, the direction of the color changes can be confidently predicted by quantum chemical calculations. The findings, based on the electronic interaction between π-conjugated scaffolds and hypervalent main-group elements, provide logical design strategies for advanced stimuli-responsive materials.
{"title":"Stimuli-Responsive Optical Materials Based on Hypervalent Antimony-Containing Conjugated Molecules","authors":"Kazuya Tanimura, Masayuki Gon, Kazuo Tanaka, Yoshiki Chujo","doi":"10.1002/adfm.202418600","DOIUrl":"https://doi.org/10.1002/adfm.202418600","url":null,"abstract":"Stimuli-responsive materials have been applied for sensor devices because they can transform and amplify various target stimuli into observable signals. Much effort has been devoted to exploring effective molecular designs for obtaining stimuli-responsive behaviors by taking advantage of the unique optoelectronic properties of π-conjugated molecules involving various elements. This study focuses on the modulation of the electronic state of the π-conjugated scaffolds by the oxidation number change of the hypervalent antimony. This study demonstrate that the strength of the intramolecular interaction between hypervalent antimony and the π-conjugated framework can be tuned with ligand structure, substituent effect, and oxidation number shifts of hypervalent antimony. In particular, the color changes represented by hypsochromic and bathochromic wavelength shifts of optical bands are achieved by the oxidative reaction of hypervalent antimony in the solid state. Significantly, the direction of the color changes can be confidently predicted by quantum chemical calculations. The findings, based on the electronic interaction between π-conjugated scaffolds and hypervalent main-group elements, provide logical design strategies for advanced stimuli-responsive materials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"50 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665390","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}
Kun Yu, Huichao Ji, Guangli Ye, Liangjie Fu, Xiongbo Dong, Huaming Yang
Reactive oxygen species (ROS) have been growing as an emerging “hot” topic in antimicrobial applications. However, optimizing antimicrobial activity by enhancing ROS generation remains a formidable challenge. Here, using bassanite as a proof of concept, the facet engineering of bassanite matrix can enhance the ROS generation efficiency via tuning the d-band center of Cu atom is proposed. Theoretical calculation and experimental investigations reveal that the d-band center of Cu atoms is significantly shifted upward when Cu doped into the (204) facet of bassanite compared to the (400) facet. A higher d-band center facilitates adsorption and activation between Cu and O2 through the formation of stronger d-π* orbital hybridization, resulting in increased ROS production. Through engineering, the material exhibits better antimicrobial activity when Cu doped into the (204) facet, which presents a clear potential in construction materials and personal protection. This work shed light on designing new materials with high antimicrobial activity and the application of facet engineering.
活性氧（ROS）已逐渐成为抗菌应用中的一个新兴 "热门 "话题。然而，通过增强 ROS 生成来优化抗菌活性仍然是一项艰巨的挑战。在此，我们以巴桑石为概念验证，提出了通过调整铜原子的 d 波段中心来提高 ROS 生成效率的巴桑石基体刻面工程。理论计算和实验研究表明，与（400）面相比，当铜掺杂到巴山石的（204）面时，铜原子的 d 带中心会明显上移。更高的 d 带中心通过形成更强的 d-π* 轨道杂化，促进了 Cu 和 O2 之间的吸附和活化，从而增加了 ROS 的产生。通过工程设计，当 Cu 掺杂到 (204) 面时，该材料表现出更好的抗菌活性，在建筑材料和个人防护方面具有明显的潜力。这项工作为设计具有高抗菌活性的新材料以及面工程的应用提供了启示。
{"title":"Facet Engineering Modulates d-π* Hybridization for Boosting Antimicrobial Activity","authors":"Kun Yu, Huichao Ji, Guangli Ye, Liangjie Fu, Xiongbo Dong, Huaming Yang","doi":"10.1002/adfm.202418440","DOIUrl":"https://doi.org/10.1002/adfm.202418440","url":null,"abstract":"Reactive oxygen species (ROS) have been growing as an emerging “hot” topic in antimicrobial applications. However, optimizing antimicrobial activity by enhancing ROS generation remains a formidable challenge. Here, using bassanite as a proof of concept, the facet engineering of bassanite matrix can enhance the ROS generation efficiency via tuning the <i>d</i>-band center of Cu atom is proposed. Theoretical calculation and experimental investigations reveal that the <i>d</i>-band center of Cu atoms is significantly shifted upward when Cu doped into the (204) facet of bassanite compared to the (400) facet. A higher <i>d</i>-band center facilitates adsorption and activation between Cu and O<sub>2</sub> through the formation of stronger <i>d</i>-<i>π<sup>*</sup></i> orbital hybridization, resulting in increased ROS production. Through engineering, the material exhibits better antimicrobial activity when Cu doped into the (204) facet, which presents a clear potential in construction materials and personal protection. This work shed light on designing new materials with high antimicrobial activity and the application of facet engineering.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"18 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665391","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}
