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Polyfunctional eutectogels with multiple hydrogen-bond-shielded amorphous networks for soft ionotronics 用于软离子电子学的具有多重氢键屏蔽非晶网络的多官能团共晶凝胶
IF 17.3 2区 医学 Q2 CHEMISTRY, MEDICINAL Pub Date : 2024-11-06 DOI: 10.1016/j.matt.2024.09.009
Yizhe Shao , Chao Dang , Haobo Qi , Ziyang Liu , Haoran Pei , Tongqing Lu , Wei Zhai
Eutectogels, consisting of three-dimensional polymeric networks saturated with deep eutectic solvents (DESs), present a promising option for soft ionic conductors. Instead of modifying polymer chains, we propose a new DES system comprising phytic acid (PA) and choline chloride (ChCl), which enhances dynamic and interactive bonding with polymeric networks to create innovative eutectogels. Here, we develop polyfunctional eutectogels (PETGs) by encapsulating polyvinyl alcohol (PVA) networks with our DES using an evaporation-induced confinement strategy. Experimental validation and numerical calculations demonstrate that PA forms high-density dynamic hydrogen bonds with PVA while shielding hydrogen bonds between PVA chains. This results in a multiple hydrogen-bond-shielded amorphous network (MHSN) with undetectable crystalline regions, thereby promoting ion migration to ensure high conductivity. Moreover, our PETG exhibits rapid self-healing, freeze resistance, self-adhesion, antibacterial properties, and dual sensitivities attributable to the MHSN. We demonstrate the potential of PETGs for applications in motion sensing, machine learning, human-machine interaction, and energy harvesting.
共晶凝胶由饱和深共晶溶剂(DES)的三维聚合物网络组成,是一种前景广阔的软离子导体。我们提出了一种由植酸(PA)和氯化胆碱(ChCl)组成的新型 DES 系统,而不是对聚合物链进行改性,它能增强与聚合物网络的动态互动结合,从而创造出创新的共晶凝胶。在这里,我们采用蒸发诱导限制策略,将聚乙烯醇(PVA)网络与我们的 DES 一起封装,从而开发出多功能共晶凝胶(PETGs)。实验验证和数值计算表明,聚酰胺与 PVA 形成了高密度的动态氢键,同时屏蔽了 PVA 链之间的氢键。这就形成了一个无法检测到结晶区域的多重氢键屏蔽无定形网络(MHSN),从而促进了离子迁移,确保了高导电性。此外,由于 MHSN 的存在,我们的 PETG 还具有快速自愈合、抗冻性、自粘性、抗菌性和双重敏感性。我们展示了 PETG 在运动传感、机器学习、人机交互和能量收集方面的应用潜力。
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引用次数: 0
Three-terminal quantum dot light-emitting synapse with active adaptive photoelectric outputs for complex image processing/parallel computing 具有主动自适应光电输出的三端量子点发光突触,用于复杂图像处理/并行计算
IF 17.3 2区 医学 Q2 CHEMISTRY, MEDICINAL Pub Date : 2024-11-06 DOI: 10.1016/j.matt.2024.06.050
Cong Chen , Zhenjia Chen , Di Liu , Xianghong Zhang , Changsong Gao , Liuting Shan , Lujian Liu , Tianjian Chen , Tailiang Guo , Huipeng Chen
Machine vision enables machines to extract rich information from image or video data and make intelligent decisions. However, approaches using artificial synapse hardware systems significantly limit the real-time and accuracy in machine vision segmentation amid complex environments. Addressing this, we propose a novel three-terminal adaptive artificial-light-emitting synapse (AALS) capable of photoelectric double output along with adaptive behavior. The device uses silver nanowires (AgNWs) as polar conductive bridges to reduce reliance on transparent electrodes, while polyvinyl alcohol (PVA) dielectric layers adaptively modulate charge carrier concentrations in conductive channels. Additionally, we have designed an adaptive parallel neural network (APNN) and applied it to autonomous driving image processing. This innovation significantly reduces adaptation time and notably enhances mean pixel accuracy (MPA) for semantic segmentation under overexposure and low-light conditions by 142.2% and 304.4%, respectively. Therefore, this work introduces new strategies for advanced adaptive vision, promising significant potential in intelligent driving and neuromorphic computing.
