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Coupling Solvation Structure Regulation and Interface Engineering via Reverse Micelle Strategy Toward Highly Stable Zn Metal Anode 通过反向胶束策略将溶解结构调控与界面工程相结合,实现高稳定性锌金属阳极
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1002/adfm.202417695
Hui Peng, Danyang Wang, Xin Wang, Wenxing Miao, Jingtian Zeng, Bo Tao, Yue Li, Ying Tang, Guofu Ma
The stability of aqueous Z inc (Zn) ion energy storage devices is significantly compromised by the instability at the electrode/electrolyte interface, which can result in the growth of Zn dendrites, self‐corrosion, and various other side reactions. Regulating the Zn‐ion (Zn2+) solvation structure through electrolyte additives has been proved to be effective strategy in stabilizing the Zn anode, but the influence of free water on the solvation structure is often lacking in‐depth exploration. Herein, the piperazine‐N,N‐bis(2‐hydroxypropanesulfonic acid) sodium salt (POPSO‐Na) is presented as a multifunctional electrolyte additive, which enhances the stability of the Zn anode by modulating the deposition and stripping environment of Zn2⁺ and limiting the presence of free water in the electrolyte during cycling. Theoretical calculation and experimental results demonstrate that the POPSO‐Na additive can not only replace the structural water around Zn2+ to destroy the original solvation sheath, but also form reverse micelle interface structure to hinder the proton transition and constrain the free water in the electrolyte. Thus, the Zn||Zn battery utilizing the ZnSO4+POPSO‐Na electrolyte exhibits an impressive cycle life of 1600 h at a current density of 1 mA cm−2, achieving an average Coulomb efficiency (CE) of ≈100%, which is significantly better than that observed with the ZnSO4 electrolyte. Moreover, the Zn||Cu battery with ZnSO4+POPSO‐Na electrolyte achieves high stability even after cycling for over 2000 h.
由于电极/电解质界面的不稳定性会导致锌枝晶的生长、自腐蚀和其他各种副反应,从而严重影响水性锌离子(Zn)储能装置的稳定性。通过电解质添加剂调节锌离子(Zn2+)的溶解结构已被证明是稳定锌阳极的有效策略,但自由水对溶解结构的影响往往缺乏深入探讨。本文将哌嗪-N,N-双(2-羟基丙磺酸)钠盐(POPSO-Na)作为一种多功能电解质添加剂,通过调节 Zn2⁺的沉积和剥离环境,限制循环过程中电解质中自由水的存在,从而提高锌阳极的稳定性。理论计算和实验结果表明,POPSO-Na 添加剂不仅能取代 Zn2+ 周围的结构水,破坏原有的溶解鞘,还能形成反向胶束界面结构,阻碍质子转变,限制电解液中的自由水。因此,使用 ZnSO4+POPSO-Na 电解质的 Zn||Zn 电池在电流密度为 1 mA cm-2 时的循环寿命达到了惊人的 1600 h,平均库仑效率(CE)≈100%,明显优于 ZnSO4 电解质。此外,采用 ZnSO4+POPSO-Na 电解质的 Zn||Cu 电池在循环超过 2000 小时后仍能保持高稳定性。
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引用次数: 0
Advanced Electrode Materials for Low‐Temperature Na Storage 用于低温储存钠的先进电极材料
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1002/adfm.202419173
Wensun Zhu, Shitan Xu, Shoumeng Yang, Yang Yang, Xianhong Rui
Sodium‐ion batteries have drawn worldwide attention as ideal candidates for the upcoming generation of large‐scale electrical energy storage devices due to the low cost and abundance of sodium. Due to its unique electrochemical and chemical properties, sodium‐ion batteries hold the promise of breaking geographical and environmental constraints, achieving efficient sodium storage under low‐temperature conditions. However, low‐temperature sodium‐ion batteries, especially for their electrode materials, still face numerous challenges, such as the sluggish electrochemical reaction kinetics, poor material stability, significant volume changes leading to the pulverization of materials and the rapid degradation of battery performance. Here, it is focused on the modification methods for electrode materials, the research progress on cathode and anode materials of low‐temperature sodium‐ion batteries is summarized systematically and the other components of the electrodes are discussed briefly, and the shortcomings of the current research and possible future research directions are discussed thoroughly.