Wen Ye, Meng Li, Guixiang Li, Lihua Jiang, Shun Tian, Shihong Dong, Qingfeng Xu, Dongyun Chen, Mohammad Khaja Nazeeruddin, Paul J. Dyson, Antonio Abate, Jian-Mei Lu
Solution-processed lead-free halide perovskite gas sensors possess low gas detection limits, offering promising alternatives to traditional metal oxide chemiresistors. However, halide perovskite chemiresistors often suffer from poor selectivity and durability due to a lack of coordinatively unsaturated surface metal ions and their sensitivity to humidity. To address these issues, a general strategy is presented in which the Cs2PdBr6 perovskite surface is coated with covalent organic framework (COF) to provide hybrid sensor materials that are highly sensitive to specific gases and demonstrate excellent stability under real-working conditions. The hybrid chemiresistors demonstrate high sensitivity and controllable selectivity toward NO2 or NH3 gases. Specifically, TAPB–PDA@Cs2PdBr6 achieves a detection limit of 10 ppb for NO2, the lowest value reported for a perovskite-based gas sensor, maintaining its performance after continuous exposure to ambient air for several weeks. In contrast, COF-5@Cs2PdBr6 shows high selectivity to NH3 and has a detection limit of 40 ppb. Structural and spectroscopic characterization combined with mechanistic studies provide molecular-level insights into the outstanding properties of these new hybrid sensor materials, which set a new benchmark in the field, i.e., surpassing the selectivity and sensitivity of conventional halide perovskite sensors.
{"title":"Covalent Organic Framework-Enhanced Metal Halide Perovskites for Selective and Sensitive Gas Sensing","authors":"Wen Ye, Meng Li, Guixiang Li, Lihua Jiang, Shun Tian, Shihong Dong, Qingfeng Xu, Dongyun Chen, Mohammad Khaja Nazeeruddin, Paul J. Dyson, Antonio Abate, Jian-Mei Lu","doi":"10.1002/adfm.202418897","DOIUrl":"https://doi.org/10.1002/adfm.202418897","url":null,"abstract":"Solution-processed lead-free halide perovskite gas sensors possess low gas detection limits, offering promising alternatives to traditional metal oxide chemiresistors. However, halide perovskite chemiresistors often suffer from poor selectivity and durability due to a lack of coordinatively unsaturated surface metal ions and their sensitivity to humidity. To address these issues, a general strategy is presented in which the Cs<sub>2</sub>PdBr<sub>6</sub> perovskite surface is coated with covalent organic framework (COF) to provide hybrid sensor materials that are highly sensitive to specific gases and demonstrate excellent stability under real-working conditions. The hybrid chemiresistors demonstrate high sensitivity and controllable selectivity toward NO<sub>2</sub> or NH<sub>3</sub> gases. Specifically, TAPB–PDA@Cs<sub>2</sub>PdBr<sub>6</sub> achieves a detection limit of 10 ppb for NO<sub>2</sub>, the lowest value reported for a perovskite-based gas sensor, maintaining its performance after continuous exposure to ambient air for several weeks. In contrast, COF-5@Cs<sub>2</sub>PdBr<sub>6</sub> shows high selectivity to NH<sub>3</sub> and has a detection limit of 40 ppb. Structural and spectroscopic characterization combined with mechanistic studies provide molecular-level insights into the outstanding properties of these new hybrid sensor materials, which set a new benchmark in the field, i.e., surpassing the selectivity and sensitivity of conventional halide perovskite sensors.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"21 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665389","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}
Yuhong Cui, Guoliang Ru, Tianyi Zhang, Ke Yang, Shujuan Liu, Weihong Qi, Qian Ye, Xuqing Liu, Feng Zhou