机器视觉使机器能够从图像或视频数据中提取丰富的信息并做出智能决策。然而,使用人工突触硬件系统的方法大大限制了复杂环境中机器视觉分割的实时性和准确性。针对这一问题,我们提出了一种新型三端自适应人工发光突触(AALS),该突触具有光电双输出和自适应行为。该装置使用银纳米线(AgNWs)作为极性导电桥,以减少对透明电极的依赖,而聚乙烯醇(PVA)电介质层可自适应调节导电通道中的电荷载流子浓度。此外,我们还设计了一种自适应并行神经网络(APNN),并将其应用于自动驾驶图像处理。这一创新大大缩短了适应时间,并显著提高了过曝和弱光条件下语义分割的平均像素精度(MPA),分别提高了 142.2% 和 304.4%。因此,这项工作为先进的自适应视觉引入了新策略,有望在智能驾驶和神经形态计算领域大显身手。
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引用次数: 0
Thermodynamic origin of nonvolatility in resistive memory 电阻式存储器非挥发性的热力学起源
IF 17.3 2区 医学 Q2 CHEMISTRY, MEDICINAL Pub Date : 2024-11-06 DOI: 10.1016/j.matt.2024.07.018
Jingxian Li , Anirudh Appachar , Sabrina L. Peczonczyk , Elisa T. Harrison , Anton V. Ievlev , Ryan Hood , Dongjae Shin , Sangmin Yoo , Brianna Roest , Kai Sun , Karsten Beckmann , Olya Popova , Tony Chiang , William S. Wahby , Robin B. Jacobs-Godrim , Matthew J. Marinella , Petro Maksymovych , John T. Heron , Nathaniel Cady , Wei D. Lu , Yiyang Li
Electronic switches based on the migration of high-density point defects, or memristors, are poised to revolutionize post-digital electronics. Despite significant research, key mechanisms for filament formation and oxygen transport remain unresolved, hindering our ability to predict and design device properties. For example, experiments have achieved 10 orders of magnitude longer retention times than predicted by current models. Here, using electrical measurements, scanning probe microscopy, and first-principles calculations on tantalum oxide memristors, we reveal that the formation and stability of conductive filaments crucially depend on the thermodynamic stability of the amorphous oxygen-rich and oxygen-poor compounds, which undergo composition phase separation. Including the previously neglected effects of this amorphous phase separation reconciles unexplained discrepancies in retention and enables predictive design of key performance indicators such as retention stability. This result emphasizes non-ideal thermodynamic interactions as key design criteria in post-digital devices with defect densities substantially exceeding those of today’s covalent semiconductors.
