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Environmentally tolerant multifunctional eutectogel for highly sensitive wearable sensors. 适用于高灵敏度可穿戴传感器的环保多功能共聚物。
IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-14 DOI: 10.1039/d4mh01665c
Zhengen Wei, Lianghao Jia, Jinyu Yu, Hanrui Xu, Xing Guo, Tao Xiang, Shaobing Zhou

Flexible hydrogel sensors have found extensive applications. However, the insufficient sensing sensitivity and the propensity to freeze at low temperatures restrict their use, particularly in frigid conditions. Herein, a multifunctional eutectogel with high transparency, anti-freezing, anti-swelling, adhesive, and self-healing properties is prepared by a one-step photopolymerization of acrylic acid and lauryl methacrylate in a binary solvent comprising water and deep eutectic solvent (DES). The results from the molecular dynamics simulations and density functional theory indicate that the hydrogen bonds between DES and water mixtures possess better stability than those between water molecules. On the other hand, DES breaks down hydrogen bonds in water, providing eutectogels with excellent anti-freezing even at -60 °C. Cetyltrimethylammonium bromide is incorporated to establish stable hydrophobic interactions and electrostatic attractions with polymer chains in the eutectogel network, resulting in superior mechanical (elongation at break of 2890%) and anti-swelling (only 2% swelling in water over 7 days) properties. The eutectogel-based strain sensors exhibit remarkable sensitivity, achieving a gauge factor of up to 15.4. The multifunctional eutectogel sensors can monitor motion and transmit encrypted information at low temperatures, demonstrating considerable potential for applications in flexible electronics within low-temperature environments.

柔性水凝胶传感器有广泛的应用。然而,感应灵敏度不足和在低温下结冰的倾向限制了它们的使用,特别是在寒冷的条件下。本发明利用丙烯酸和甲基丙烯酸月桂酯在由水和深度共晶溶剂(DES)组成的二元溶剂中一步光聚合制备了一种具有高透明度、防冻、抗膨胀、粘接和自愈性能的多功能共聚物。分子动力学模拟和密度泛函理论的结果表明,DES与水混合物之间的氢键比水分子之间的氢键具有更好的稳定性。另一方面,DES破坏水中的氢键,即使在-60°C下也能使共凝胶具有优异的抗冻性。十六烷基三甲基溴化铵与共聚网络中的聚合物链建立稳定的疏水相互作用和静电吸引力,从而产生优越的机械性能(断裂伸长率为2890%)和抗膨胀性能(在水中7天内仅膨胀2%)。基于共晶的应变传感器具有显著的灵敏度,测量系数高达15.4。多功能共tectol传感器可以在低温下监测运动和传输加密信息,在低温环境下的柔性电子应用中显示出相当大的潜力。
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引用次数: 0
Solvothermally optimizing Ag2Te/Ag2S composites with high thermoelectric performance and plasticity. 溶解热优化具有高热电性能和可塑性的 Ag2Te/Ag2S 复合材料。
IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-13 DOI: 10.1039/d4mh01654h
Min Zhu, Xiao-Lei Shi, Meng Li, Hao Wu, De-Zhuang Wang, Liang-Cao Yin, Ting Wu, Wei-Di Liu, Yan Huang, Zhi-Gang Chen, Qingfeng Liu

Silver-based fast ionic conductors show promising potential in thermoelectric applications. Among these, Ag2S offers unique high plasticity but low electrical conductivity, whereas Ag2Te exhibits high intrinsic electrical conductivity yet faces limitations due to high thermal conductivity and poor plasticity. Developing a composite thermoelectric material that combines the benefits of both is therefore essential. Here, this study reports the successful synthesis of Ag2Te/Ag2S composites via a facile and low-cost solvothermal method. By finely adjusting the composition of Ag2S and Ag2Te to obtain the optimized carrier concentration and the enhanced mobility, the figure of merit ZT of Ag2Te/Ag2S composites reached ∼0.42 at 373 K and ∼0.38 at 298 K, both surpassing those of pure Ag2S and Ag2Te. This increase in ZT also benefits from lattice defects created by the solvothermally synthesized biphasic composition, effectively scattering phonons of various wavelengths and reducing thermal conductivity compared to pure Ag2Te. Additionally, the plasticity of the Ag2Te/Ag2S composites improved considerably over pure Ag2Te, achieving a bending strain of ∼2.5% (versus ∼1.2% for intrinsic Ag2Te). This study can fill a critical gap in the research on composite silver-based fast ionic conductors synthesized via wet chemical methods and provide valuable guidance for future exploration.