钠离子电池因成本低廉、钠资源丰富而备受世界瞩目,是下一代大规模电能存储设备的理想候选材料。由于其独特的电化学和化学特性,钠离子电池有望打破地理和环境限制,在低温条件下实现高效钠存储。然而,低温钠离子电池,尤其是其电极材料,仍然面临着诸多挑战,如电化学反应动力学迟缓、材料稳定性差、体积变化大导致材料粉碎和电池性能快速衰减等。在此,重点介绍了电极材料的改性方法,系统总结了低温钠离子电池正负极材料的研究进展,并对电极的其他组分进行了简要讨论,深入探讨了当前研究的不足和未来可能的研究方向。
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引用次数: 0
Intrinsic Activity: A Critical Challenge of Alkaline Hydrogen Oxidation Reaction 内在活性:碱性氢氧化反应的关键挑战
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1002/adfm.202414570
Xiaoyun Song, Qimei Yang, Kaisheng Zou, Zhenyang Xie, Jian Wang, Wei Ding
Anion exchange membrane fuel cells (AEMFCs) are advantageous for reducing or even eliminating the dependency on platinum resources, as the alkaline environment allows the use of non‐precious metal catalysts for oxygen reduction reaction at the cathode. However, the intrinsic activity of hydrogen oxidation reaction (HOR) catalysts in alkaline environments is 2 to 4 orders of magnitude lower than in acidic environments, which becomes the major challenge for AEMFCs. This review examines the current developments in the intrinsic activity of alkaline HOR catalysts and systematically summarizes the hydrogen activation mechanism with a focus on potential influencing factors and enhancement strategies. Furthermore, it offers insights into the prospects for developing more efficient alkaline HOR catalysts.
阴离子交换膜燃料电池(AEMFC)具有减少甚至消除对铂资源依赖的优势,因为碱性环境允许使用非贵金属催化剂在阴极进行氧还原反应。然而,碱性环境中氢氧化反应催化剂的内在活性比酸性环境中低 2 到 4 个数量级,这成为 AEMFCs 面临的主要挑战。本综述探讨了碱性 HOR 催化剂内在活性的最新进展,并系统总结了氢活化机理,重点介绍了潜在的影响因素和增强策略。此外,它还对开发更高效的碱性氢氧化还原催化剂的前景提出了见解。
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引用次数: 0
Synthetic Photoresponsive Hydrogels Enable In Situ Control Over Murine Intestinal Monolayer Differentiation and Crypt Formation 合成光致伸缩性水凝胶可原位控制小鼠肠道单层分化和隐窝形成
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1002/adfm.202413778
Mark W. Young, Colter E. Oroke, Bruce E. Kirkpatrick, Michael R. Blatchley, Peter J. Dempsey, Kristi S. Anseth
As a model of the intestinal epithelium, intestinal stem cells (ISCs) are grown and differentiated as monolayers on materials where stochastic organization of the crypt and villi cells occurs. An allyl sulfide crosslinked photoresponsive hydrogel with a shear modulus of 1.6 kPa is developed and functionalized with GFOGER, Bm‐binder peptide ligands for monolayer growth of ISCs. The allyl sulfide chemistry allows in situ control of mechanics in the presence of growing ISC monolayers and structured irradiation affords spatial regulation of the hydrogel properties. Specifically, ISC monolayers grown on 1.6 kPa substrates are in situ softened to 0.29 kPa, using circular patterns 50, 75, and 100 µm in diameter, during differentiation, resulting in control over the size and arrangement of de novo crypts and monolayer cellularity. These photoresponsive materials should be useful in applications ranging from studying crypt evolution to drug screening and transport across tissues of changing cellular composition. Spatiotemporal softening enables control over the size and arrangement of de novo crypts within intestinal monolayers.