With the rapid advancement of wearable electronics, soft robotics, and camouflage technologies, there is an urgent demand for flexible, multifunctional electromagnetic wave absorbing materials. Traditional absorbers, including metal- and carbon-based materials, often lack the flexibility required for such applications. In this work, a novel strategy is proposed for developing a flexible absorber by combining a conductive filler with a Schottky heterogeneous interface and a polymer network framework. Ti3C2Tx MXene is modified with ZnS via a low-temperature hydrothermal method, forming a Ti3C2Tx/ZnS composite. This composite is subsequently embedded in a copolymer matrix of polyvinyl alcohol (PVA) and acrylamide (AAm), dispersed in a binary water-glycerol solution. The Schottky interface between Ti3C2Tx and ZnS enhances electron transfer at the heterophase boundary, significantly improving interface polarisation. Simultaneously, interactions between water and glycerol restrict the rotation of polar molecules under external electromagnetic fields, optimising polarisation loss within the gel. Experimental results demonstrate that the Ti3C2Tx/ZnS gel achieves a minimum reflection loss (RLmin) of −43.76 dB at 8.79 GHz, with an effective absorption bandwidth (EAB) covering the entire X-band. Additionally, the gel exhibit exceptional stretchability, frost resistance, shape adaptability, and photothermal conversion properties.
{"title":"Schottky Interface Engineering in Ti3C2Tx/ZnS Organic Hydrogels for High-Performance Multifunctional Flexible Absorbers","authors":"Yuhong Cui, Guoliang Ru, Tianyi Zhang, Ke Yang, Shujuan Liu, Weihong Qi, Qian Ye, Xuqing Liu, Feng Zhou","doi":"10.1002/adfm.202417346","DOIUrl":"https://doi.org/10.1002/adfm.202417346","url":null,"abstract":"With the rapid advancement of wearable electronics, soft robotics, and camouflage technologies, there is an urgent demand for flexible, multifunctional electromagnetic wave absorbing materials. Traditional absorbers, including metal- and carbon-based materials, often lack the flexibility required for such applications. In this work, a novel strategy is proposed for developing a flexible absorber by combining a conductive filler with a Schottky heterogeneous interface and a polymer network framework. Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> MXene is modified with ZnS via a low-temperature hydrothermal method, forming a Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/ZnS composite. This composite is subsequently embedded in a copolymer matrix of polyvinyl alcohol (PVA) and acrylamide (AAm), dispersed in a binary water-glycerol solution. The Schottky interface between Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> and ZnS enhances electron transfer at the heterophase boundary, significantly improving interface polarisation. Simultaneously, interactions between water and glycerol restrict the rotation of polar molecules under external electromagnetic fields, optimising polarisation loss within the gel. Experimental results demonstrate that the Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub>/ZnS gel achieves a minimum reflection loss (RL<sub>min</sub>) of −43.76 dB at 8.79 GHz, with an effective absorption bandwidth (EAB) covering the entire X-band. Additionally, the gel exhibit exceptional stretchability, frost resistance, shape adaptability, and photothermal conversion properties.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665392","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}
Gabriele Greco, Benjamin Schmuck, Vincenzo Fazio, Giuseppe Puglisi, Giuseppe Florio, Nicola Maria Pugno, Luca Fambri, Anna Rising
Silk-based materials are sought after across various industries due to their remarkable properties, including high strength and flexibility. However, their practical application depends largely on how well these properties are maintained under different environmental conditions. Despite significant advancements in the large-scale production of artificial silk fibers, the effects of temperature on their mechanical behavior are understudied. In this study, the mechanical properties of artificial spider silk fibers between −80 and +120 °C are examined and compared to both synthetic and natural silk fibers. The findings reveal that artificial silk fibers maintain their strength up to +120 °C, though the strain at break slightly decreases, remaining above 60%. At −80 °C, the fibers exhibit increased strength, but the strain at break is reduced. While these artificial fibers closely mimic the behavior of natural silk, they show a noticeable reduction in extensibility at low temperatures. Complementing experimental data, differential scanning calorimetry, and thermogravimetric analysis are also conducted, proposing a simple physical model to explain the observed temperature-induced softening. Encouragingly, the degradation temperature of artificial silk is comparable to that of native silkworm and spider silk. This study underscores the importance of enhancing the mechanical robustness of artificial silk to expand its applications.