银基快速离子导体在热电领域具有广阔的应用前景。其中,Ag2S具有独特的高塑性,但电导率低,而Ag2Te具有高的固有电导率,但由于热导率高,塑性差而面临局限性。因此,开发一种结合两者优点的复合热电材料至关重要。在这里,本研究报告了通过简单和低成本的溶剂热方法成功合成Ag2Te/Ag2S复合材料。通过精细调整Ag2S和Ag2Te的组成来获得优化的载流子浓度和增强的迁移率,Ag2Te/Ag2S复合材料的优点ZT在373 K和298 K时分别达到了~ 0.42和~ 0.38,均超过了纯Ag2S和Ag2Te。这种ZT的增加也得益于溶剂热合成的双相成分产生的晶格缺陷,与纯Ag2Te相比,有效地散射各种波长的声子并降低热导率。此外,与纯Ag2Te相比,Ag2Te/Ag2S复合材料的塑性得到了显著改善,弯曲应变达到了~ 2.5%(而本质Ag2Te为~ 1.2%)。该研究填补了湿化学方法合成银基复合快速离子导体研究的关键空白,为今后的探索提供了有价值的指导。
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引用次数: 0
Acetylene semi-hydrogenation catalyzed by Pd single atoms sandwiched in zeolitic imidazolate frameworks via hydrogen activation and spillover. 夹在沸石咪唑啉框架中的钯单原子通过氢活化和溢出催化乙炔半氢化。
IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-13 DOI: 10.1039/d4mh01787k
Yan-Ting Li, Wen-Gang Cui, Ying-Fei Huo, Lei Zhou, Xinqiang Wang, Fan Gao, Qiang Zhang, Wei Li, Tong-Liang Hu

The semi-hydrogenation of alkynes into alkenes rather than alkanes is of great importance in the chemical industry, and palladium-based metallic catalysts are currently employed. Unfortunately, a fairly high cost and uncontrollable over-hydrogenation impeded the application of Pd-based catalysts on a large scale. Herein, a sandwich structure single atom Pd catalyst, Z@Pd@Z, was prepared via impregnation exchange and epitaxial growth methods (Z stands for ZIF-8), in which Pd single atoms were stabilized by pyrrolic N in a zeolitic imidazolate framework (ZIF-8). Semi-hydrogenation of acetylene was performed and Z@Pd@Z achieved 100% acetylene conversion at 120 °C with an ethylene selectivity of more than 98.3% at an extra low Pd concentration. Z@Pd@Z exhibited a specific activity of 1872.69 mLC2H4 mgPd-1 h-1, surpassing most of the reported Pd-based catalysts. The existence of Pd single atoms coordinated by nitrogen (Pd-N4) was verified by XAS (synchrotron X-ray absorption spectroscopy), which provided active sites for H2 dissociation and the dissociated hydrogen quickly spilled over the surface of the outer ZIF layer to hydrogenate alkyne to ethene; besides, the catalytic activity could be controlled by adjusting the thickness of the outer ZIF layer. The confinement of the ZIF on Pd single-atom sites and the high energy barrier of ethylene hydrogenation were found to be responsible for the superior C2H2 semi-hydrogenation activity. This work opens up valuable insights into the design of ZIF-derived single-atom catalysts for efficient acetylene selective hydrogenation.