作为肠上皮细胞的模型,肠干细胞(ISCs)以单层形式在隐窝和绒毛细胞随机组织的材料上生长和分化。我们开发了一种剪切模量为 1.6 kPa 的烯丙基硫醚交联光致伸缩性水凝胶,并用 GFOGER、Bm 粘合剂肽配体对其进行了功能化处理,以促进肠干细胞的单层生长。烯丙基硫醚化学成分可在生长的 ISC 单层存在的情况下对力学进行原位控制,而结构化辐照则可对水凝胶的特性进行空间调节。具体来说,在分化过程中,使用直径分别为 50、75 和 100 微米的圆形图案,将生长在 1.6 千帕基底上的 ISC 单层原位软化至 0.29 千帕,从而控制新生隐窝的大小和排列以及单层细胞性。这些光致伸缩材料的应用范围很广,从研究隐窝演化到药物筛选,以及在细胞组成不断变化的组织中的运输,都会有所帮助。时空软化可控制肠单层中新生隐窝的大小和排列。
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引用次数: 0
ZnO‐CuS/F127 Hydrogels with Multienzyme Properties for Implant‐Related Infection Therapy by Inhibiting Bacterial Arginine Biosynthesis and Promoting Tissue Repair 具有多酶特性的 ZnO-CuS/F127 水凝胶可通过抑制细菌精氨酸合成和促进组织修复来治疗与种植体有关的感染
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1002/adfm.202415778
Yiwei Sun, Wei Zhang, Zhiwen Luo, Can Zhu, Yiqun Zhang, Zheng Shu, Cailiang Shen, Xiaxi Yao, Yuanyin Wang, Xianwen Wang
Implant‐related infections are characterized by the formation of bacterial biofilms. Current treatments have various drawbacks. Nanozymes with enzyme‐like activity can produce highly toxic substances to kill bacteria and remove biofilms without inducing drug resistance. However, it is difficult for current monometallic nanozymes to function well in complex biofilm environments. Therefore, the development of multimetallic nanozymes with efficient multienzyme activities is crucial. In the present study, bimetallic nanozyme, ZnO‐CuS nanoflowers with peroxidase (POD), glutathione oxidase (GSH‐Px), and catalase (CAT) activity are successfully synthesized via calcination and loaded into F127 hydrogels for the treatment of implant‐related infections. The ability of ZnO‐CuS nanoflowers to bind bacteria is key for efficient antimicrobial activity. In addition, ZnO‐CuS nanoflowers with H2O2 disrupt the metabolism of MRSA, including arginine synthesis, nucleotide excision repair, energy metabolism, and protein synthesis. ZnO‐CuS/F127 hydrogel in combination with H2O2 has been demonstrated to be effective in clearing biofilm infection and facilitating the switch of M1 macrophages to M2‐repairative phenotype macrophages for the treatment of implant infections in mice. Furthermore, ZnO‐CuS/F127 hydrogels have favorable biosafety, and their toxicity is negligible. ZnO‐CuS/F127 hydrogel has provided a promising biomedical strategy for the healing of implant‐related infections, highlighting the potential of bimetallic nanozymes for clinical applications.