蚕丝基材料具有高强度和柔韧性等显著特性，因此受到各行各业的追捧。然而，它们的实际应用在很大程度上取决于在不同环境条件下如何保持这些特性。尽管在大规模生产人造丝纤维方面取得了重大进展，但温度对其机械行为的影响仍未得到充分研究。本研究考察了人造蜘蛛丝纤维在 -80 至 +120 °C 之间的机械性能，并将其与合成纤维和天然纤维进行了比较。研究结果表明，人造蛛丝纤维在 +120 °C 时仍能保持强度，但断裂应变略有下降，仍保持在 60% 以上。在-80 °C时，纤维强度增加，但断裂应变降低。虽然这些人造纤维与天然丝的行为非常相似，但它们在低温下的延展性明显下降。为补充实验数据，还进行了差示扫描量热法和热重分析，提出了一个简单的物理模型来解释观察到的温度诱导软化现象。令人鼓舞的是，人造丝的降解温度与本地蚕丝和蜘蛛丝的降解温度相当。这项研究强调了提高人造丝机械坚固性以扩大其应用的重要性。
{"title":"Temperature-Induced Effects on Wet-Spun Artificial Spider Silk Fibers","authors":"Gabriele Greco, Benjamin Schmuck, Vincenzo Fazio, Giuseppe Puglisi, Giuseppe Florio, Nicola Maria Pugno, Luca Fambri, Anna Rising","doi":"10.1002/adfm.202418435","DOIUrl":"https://doi.org/10.1002/adfm.202418435","url":null,"abstract":"Silk-based materials are sought after across various industries due to their remarkable properties, including high strength and flexibility. However, their practical application depends largely on how well these properties are maintained under different environmental conditions. Despite significant advancements in the large-scale production of artificial silk fibers, the effects of temperature on their mechanical behavior are understudied. In this study, the mechanical properties of artificial spider silk fibers between −80 and +120 °C are examined and compared to both synthetic and natural silk fibers. The findings reveal that artificial silk fibers maintain their strength up to +120 °C, though the strain at break slightly decreases, remaining above 60%. At −80 °C, the fibers exhibit increased strength, but the strain at break is reduced. While these artificial fibers closely mimic the behavior of natural silk, they show a noticeable reduction in extensibility at low temperatures. Complementing experimental data, differential scanning calorimetry, and thermogravimetric analysis are also conducted, proposing a simple physical model to explain the observed temperature-induced softening. Encouragingly, the degradation temperature of artificial silk is comparable to that of native silkworm and spider silk. This study underscores the importance of enhancing the mechanical robustness of artificial silk to expand its applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"107 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665575","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}
The key issue in utilizing solid polymer electrolytes for high-energy-density lithium metal batteries is to balance the conflicting demands of superior processability, adequate ionic conductivity, and mechanical stability. Inspired by molecular structure design, a metal-organic framework-derived polyether poly(urethane urea) solid polymer electrolyte (denoted as ePU@H SPE) has been synthesized via a facile polycondensation method involving covalent crosslinking. The reduced crystallinity and numerous polar groups in ePU@H SPEs enhance Li salt dissociation and create efficient Li+ ion diffusion channels, yielding remarkable ionic conductivity (1.48 × 10−4 S cm−1). The polymer backbones, incorporating covalent bonds and dynamic hydrogen bonds, provide superb mechanical strength (5.12 GPa), high toughness (1240%), and excellent resilience, which suppress lithium dendrite growth and buffer electrode volume fluctuations during cycling. Leveraging these attributes, the well-designed ePU@H SPE enables ultra-high durability in lithium plating/stripping over 2300 h. Moreover, the integrated LFP|ePU@H|Li batteries, generating delicate electrode/electrolyte interfacial contact, deliver an exceptionally long lifespan (86% retention over 500 cycles at 1 C). Moreover, the LFP|ePU@H|Li pouch cell operates reliably even under severe deformation and external damage. Impressively, the stable cycling performance of full batteries incorporating high-voltage LCO and high-capacity S cathodes further verifies the significant potential of advanced ePU@H SPEs for practical applications.