基于高密度点缺陷迁移的电子开关(或称忆阻器)有望彻底改变后数字电子技术。尽管开展了大量研究,但灯丝形成和氧气传输的关键机制仍未得到解决,这阻碍了我们预测和设计器件特性的能力。例如,实验所获得的保留时间比现有模型预测的时间长 10 个数量级。在这里,我们利用电学测量、扫描探针显微镜和对氧化钽忆阻器的第一原理计算,揭示了导电丝的形成和稳定性在很大程度上取决于非晶态富氧和贫氧化合物的热力学稳定性,它们会发生成分相分离。将以前被忽视的这种非晶相分离的影响包括在内,可以调和无法解释的保留差异,并实现对保留稳定性等关键性能指标的预测性设计。这一结果强调,在缺陷密度大大超过当今共价半导体的后数字设备中,非理想热力学相互作用是关键的设计标准。
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引用次数: 0
Dual robust electrode-electrolyte interfaces enabled by fluorinated electrolyte for high-performance zinc metal batteries 氟化电解质为高性能锌金属电池提供了坚固的电极-电解质双界面
IF 17.3 2区 医学 Q2 CHEMISTRY, MEDICINAL Pub Date : 2024-11-06 DOI: 10.1016/j.matt.2024.08.002
Xun Guo , Hu Hong , Qing Li , Jiaxiong Zhu , Zhuoxi Wu , Yanbo Wang , Shuo Yang , Zhaodong Huang , Yan Huang , Nan Li , Chunyi Zhi
Rechargeable zinc metal batteries (ZMBs) are promising for fabricating low-cost, safe, and high-energy-density storage systems. However, ZMBs typically undergo interfacial side reactions and cathode dissolution during cycling, resulting in the depletion of active materials and performance decay of batteries. Here, we develop a localized high-concentration fluorinated electrolyte featuring a high fluorine/oxygen atomic ratio (388.72%) with beneficial solvation chemistry, fostering the simultaneous formation of a cathode-electrolyte interphase (CEI) enriched with C–F bonds and a ZnF2-dominant solid-electrolyte interphase (SEI). The constructed robust electrode-electrolyte interfaces (EEIs) contribute to dendrite-free zinc deposition and a highly stable cathode, demonstrating soft-packed Zn||Mn-doped V2O5 batteries with an exceptional energy density (91.25 Wh kg−1cathode+anode) and capacity retention (90.5%) over 500 cycles employing a limited zinc supply. The anode-free ZMBs deliver a record power density of 153.9 Wh kg−1cathode+anode with a high capacity retention of 80.2% over 1,500 cycles. This research provides significant insights for interface construction in multivalent ion batteries.
可充电锌金属电池(ZMB)在制造低成本、安全和高能量密度存储系统方面前景广阔。然而,锌金属电池在循环过程中通常会发生界面副反应和阴极溶解,导致活性材料耗竭和电池性能下降。在这里,我们开发了一种局部高浓度含氟电解质,它具有高氟/氧原子比(388.72%)和有利的溶解化学性质,可同时形成富含 C-F 键的阴极-电解质相(CEI)和以 ZnF2 为主导的固态-电解质相(SEI)。所构建的坚固电极-电解质界面(EEIs)有助于实现无枝晶锌沉积和高度稳定的阴极,在使用有限锌供应的 500 次循环过程中,展示了能量密度(91.25 Wh kg-1(阴极+阳极))和容量保持率(90.5%)极高的软包装锌||锰掺杂 V2O5 电池。无阳极 ZMB 的功率密度达到创纪录的 153.9 Wh kg-1(阴极+阳极),在 1,500 次循环中的容量保持率高达 80.2%。这项研究为多价离子电池的界面构造提供了重要启示。
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引用次数: 0
Emulsions that store oxygen for fast ORR kinetics and multifunctional robotic and mobility systems 用于快速 ORR 动力学和多功能机器人与移动系统的储氧乳液
IF 17.3 2区 医学 Q2 CHEMISTRY, MEDICINAL Pub Date : 2024-11-06 DOI: 10.1016/j.matt.2024.08.010
Alissa C. Johnson , Alice S. Fontaine , Emily A. Beeman , William J. Townsend , James H. Pikul
Human circulatory systems store large concentrations of oxygen and provide it continuously and simultaneously to trillions of cells without the need for each cell to access the surrounding environment. Inspired by biological circulatory systems, we envision future robotic systems with multifunctional, fully integrated, air-rechargeable energy delivery and storage. We present an aqueous air catholyte emulsion (ACE) with high oxygen solubility that can derive energy entirely from dissolved oxygen. With only 20% silicone oil by volume, ACEs can store twice as much dissolved oxygen (15 mg/L) as pure KOH samples, remain stable for several months, and show superior oxygen reduction reaction kinetics compared to KOH. Zinc-air flow cells with fully submerged electrodes can achieve 4.6 mW/cm2 at 5.6 mA/cm2. A multifunctional actuator flow cell configuration employs an ACE as both a hydraulic actuator and an energy storage fluid, demonstrating the feasibility of ACEs as multifunctional, flexible power sources for soft robotic systems.