与种植体相关的感染以细菌生物膜的形成为特征。目前的治疗方法存在各种弊端。具有类似酶活性的纳米酶可以产生剧毒物质,杀死细菌并清除生物膜,同时不会诱发耐药性。然而,目前的单金属纳米酶很难在复杂的生物膜环境中发挥良好作用。因此,开发具有高效多酶活性的多金属纳米酶至关重要。在本研究中,通过煅烧成功合成了具有过氧化物酶(POD)、谷胱甘肽氧化酶(GSH-Px)和过氧化氢酶(CAT)活性的双金属纳米酶 ZnO-CuS纳米花,并将其装载到 F127 水凝胶中,用于治疗与种植体相关的感染。ZnO-CuS 纳米花结合细菌的能力是高效抗菌的关键。此外,含有 H2O2 的 ZnO-CuS 纳米花会破坏 MRSA 的新陈代谢,包括精氨酸合成、核苷酸切除修复、能量代谢和蛋白质合成。实验证明,ZnO-CuS/F127 水凝胶与 H2O2 结合使用可有效清除生物膜感染,并促进 M1 型巨噬细胞向 M2 修复表型巨噬细胞转换,从而治疗小鼠的植入感染。此外,ZnO-CuS/F127 水凝胶还具有良好的生物安全性,其毒性可忽略不计。ZnO-CuS/F127 水凝胶为植入物相关感染的愈合提供了一种前景广阔的生物医学策略,凸显了双金属纳米酶在临床应用方面的潜力。
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引用次数: 0
Crystallization Control of Blade-Coated Wide Bandgap FACs-Based Perovskite 基于刀片涂层宽带隙 FAC 的过磷酸盐的结晶控制
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1002/adfm.202417493
Xin Ge, Zixuan Huang, Biao Shi, Pengyang Wang, Zhen Liu, You Gao, Xiaona Du, Ying Zhao, Xiaodan Zhang
Transforming perovskite solar cells into commercial production requires advanced scalable deposition technology. However, the deposition of high-quality perovskite thin films using the blade coating method presents challenges, especially in controlling the nucleation and crystallization of perovskite. In this work, an effective approach is proposed for controlling nucleation and crystallization by simultaneously incorporating two kinds of ionic liquid, namely 1H-imidazole acetate (IMAc), and 1-buty-3-methylimidazolium tetrafluoroborate (BMIMBF4), into the precursor solution. This innovative strategy initiates ππ interactions between IM and BMIM cations, thereby enhancing the interaction between cations and the Pb-I framework. The competitive mechanism of interaction with Pb-I framework effectively suppresses the formation of unfavorable mesophase, thereby enabling a single crystallization pathway from NMP + PbI2 to α-perovskite. Consequently, this method effectively reduces defects and enhances the crystal quality of α-perovskite film. Based on this strategy, the power conversion efficiency of the p-i-n wide bandgap perovskite device prepared by the blade coating method, is increased to 21.31%, representing one of the highest efficiencies achieved with this technology for 1.68 eV bandgap FACs-based perovskites. Thus, this approach emerges as a feasible breakthrough strategy that may unleash the full potential of perovskite solar cells.
要将过氧化物太阳能电池投入商业生产,需要先进的可扩展沉积技术。然而,使用叶片镀膜法沉积高质量的包晶体薄膜面临着挑战,尤其是在控制包晶体的成核和结晶方面。本研究提出了一种控制成核和结晶的有效方法,即在前驱体溶液中同时加入两种离子液体,即 1H-imidazole acetate (IMAc) 和 1-buty-3-methylimidazolium tetrafluoroborate (BMIMBF4)。这种创新策略启动了 IM 和 BMIM 阳离子之间的 π-π 相互作用,从而增强了阳离子与 Pb-I 框架之间的相互作用。与 Pb-I 框架相互作用的竞争机制有效地抑制了不利介相的形成,从而实现了从 NMP + PbI2 到 α-perovskite 的单一结晶途径。因此,这种方法能有效减少缺陷,提高 α-perovskite 薄膜的晶体质量。基于这种策略,用叶片镀膜法制备的 pi-n 宽带隙过氧化物器件的功率转换效率提高到了 21.31%,这代表了用这种技术制备 1.68 eV 带隙 FACs 基过氧化物的最高效率之一。因此,这种方法是一种可行的突破性战略,可以充分释放出包晶石太阳能电池的潜力。