在化学工业中,将炔烃半氢化成烯烃而不是烷烃具有重要意义,目前采用的是钯基金属催化剂。遗憾的是,相当高的成本和不可控的过氢化阻碍了钯基催化剂的大规模应用。本文通过浸渍交换和外延生长方法制备了一种三明治结构的单原子钯催化剂 Z@Pd@Z(Z 代表 ZIF-8),其中钯单原子被吡咯烷 N 稳定在沸石咪唑酸框架(ZIF-8)中。Z@Pd@Z 在 120 °C 时实现了 100% 的乙炔转化,在超低钯浓度下乙烯选择性超过 98.3%。Z@Pd@Z 的比活度为 1872.69 mLC2H4 mgPd-1 h-1,超过了大多数已报道的钯基催化剂。XAS(同步辐射 X 射线吸收光谱)验证了氮配位钯单原子(Pd-N4)的存在,这为 H2 离解提供了活性位点,离解的氢迅速溢出 ZIF 外层表面,将炔烃氢化为乙烯;此外,催化活性可通过调节 ZIF 外层的厚度来控制。研究发现,ZIF 对钯单原子位点的限制和乙烯氢化的高能垒是 C2H2 半氢化活性优异的原因。这项研究为设计 ZIF 衍生单原子催化剂以实现高效乙炔选择性氢化提供了宝贵的见解。
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引用次数: 0
Lanthanide-polyoxometalate-based self-erasing luminescent hydrogels with time-dependent and resilient properties for advanced information encryption. 基于镧系多金属氧酸盐的自擦发光水凝胶,具有时间依赖性和弹性特性,用于高级信息加密。
IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-13 DOI: 10.1039/d4mh01451k
Yumei Hua, Jingfang Li, Min Gao, Liye Liang, Sicong Zhao, Guangming Li

In such an era of information explosion, improving the level of information security is still a challenging task. Self-erasing luminescent hydrogels are becoming ideal candidates for improving the level of information security with simple encryption and decryption methods. Herein, a lanthanide-polyoxometalate-based self-erasing luminescent hydrogel with time-dependent and resilient properties was constructed through a covalent crosslinked network constructed with polyacrylamide and a non-covalent crosslinked network constructed with [2-(methacryloyloxy)ethyl]trimethyl ammonium chloride/Na9DyW10O36, along with doping urease. This acquired hydrogel exhibited reversible luminescence switching properties in the presence of HCl-urea mixed solution. At the same time, obvious changes in the luminescence intensity can be seen on the timescale by modulating the concentrations of HCl and urea/urease. Based on this, the information loaded onto the hydrogel by using a HCl-urea mixed solution self-erased over time, leading to misinformation during this process. The real information can only be recognized at a specific time. Moreover, the information is self-erased permanently, which can avoid secondary leakage of information. In addition, the hydrogel has excellent resilience. The information can be loaded in the stretched state of the hydrogel, resulting in the information only being recognized in the re-stretched state of the hydrogel while the information cannot be recognized in the normal state of the hydrogel. The combination of time-dependent and resilient properties of the hydrogel can further improve the level of information security effectively. This self-erasing luminescent hydrogel with time-dependent and resilient properties has great potential in improving the security of information encryption.

在这样一个信息爆炸的时代,提高信息安全水平仍然是一项具有挑战性的任务。自擦发光水凝胶正成为通过简单的加密和解密方法提高信息安全水平的理想候选者。本文通过聚丙烯酰胺共价交联网络和[2-(甲基丙烯氧基)乙基]三甲基氯化铵/Na9DyW10O36非共价交联网络,以及掺杂脲酶,构建了一种具有时间依赖性和弹性的镧系多金属氧酸盐基自擦发光凝胶。该水凝胶在盐酸-尿素混合溶液中表现出可逆的发光开关特性。同时,通过调节HCl和尿素/脲酶的浓度,在时间尺度上可以观察到明显的发光强度变化。在此基础上,通过使用盐酸-尿素混合溶液加载到水凝胶上的信息会随着时间的推移而自我擦除,从而在此过程中导致错误信息。真实的信息只有在特定的时间才能被识别。此外,该信息是永久自擦的,可以避免信息的二次泄露。此外,水凝胶具有优异的回弹性。所述信息可以在水凝胶的拉伸状态下加载,导致所述信息仅在水凝胶的再拉伸状态下被识别,而在水凝胶的正常状态下不能被识别。水凝胶的时变特性和弹性特性相结合,可以进一步有效地提高信息安全水平。这种具有时间依赖性和弹性的自擦发光水凝胶在提高信息加密安全性方面具有很大的潜力。
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引用次数: 0
Sensor-combined organ-on-a-chip for pharmaceutical and medical sciences: from design and materials to typical biomedical applications. 用于制药和医学科学的传感器组合器官芯片:从设计和材料到典型生物医学应用。
IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-13 DOI: 10.1039/d4mh01174k
Yumeng Liao, Danni Chai, Quan Wang, Xueqi Wang, Qian Yong, Zhaoming Cheng, Chuanjun Zhang, Di Zhang, Boshi Liu, Rui Liu, Zheng Li