人体循环系统可储存高浓度的氧气,并持续、同步地向数以万亿计的细胞提供氧气,而每个细胞都无需接触周围环境。受生物循环系统的启发,我们设想未来的机器人系统将具备多功能、完全集成、可充电的空气能量输送和储存系统。我们提出了一种具有高氧气溶解度的水性空气阴离子乳液(ACE),它可以完全从溶解氧中获取能量。与纯 KOH 样品相比,ACE 的硅油含量仅为 20%,其溶解氧储存量是纯 KOH 样品的两倍(15 毫克/升),可保持稳定数月,并显示出更优越的氧还原反应动力学。完全浸没电极的锌-空气流动池可以在 5.6 mA/cm2 的条件下达到 4.6 mW/cm2。一种多功能致动器流动电池配置将 ACE 同时用作液压致动器和储能流体,证明了 ACE 作为软机器人系统多功能、灵活电源的可行性。
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引用次数: 0
Manipulating cation-anion coordination in fire-retardant electrolytes to enable high-areal-capacity fluoride conversion batteries 操纵阻燃电解质中的阳离子-阴离子配位,实现高铝容量氟化物转换电池
IF 17.3 2区 医学 Q2 CHEMISTRY, MEDICINAL Pub Date : 2024-11-06 DOI: 10.1016/j.matt.2024.07.007
Keyi Chen , Wujie Qiu , Meng Lei , Chuanzhong Lai , Jianjun Liu , Chilin Li
Resource-abundant and multi-redox iron fluorides are considered promising cathodes for large-scale battery systems. However, existing research often overlooks the critical issues at the fluoride-electrolyte interface that cause voltage plateau blurring and capacity degradation. Here, we propose an interfacial engineering strategy for the conversion-type FeF3 cathode enabled by manipulating the cation-anion coordination in a fire-retardant electrolyte. Lithium difluoro(oxalato)borate has strong electron affinity and induces an anion-rich inner solvation sheath, thereby dominating the construction of the cathode-electrolyte interphase (CEI). The inorganic-enriched CEI layer features electron insulation and facile mass transport, which could suppress interfacial parasitic reactions and promote fluoride structural reversibility. The Li-FeF3 cell enables well-preserved voltage plateaus and a high capacity of 412 mAh g−1 with inspiring cycle durability. The superior electrolyte wettability further contributes to a reversible areal capacity as high as 2.94 mAh cm−2 for fluoride cathode under high FeF3 mass loading of ∼7.0 mg cm−2 and lean electrolyte conditions.
资源丰富的多氧化还原氟化铁被认为是有希望用于大规模电池系统的阴极。然而,现有研究往往忽视了氟化物-电解质界面的关键问题,这些问题会导致电压高原模糊和容量下降。在此,我们提出了一种界面工程策略,通过操纵阻燃电解质中阳离子与阴离子的配位,实现转换型 FeF3 阴极。二氟(草酸)硼酸锂具有很强的电子亲和性,能诱导出富含阴离子的内部溶解鞘,从而主导阴极-电解质间相 (CEI) 的构建。富含无机物的 CEI 层具有电子绝缘和易于质量传输的特点,可抑制界面寄生反应并促进氟化物结构的可逆性。锂-铁-FeF3 电池能很好地保留电压高原,并具有 412 mAh g-1 的高容量和令人振奋的循环耐久性。优越的电解质润湿性进一步促进了氟化阴极在 FeF3 质量负荷为 7.0 mg cm-2 和贫电解质条件下的可逆面积容量高达 2.94 mAh cm-2。
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引用次数: 0
Finding value in rarity: Cerium in MOFs and perovskites 从稀有中寻找价值:MOFs 和过氧化物中的铈
IF 17.3 2区 医学 Q2 CHEMISTRY, MEDICINAL Pub Date : 2024-11-06 DOI: 10.1016/j.matt.2024.09.025
Steve Cranford
Rare earth elements (REEs) are crucial components in nearly all modern electronics. Two recent manuscripts utilize cerium as the key element in two diverse applications (catalysis and optoelectronics) integrated within two diverse emerging materials science platforms (MOFs and perovskites). Such studies pave the way for more exploratory investigations across REEs.