{"title":"Crystallization Control of Blade-Coated Wide Bandgap FACs-Based Perovskite","authors":"Xin Ge, Zixuan Huang, Biao Shi, Pengyang Wang, Zhen Liu, You Gao, Xiaona Du, Ying Zhao, Xiaodan Zhang","doi":"10.1002/adfm.202417493","DOIUrl":"https://doi.org/10.1002/adfm.202417493","url":null,"abstract":"Transforming perovskite solar cells into commercial production requires advanced scalable deposition technology. However, the deposition of high-quality perovskite thin films using the blade coating method presents challenges, especially in controlling the nucleation and crystallization of perovskite. In this work, an effective approach is proposed for controlling nucleation and crystallization by simultaneously incorporating two kinds of ionic liquid, namely 1H-imidazole acetate (IMAc), and 1-buty-3-methylimidazolium tetrafluoroborate (BMIMBF<sub>4</sub>), into the precursor solution. This innovative strategy initiates <i>π</i>–<i>π</i> interactions between IM and BMIM cations, thereby enhancing the interaction between cations and the Pb-I framework. The competitive mechanism of interaction with Pb-I framework effectively suppresses the formation of unfavorable mesophase, thereby enabling a single crystallization pathway from NMP + PbI<sub>2</sub> to α-perovskite. Consequently, this method effectively reduces defects and enhances the crystal quality of α-perovskite film. Based on this strategy, the power conversion efficiency of the p-i-n wide bandgap perovskite device prepared by the blade coating method, is increased to 21.31%, representing one of the highest efficiencies achieved with this technology for 1.68 eV bandgap FACs-based perovskites. Thus, this approach emerges as a feasible breakthrough strategy that may unleash the full potential of perovskite solar cells.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"21 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642790","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
Optimizing Hygroscopic Metal–Organic Frameworks via EDTA‐Mediated Structural Reinforcement and Photothermal Modification 通过 EDTA 介导的结构强化和光热修饰优化吸湿性金属有机框架
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1002/adfm.202416241
Mingren Cheng, Xin Lian, Haoyu Bai, Xinsheng Wang, Jian Xu, Moyuan Cao, Xian‐He Bu
Hygroscopic metal–organic frameworks (MOFs) are considered as superior moisture sorbents due to their highly adjustable and desired water adsorption/release performance, enabling effective atmospheric water harvesting (AWH) in arid regions. However, the water adsorption capacity, recycling stability, and functionality of current MOFs should be further improved to meet the requirements of practical AWH systems. Here the hydrophilicity at low relative humidity (RH) and cycling stability of MOF‐808 are simultaneously enhanced through the ethylenediaminetetraacetic acid (EDTA)‐mediated post‐modification. Based on the structural reinforcement, EDTA‐modified MOF‐808 (E‐MOF‐808) delivers a stable water uptake capacity of 0.39 g g−1 at 25% RH even after 50 water adsorption–desorption cycles, more than five times that of pristine MOF‐808. In addition, bridging by EDTA with the strong chelating ability, the E‐MOF‐808 can spontaneously capture Cu2+ for further functional improvement. Accordingly, light‐absorbing CuS nanoparticles can be in situ decorated on E‐MOF‐808 for facilitating solar‐driven water release. It is envisioned that this EDTA‐mediated function enhancement should provide valuable insights into the all‐in‐one design of versatile MOFs sorbents.