利用固体聚合物电解质制造高能量密度锂金属电池的关键问题是如何平衡出色的加工性、足够的离子导电性和机械稳定性这三者之间的矛盾。受分子结构设计的启发，我们通过共价交联的简便缩聚法合成了一种源自金属有机框架的聚醚聚（氨基脲）固体聚合物电解质（简称 ePU@H SPE）。ePU@H 固态聚合物电解质的结晶度降低，且含有大量极性基团，这增强了锂盐的解离，并形成了高效的锂离子扩散通道，从而产生了显著的离子电导率（1.48 × 10-4 S cm-1）。聚合物骨架包含共价键和动态氢键，具有超强的机械强度（5.12 GPa）、高韧性（1240%）和出色的回弹性，可抑制锂枝晶的生长和缓冲电极在循环过程中的体积波动。此外，集成的 LFP|ePU@H|Li 电池可产生微妙的电极/电解质界面接触，具有超长的使用寿命（在 1 C 温度下循环 500 次，保持率为 86%）。此外，LFP|ePU@H|锂袋式电池即使在严重变形和外部损坏的情况下也能可靠运行。令人印象深刻的是，包含高电压 LCO 和高容量 S 阴极的全电池的稳定循环性能进一步验证了先进 ePU@H SPE 在实际应用中的巨大潜力。
{"title":"Metal-Organic Framework-Derived Elastic Solid Polymer Electrolytes Enabled by Covalent Crosslinking for High-Performance Lithium Metal Batteries","authors":"Sha Li, Fei Pei, Yu Ding, Xiangyang Guo, Xiaoping Zhang, Hongwei Tao, Zhengyou He, Haitao Hu, Li Zhang","doi":"10.1002/adfm.202415495","DOIUrl":"https://doi.org/10.1002/adfm.202415495","url":null,"abstract":"The key issue in utilizing solid polymer electrolytes for high-energy-density lithium metal batteries is to balance the conflicting demands of superior processability, adequate ionic conductivity, and mechanical stability. Inspired by molecular structure design, a metal-organic framework-derived polyether poly(urethane urea) solid polymer electrolyte (denoted as ePU@H SPE) has been synthesized via a facile polycondensation method involving covalent crosslinking. The reduced crystallinity and numerous polar groups in ePU@H SPEs enhance Li salt dissociation and create efficient Li<sup>+</sup> ion diffusion channels, yielding remarkable ionic conductivity (1.48 × 10<sup>−4</sup> S cm<sup>−1</sup>). The polymer backbones, incorporating covalent bonds and dynamic hydrogen bonds, provide superb mechanical strength (5.12 GPa), high toughness (1240%), and excellent resilience, which suppress lithium dendrite growth and buffer electrode volume fluctuations during cycling. Leveraging these attributes, the well-designed ePU@H SPE enables ultra-high durability in lithium plating/stripping over 2300 h. Moreover, the integrated LFP|ePU@H|Li batteries, generating delicate electrode/electrolyte interfacial contact, deliver an exceptionally long lifespan (86% retention over 500 cycles at 1 C). Moreover, the LFP|ePU@H|Li pouch cell operates reliably even under severe deformation and external damage. Impressively, the stable cycling performance of full batteries incorporating high-voltage LCO and high-capacity S cathodes further verifies the significant potential of advanced ePU@H SPEs for practical applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"32 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665576","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}
HakSu Jang, Gwang Hyeon Kim, Dong Won Jeon, Hyeon Jun Park, BitNa Bae, Nagamalleswara Rao Alluri, Cheol Min Kim, Changyeon Baek, Min-Ku Lee, Sung Beom Cho, Gyoung-Ja Lee, Kwi-Il Park
Flexibility, higher piezoelectric performance, and long-lasting stability of devices have a great demand in next generation energy technologies. Polyvinylidene fluoride (PVDF) polymer has a greater mechanical flexibility, but it suffers from low piezoelectric performance. Herein, sandwich-structured piezoelectric film (SS-PF) is designed by inserting the conductive poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) layer between two PVDF layers. The SS-PF based flexible piezoelectric energy harvester (f-PEH) generates higher voltage and current of 3.73 times and 4.64 times than the pristine PVDF film type f-PEH. Moreover, the SS-PF based f-PEH shows no degradation in the output voltage confirming the excellent long-lasting stability over 6 months. DFT simulation shows the occurrence of intermolecular forces between the PVDF/PEDOT:PSS interface. The electric field-dependent charges alignment in PEDOT:PSS may induce the charge accumulation at the PSS-PVDF interface and charge depletion at the PEDOT-PVDF interface leading to the change in orientation of molecular structure in PVDF. Next, the SS-PF based f-PEH is tested for a vibration sensor to monitor the vibrations of curvy pipes and machines, and its output voltages are comparable with the commercial PVDF vibration sensor to confirm the real-time use. The results present a novel design strategy, indicating a new direction for investigating piezo-polymer-based f-PEH.