Organ-on-a-chip (OoC) is a breakthrough technology in biomedicine. As microphysiological systems constructed in vitro, OoCs can simulate the main structures and functions of human organs, thereby providing a powerful tool for drug screening and disease model construction. Furthermore, the coupling of OoCs and sensors has been an innovative discovery in the field of biomedical and electronic engineering in recent years. The integration of sensors into OoCs allows the real-time monitoring of the changes in the microenvironmental parameters within the chip, reflecting the physiological responses of cells or tissues in the OoC and providing more accurate data support for drug development and disease treatment. In this work, we briefly outline the design ideas of OoCs, summarize the commonly used materials for OoCs and their advantages and disadvantages, and provide the most recent practical examples of the combination of OoCs and sensors in pharmaceutical and medical sciences. Furthermore, perspectives, challenges and their solutions in the future development of this technology are provided, with the aim to inspire the researchers to work toward the subsequent development of OoCs having improved reliability.

器官芯片技术是生物医学领域的一项突破性技术。ooc作为体外构建的微生理系统,可以模拟人体器官的主要结构和功能,为药物筛选和疾病模型构建提供了有力的工具。此外,ooc与传感器的耦合是近年来生物医学和电子工程领域的一项创新发现。将传感器集成到OoC中,可以实时监测芯片内微环境参数的变化,反映OoC中细胞或组织的生理反应,为药物开发和疾病治疗提供更准确的数据支持。在这项工作中,我们简要概述了OoCs的设计思想,总结了OoCs的常用材料及其优缺点,并提供了OoCs与传感器在制药和医学科学中结合的最新实际例子。展望了该技术未来发展的前景、挑战和解决方案,旨在激励研究人员朝着提高可靠性的ooc的后续发展而努力。
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引用次数: 0
Highly polarized single-crystal organic light-emitting devices with low turn-on voltage and high brightness. 具有低开启电压和高亮度的高偏振单晶有机发光器件。
IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-13 DOI: 10.1039/d4mh01376j
Aijia Pang, Fan Yin, Jianbo De, Cunbin An, Bo Liao, Chunling Gu, Qing Liao, Hongbing Fu

Linearly-polarized organic electroluminescent devices have gained significant attention due to their potential applications across various fields. However, traditional thin-film organic light-emitting diodes (OLEDs) face significant challenges, primarily due to the necessity of incorporating complex optical elements. In this study, we present linearly-polarized OLEDs (LP-OLEDs) based on organic single crystals that we have designed and prepared. These devices exhibit a degree of polarization (DOP) of up to 0.96 for photoluminescence and 0.95 for electroluminescence, values that are close to the ideal linearly-polarized light (DOP = 1). The LP-OLEDs demonstrate outstanding performance, with a low turn-on voltage of just 2.5 volts, an exceptionally high brightness of 200 000 cd m-2, and a current density surpassing 300 A cm-2. This is the best overall performance reported for single crystal-based OLEDs to date. These results open the door to the development of next-generation, low-power consumption displays, marking a significant step forward in the field of organic single crystal-based LP-OLEDs.