吸湿性金属有机框架(MOFs)因其高度可调和理想的吸水/释水性能而被认为是上佳的水分吸附剂,可在干旱地区实现有效的大气集水(AWH)。然而,目前 MOFs 的吸水能力、循环稳定性和功能性有待进一步提高,以满足实际大气集水系统的要求。在这里,通过乙二胺四乙酸(EDTA)介导的后修饰,MOF-808 在低相对湿度(RH)下的亲水性和循环稳定性同时得到了增强。在结构强化的基础上,EDTA修饰的MOF-808(E-MOF-808)在25%相对湿度条件下,即使经过50次吸水-解吸循环,也能提供0.39 g-1的稳定吸水能力,是原始MOF-808的五倍以上。此外,通过具有强螯合能力的 EDTA 桥接,E-MOF-808 还能自发捕获 Cu2+,进一步提高功能。因此,可以在 E-MOF-808 上原位装饰吸光的 CuS 纳米粒子,以促进太阳能驱动的水释放。预计这种由 EDTA 介导的功能增强将为多功能 MOFs 吸附剂的一体化设计提供宝贵的启示。
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引用次数: 0
Multi‐Solvent‐Induced Gradient Aggregation Rendered Superstrong, Tough, Stretchable, and Fatigue‐Resistant Lignin‐Based Supramolecular Hydrogels 多溶剂诱导梯度聚合生成超强、坚韧、可拉伸和抗疲劳的木质素基超分子水凝胶
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1002/adfm.202417206
Yihui Gu, Wenjuan Wu, Chaofeng Zhang, Xinrui Li, Xinyu Guo, Yilin Wang, Yufeng Yuan, Bo Jiang, Yongcan Jin
A hydrogel that is expected as a biomedical load‐bearing material remains a substantial challenge. In this work, a multi‐solvent‐induced gradient aggregation state strategy is developed to construct lignin‐based supramolecular hydrogels that feature superstrong, tough, stretchable, and fatigue‐resistant properties. The multi‐solvent high‐temperature annealing induces the gradient crystallization of polyvinyl alcohol and the self‐assembly of lignin. The interior strong hydrogen‐binding and the external weak non‐covalent‐binding forms a gradient aggregation state microstructure and compact macrostructure, where lignin acts as an interfacial molecular bridge. By sharing interconnection points to collaboratively dissipate energy, the developed hydrogels demonstrate high modulus (74.4 MPa), toughness (90 MJ m−3), tear (34,000 J m−2), tensile (24.8 MPa), and compressive strength (60 MPa). Moreover, such lignin‐based supramolecular hydrogels also exhibit extraordinary fatigue resistance, biocompatibility, and reactive oxygen species scavenging activity. This gradient non‐covalent conjoined‐network caused by multi‐solvent high‐temperature annealing provides a new design strategy and potential for developing biomaterials that mimic biomedical load‐bearing materials (e.g., natural tendons and ligaments).
一种有望成为生物医学承重材料的水凝胶仍然是一项巨大的挑战。本研究开发了一种多溶剂诱导梯度聚集态策略,用于构建木质素基超分子水凝胶,这种水凝胶具有超强、坚韧、可拉伸和抗疲劳的特性。多溶剂高温退火诱导了聚乙烯醇的梯度结晶和木质素的自组装。内部的强氢结合和外部的弱非共价结合形成了梯度聚集态的微观结构和紧密的宏观结构,其中木质素起到了界面分子桥的作用。通过共享互连点协同消散能量,所开发的水凝胶具有高模量(74.4 兆帕)、韧性(90 兆焦耳/立方米)、撕裂强度(34,000 焦耳/立方米)、拉伸强度(24.8 兆帕)和压缩强度(60 兆帕)。此外,这种基于木质素的超分子水凝胶还表现出非凡的抗疲劳性、生物相容性和活性氧清除活性。多溶剂高温退火所产生的这种梯度非共价连接网络为开发模拟生物医学承重材料(如天然肌腱和韧带)的生物材料提供了一种新的设计策略和潜力。
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引用次数: 0
Transient Structural Transition in Ovonic Threshold Switching Glass 卵形阈值开关玻璃中的瞬态结构转变
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1002/adfm.202415462
Yeon‐Woo Seong, Hoedon Kwon, Changwoo Lee, Hyeonwook Lim, Kwnagsik Jeong, Hee Jun Shin, Mann‐Ho Cho
Ovonic threshold switching (OTS), characterized by a rapid resistance drop in chalcogenide glass, has enabled the realization of memory and selectors. Despite over five decades of development, the challenges in characterizing the transient switching in amorphous materials upon reaching the threshold voltage have hindered the establishment of its underlying mechanism. This study uses femtosecond terahertz spectroscopy and ab initio simulation to elucidate the dynamics of the free‐carrier and IR‐active phonons involved in OTS. Specifically, in Te‐rich amorphous GeTe, the generation of transient phonons is observed within picoseconds, a phenomenon associated with an increased Born effective charge due to the alignment of Te‐centered bonds. The findings demonstrate a correlation between the enhancement of polarizability, due to orbital alignment during the disorder–order structural transition while maintaining a macroscopic amorphous structure, and the switching behavior. These results provide valuable insights into the enigmatic OTS phenomenon.