稀土元素 (REE) 是几乎所有现代电子产品的关键成分。最近的两篇手稿将铈作为关键元素应用于两个不同的应用领域(催化和光电子学),并将其整合到两个不同的新兴材料科学平台(MOFs 和过氧化物)中。这些研究为对各种稀土元素进行更多探索性研究铺平了道路。
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引用次数: 0
The interactions between halide perovskites and oxygen: From stages to strategies 卤化物过氧化物与氧气之间的相互作用:从阶段到战略
IF 17.3 2区 医学 Q2 CHEMISTRY, MEDICINAL Pub Date : 2024-11-06 DOI: 10.1016/j.matt.2024.08.007
Yangyang Ju , Xiangmin Hu , Xian-gang Wu , Chenhui Wang , Alexander Baranov , Anatoly Pushkarev , Haizheng Zhong
Metal halide perovskites (MHPs) face stability challenges particularly due to their susceptibility to oxygen exposure, hindering their practical applications. Unraveling the complicated photophysical and photochemical behaviors of MHPs in the presence of oxygen is essential to overcome this obstacle. To address this critical issue, we aim to integrate the recent findings and elucidate the dynamics of perovskite-oxygen interactions. The interactions between MHPs and oxygen are clarified in four fundamental stages: adsorption on the surface, surface reactions, diffusion of reactive oxygen species (1O2, O2, O22−), and bulk reactions. We try to provide a comprehensive and nuanced understanding of these interactions, emphasizing the underlying mechanisms governing charge and energy transfers. Within this framework, we particularly discuss the pronounced vulnerability of tin (Sn)-based perovskites to oxygen and analyze the distinct factors that amplify this susceptibility. Following this, we summarize the impact of oxygen exposure on the photoelectric performance of MHPs and outline potential strategies to mitigate superoxide-mediated degradation pathways. Gaining a deeper understanding of the perovskite-oxygen interaction can offer valuable insights for material optimization and device design, ultimately enhancing stability against oxygen exposure.
金属卤化物过氧化物(MHPs)面临着稳定性方面的挑战,特别是由于它们容易受到氧气的影响,从而阻碍了它们的实际应用。要克服这一障碍,就必须揭示 MHPs 在氧气存在下复杂的光物理和光化学行为。为了解决这一关键问题,我们旨在整合近期的研究成果,阐明包晶与氧相互作用的动力学。我们从四个基本阶段阐明了 MHP 与氧的相互作用:表面吸附、表面反应、活性氧(1O2、O2-、O22-)的扩散以及块体反应。我们试图提供对这些相互作用的全面而细致的理解,强调电荷和能量转移的基本机制。在这一框架内,我们特别讨论了锡(Sn)基过氧化物对氧气的明显脆弱性,并分析了放大这种易感性的不同因素。随后,我们总结了氧气暴露对 MHP 光电性能的影响,并概述了减轻超氧化物介导的降解途径的潜在策略。更深入地了解包晶石与氧的相互作用,可以为材料优化和器件设计提供宝贵的见解,最终提高抗氧暴露的稳定性。
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引用次数: 0
Innate immunity-modulating nanobiomaterials for controlling inflammation resolution 用于控制炎症消退的先天免疫调节纳米生物材料
IF 17.3 2区 医学 Q2 CHEMISTRY, MEDICINAL Pub Date : 2024-11-06 DOI: 10.1016/j.matt.2024.09.016
Yongjiang Li , Wei Chen , Seyoung Koo , Haijun Liu , Qimanguli Saiding , Angel Xie , Na Kong , Yihai Cao , Reza Abdi , Charles N. Serhan , Wei Tao
The acute inflammatory response is an inherent protective mechanism, and its unsuccessful resolution can contribute to disease pathogenesis and potentially lead to death. Innate immune cells are the first line of host defenders and play a substantial role in inflammation initiation, amplification, resolution, or subsequent disease progression. As the resolution of inflammation is an active and highly regulated process, modulating innate immune cells, including neutrophils, monocytes and macrophages, and endothelial cells, and their interactions offer opportunities to control excessive inflammation. Nanobiomaterials have shown superior therapeutic potential in inflammation-related diseases by manipulating inflammatory responses because nanobiomaterials can target and interact with innate immune cells. Versatile nanobiomaterials can be designed for targeted modulation of specific innate immune responses. Nanopro-resolving medicines have been prepared both with pro-resolving lipid mediators and peptides, each demonstrating active resolution of inflammation in animal disease models. Here, we review innovative nanobiomaterials for modulating innate immunity and alleviating inflammation. We summarize strategies combining the design of nanobiomaterials with the nano-bio interaction for modulating innate immune profiles and propelling the advancement of nanobiomaterials for inflammatory disease treatments. We also propose the future perspectives and translational challenges of nanobiomaterials that need to be overcome in this swiftly rising field.