{"title":"Long-Lasting, Steady and Enhanced Energy Harvesting by Inserting a Conductive Layer into the Piezoelectric Polymer","authors":"HakSu Jang, Gwang Hyeon Kim, Dong Won Jeon, Hyeon Jun Park, BitNa Bae, Nagamalleswara Rao Alluri, Cheol Min Kim, Changyeon Baek, Min-Ku Lee, Sung Beom Cho, Gyoung-Ja Lee, Kwi-Il Park","doi":"10.1002/adfm.202415501","DOIUrl":"https://doi.org/10.1002/adfm.202415501","url":null,"abstract":"Flexibility, higher piezoelectric performance, and long-lasting stability of devices have a great demand in next generation energy technologies. Polyvinylidene fluoride (PVDF) polymer has a greater mechanical flexibility, but it suffers from low piezoelectric performance. Herein, sandwich-structured piezoelectric film (SS-PF) is designed by inserting the conductive poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) layer between two PVDF layers. The SS-PF based flexible piezoelectric energy harvester (f-PEH) generates higher voltage and current of 3.73 times and 4.64 times than the pristine PVDF film type f-PEH. Moreover, the SS-PF based f-PEH shows no degradation in the output voltage confirming the excellent long-lasting stability over 6 months. DFT simulation shows the occurrence of intermolecular forces between the PVDF/PEDOT:PSS interface. The electric field-dependent charges alignment in PEDOT:PSS may induce the charge accumulation at the PSS-PVDF interface and charge depletion at the PEDOT-PVDF interface leading to the change in orientation of molecular structure in PVDF. Next, the SS-PF based f-PEH is tested for a vibration sensor to monitor the vibrations of curvy pipes and machines, and its output voltages are comparable with the commercial PVDF vibration sensor to confirm the real-time use. The results present a novel design strategy, indicating a new direction for investigating piezo-polymer-based f-PEH.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665344","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}
Debasmita Sarkar, Ufuoma I. Kara, Rajan Singh, Anirban Phukan, Priyam Mondal, Roy P. Paily, Xiaoguang Wang, Uttam Manna
Individuals suffering from voice disabilities have limited access to currently available automation technologies that operate through voice commands. To address this issue, an alternative voice recognition approach is essential without directly monitoring the audio signals generated from the vocal cord. In this work, the design of a chemically reactive and conductive sponge is reported to create an underwater vibration sensor with a fast response time and high sensitivity, through orthogonal modulation of conductivity (40–2150 kΩ), water repellence (0°–154°) and mechanical properties (0.32–2.63 MPa). This class of porous sponge sensors enables the identification of subtle water waves generated at the air–water interface and extends its utility to detecting a variety of locomotion (squatting, jumping, walking, etc.), as well as automated voice recognition using a deep learning model without direct contact with the human body. Overall, this underwater vibration sensor provides a novel basis for remote interaction with automated technologies, which finds use in medical diagnostics, human-machine interfaces, and underwater communication systems.