以掺杂镓玻璃中电阻快速下降为特征的椭圆阈值开关(OTS),使存储器和选择器得以实现。尽管经过了五十多年的发展,但在表征非晶材料达到阈值电压时的瞬态开关时所面临的挑战阻碍了其基本机制的建立。本研究利用飞秒太赫兹光谱和 ab initio 模拟来阐明参与 OTS 的自由载流子和红外活性声子的动力学。具体来说,在富含碲的非晶态 GeTe 中,可在皮秒内观察到瞬态声子的产生,这种现象与碲中心键的排列导致的 Born 有效电荷增加有关。研究结果表明,在保持宏观非晶结构的同时,无序结构转变过程中轨道排列导致的极化能力增强与开关行为之间存在关联。这些结果为研究神秘的 OTS 现象提供了宝贵的见解。
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引用次数: 0
Coordination of Ultralow Permittivity and Higher Thermal Conductivity of Polyimide Induced by Unique Interfacial Self‐Assembly Behavior 独特的界面自组装行为诱导聚酰亚胺的超低脆性和较高导热性的协调
IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1002/adfm.202417843
Xiaodi Dong, Baoquan Wan, Langbiao Huang, Quanliang Zhao, Ruifeng Yao, Jinghui Gao, Can Ding, Xu Wang, Zhi‐Min Dang, George Chen, Jun‐Wei Zha
Upgrading the available dielectric materials is the most effective approach to solve the poor quality of signal transmission and heat buildup caused by high density integration. In this work, a design strategy for multilayer 3D porous composite networks is proposed, relying on the self‐assembly effect of “crystal‐like phase” to achieve the synergistic optimization of low permittivity and high thermal conductivity of polyimide. The obtained three‐layer porous polyimide composite film (PSLS) features an ultralow permittivity of 1.89, an in‐plane thermal conductivity as high as 13.58 W m−1 K−1, and maintains well electrical insulating property. Inspiringly, the first digital thermoacoustic generator with wide frequency response has been designed based on PSLS film. It achieves sound pressure levels up to 60.1 dB in the 20–100 kHz range and integrates the efficient sound generation of an ultrasonic generator with real‐time display. This work will provide a novel concept material for the smart electronics and electrical fields.
要解决高密度集成带来的信号传输质量差和热量积聚问题,提升现有介电材料是最有效的方法。本文提出了一种多层三维多孔复合网络的设计策略,依靠 "类晶相 "的自组装效应,实现了聚酰亚胺低介电常数和高导热系数的协同优化。所获得的三层多孔聚酰亚胺复合薄膜(PSLS)具有 1.89 的超低介电常数、高达 13.58 W m-1 K-1 的面内热导率和良好的电绝缘性能。令人鼓舞的是,基于 PSLS 薄膜设计出了第一台具有宽频率响应的数字热声发生器。它能在 20-100 kHz 范围内实现高达 60.1 dB 的声压级,并集成了超声波发生器的高效发声和实时显示功能。这项工作将为智能电子和电气领域提供一种新型概念材料。
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引用次数: 0
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Advanced Functional Materials
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