急性炎症反应是一种固有的保护机制,如果不能成功解决,就会导致疾病的发病,并有可能导致死亡。先天性免疫细胞是宿主的第一道防线,在炎症的引发、扩大、缓解或随后的疾病进展中发挥着重要作用。由于炎症的消退是一个活跃和高度调节的过程,因此调节先天性免疫细胞(包括中性粒细胞、单核细胞和巨噬细胞以及内皮细胞)及其相互作用为控制过度炎症提供了机会。由于纳米生物材料可以靶向先天性免疫细胞并与之相互作用,因此纳米生物材料在通过操纵炎症反应治疗炎症相关疾病方面显示出卓越的治疗潜力。多功能纳米生物材料的设计可以有针对性地调节特定的先天性免疫反应。目前已经制备出了具有促进溶解脂质介质和肽的纳米溶解药物,每种药物都在动物疾病模型中显示出了积极的炎症溶解作用。在此,我们回顾了用于调节先天免疫和缓解炎症的创新纳米生物材料。我们总结了将纳米生物材料的设计与纳米生物相互作用相结合的策略,以调节先天性免疫特征,推动纳米生物材料在炎症性疾病治疗方面的进步。我们还提出了纳米生物材料的未来展望和在这一迅速崛起的领域需要克服的转化挑战。
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引用次数: 0
Early and high-throughput plant diagnostics: strategies for disease detection. 早期和高通量植物诊断:病害检测战略。
IF 17.3 2区 医学 Q2 CHEMISTRY, MEDICINAL Pub Date : 2024-11-06 DOI: 10.1016/j.tplants.2024.10.003
Abdullah Bukhamsin, Jürgen Kosel, Matthew F McCabe, Ikram Blilou, Khaled N Salama

The rising global occurrence of plant pathogens highlights the need for a thorough reassessment of current disease detection and management schemes. To that end, we review the utility and limitations of the available sensing platforms deployed for phytodiagnostics in the field. We also discuss recent advances in the use of broad-spectrum biomarkers such as phytohormones and volatile organic compounds (VOCs), and assess the feasibility of deploying these platforms on a large scale. Because these platforms are often complementary, we propose a compressed sensing approach that combines several sensing platforms to manage plant pathogens while minimizing additional costs. Finally, we provide an outlook for the potential benefits of integrating new sensing technologies into farming for timely interventions.

植物病原体在全球的发生率不断上升,这凸显了对当前病害检测和管理方案进行彻底重新评估的必要性。为此,我们回顾了实地用于植物诊断的现有传感平台的实用性和局限性。我们还讨论了使用植物激素和挥发性有机化合物 (VOC) 等广谱生物标记物的最新进展,并评估了大规模部署这些平台的可行性。由于这些平台通常是互补的,因此我们提出了一种压缩传感方法,将多个传感平台结合起来,在管理植物病原体的同时最大限度地降低额外成本。最后,我们展望了将新传感技术融入农业生产以进行及时干预的潜在益处。
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引用次数: 0
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ACS Infectious Diseases
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