{"title":"Underwater Vibration Sensor to Enable Automated and Contactless Voice Recognition","authors":"Debasmita Sarkar, Ufuoma I. Kara, Rajan Singh, Anirban Phukan, Priyam Mondal, Roy P. Paily, Xiaoguang Wang, Uttam Manna","doi":"10.1002/adfm.202419049","DOIUrl":"https://doi.org/10.1002/adfm.202419049","url":null,"abstract":"Individuals suffering from voice disabilities have limited access to currently available automation technologies that operate through voice commands. To address this issue, an alternative voice recognition approach is essential without directly monitoring the audio signals generated from the vocal cord. In this work, the design of a chemically reactive and conductive sponge is reported to create an underwater vibration sensor with a fast response time and high sensitivity, through orthogonal modulation of conductivity (40–2150 kΩ), water repellence (0°–154°) and mechanical properties (0.32–2.63 MPa). This class of porous sponge sensors enables the identification of subtle water waves generated at the air–water interface and extends its utility to detecting a variety of locomotion (squatting, jumping, walking, etc.), as well as automated voice recognition using a deep learning model without direct contact with the human body. Overall, this underwater vibration sensor provides a novel basis for remote interaction with automated technologies, which finds use in medical diagnostics, human-machine interfaces, and underwater communication systems.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"30 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642834","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}
Chang Min Lee, Yonghee Kim, Woojo Kim, Eunho Lee, Eun Kwang Lee
Organic electrochemical transistors (OECTs) represent a promising approach for flexible, wearable, biomedical electronics, and sensors integrated with diverse substrates. Their ability to operate at low voltages and interact effectively with biological systems makes them particularly suitable for neuromorphic applications. For neuromorphic devices, OECTs must enhance electrical performance, biocompatibility, and signal storage/erasure capabilities. While UV cross‐linking methods with various side effects on organic semiconductors are predominant in improving mobility and current retention time, thermal cross‐linking based on the solution process has not been extensively explored. Additionally, despite significant research on the modification of electrolyte property, the ionic charge compensation mechanisms between multiple electrolytes are still unclear. This study employs a cross‐linking strategy involving the chemical reaction of poly(3‐hexylthiophene‐2,5‐diyl) (P3HT) with di‐tert‐butyl‐peroxide (DTBP) to create a cross‐linked P3HT active layer. Furthermore, a dual ion gel structure combining a conventional ion gel with a chitosan‐based ion gel is investigated for increased ionic transport to enhance OECT performance. Using the above two methods, the enhanced electrical performance showing the mobility of 25 F cm−1 V−1 s−1 and synaptic properties showing long‐term plasticity of cross‐linked OECTs with a dual ion gel structure are demonstrated, suggesting their potential application as high‐performance neuromorphic devices.
{"title":"High‐Performance Synaptic Devices Based on Cross‐linked Organic Electrochemical Transistors with Dual Ion Gel","authors":"Chang Min Lee, Yonghee Kim, Woojo Kim, Eunho Lee, Eun Kwang Lee","doi":"10.1002/adfm.202417539","DOIUrl":"https://doi.org/10.1002/adfm.202417539","url":null,"abstract":"Organic electrochemical transistors (OECTs) represent a promising approach for flexible, wearable, biomedical electronics, and sensors integrated with diverse substrates. Their ability to operate at low voltages and interact effectively with biological systems makes them particularly suitable for neuromorphic applications. For neuromorphic devices, OECTs must enhance electrical performance, biocompatibility, and signal storage/erasure capabilities. While UV cross‐linking methods with various side effects on organic semiconductors are predominant in improving mobility and current retention time, thermal cross‐linking based on the solution process has not been extensively explored. Additionally, despite significant research on the modification of electrolyte property, the ionic charge compensation mechanisms between multiple electrolytes are still unclear. This study employs a cross‐linking strategy involving the chemical reaction of poly(3‐hexylthiophene‐2,5‐diyl) (P3HT) with di‐tert‐butyl‐peroxide (DTBP) to create a cross‐linked P3HT active layer. Furthermore, a dual ion gel structure combining a conventional ion gel with a chitosan‐based ion gel is investigated for increased ionic transport to enhance OECT performance. Using the above two methods, the enhanced electrical performance showing the mobility of 25 F cm<jats:sup>−1</jats:sup> V<jats:sup>−1</jats:sup> s<jats:sup>−1</jats:sup> and synaptic properties showing long‐term plasticity of cross‐linked OECTs with a dual ion gel structure are demonstrated, suggesting their potential application as high‐performance neuromorphic devices.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"247 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642891","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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