线性偏振有机电致发光器件因其在各个领域的潜在应用而备受关注。然而,传统的薄膜有机发光二极管(OLED)面临着巨大的挑战,这主要是由于必须结合复杂的光学元件。在本研究中,我们介绍了基于有机单晶体设计和制备的线性偏振有机发光二极管(LP-OLED)。这些器件的光致发光极化度(DOP)高达 0.96,电致发光极化度(DOP)高达 0.95,接近理想的线性极化光(DOP = 1)。LP-OLED 性能卓越,开启电压低至 2.5 伏,亮度高达 200 000 cd m-2,电流密度超过 300 A cm-2。这是迄今所报道的单晶有机发光二极管的最佳整体性能。这些成果为开发下一代低功耗显示器打开了大门,标志着有机单晶基 LP-OLED 领域向前迈出了重要一步。
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引用次数: 0
Porous polymers: structure, fabrication and application. 多孔聚合物:结构、制造和应用。
IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-13 DOI: 10.1039/d4mh01618a
Qingxian Liu, Jinkui Xiong, Wengui Lin, Jinlong Liu, Yongbiao Wan, Chuan Fei Guo, Quan Wang, Zhiguang Liu

The porous polymer is a common and fascinating category within the vast family of porous materials. It offers valuable features such as sufficient raw materials, easy processability, controllable pore structures, and adjustable surface functionality by combining the inherent properties of both porous structures and polymers. These characteristics make it an effective choice for designing functional and advanced materials. In this review, the structural features, processing techniques and application fields of the porous polymer are discussed comprehensively to present their current status and provide a valuable tutorial guide and help for researchers. Firstly, the basic classification and structural features of porous polymers are elaborated upon to provide a comprehensive analysis from a mesoscopic to macroscopic perspective. Secondly, several established techniques for fabricating porous polymers are introduced, including their respective basic principles, characteristics of the resulting pores, and applied scopes. Thirdly, we demonstrate application research of porous polymers in various emerging frontier fields from multiple perspectives, including pressure sensing, thermal control, electromagnetic shielding, acoustic reduction, air purification, water treatment, health management, and so on. Finally, the review explores future directions for porous polymers and evaluates their future challenges and opportunities.

多孔聚合物是多孔材料大家族中一个常见而迷人的类别。它结合了多孔结构和聚合物的固有特性,具有原料充足、易于加工、孔结构可控、表面功能可调等宝贵特点。这些特点使其成为设计功能材料和先进材料的有效选择。本综述全面论述了多孔聚合物的结构特征、加工技术和应用领域,介绍了其发展现状,为研究人员提供有价值的指导和帮助。首先,阐述了多孔聚合物的基本分类和结构特征,从中观到宏观进行了全面分析。其次,介绍了几种制造多孔聚合物的成熟技术,包括其各自的基本原理、所得孔隙的特征和应用范围。第三,从压力传感、热控制、电磁屏蔽、隔音降噪、空气净化、水处理、健康管理等多个角度展示了多孔聚合物在各个新兴前沿领域的应用研究。最后,综述探讨了多孔聚合物的未来发展方向,并评估了其未来面临的挑战和机遇。
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引用次数: 0
Ultimate water capillary evaporation in bamboo-inspired evaporator. 在竹子启发的蒸发器中实现水的最终毛细蒸发。
IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-13 DOI: 10.1039/d4mh01667j
Kefan Shi, Marliyana Aizudin, Meilan Pan, Edison Huixiang Ang

Bionic evaporators inspired by natural plants like bamboo and mushrooms have emerged as efficient generators through water capillary evaporation. However, primitive natural evaporators cannot currently meet growing demand, and their performance limitations remain largely unexplored, presenting a substantial challenge. Through extensive experimentation and detailed simulation analysis, this study presents a precisely engineered H-type bamboo steam generator. This innovative design incorporates a unique node structure embedded with graphite flakes and an internode characterized by micro- and nanoporous channels, all achieved through streamlined carbonization. The results are striking: a water evaporation rate of 2.28 kg m-2 h-1 and a photothermal conversion efficiency of 90.2% under one-sun irradiation, outperforming comparable alternatives. This study also marks the first comprehensive simulation in COMSOL modeling water capillary evaporation, driven by the synergistic effects of photothermal graphitic layers, broad-spectrum solar absorption, and capillary microstructures. The chimney-assisted, enclosed cavity structure further enhances water capillary evaporation and thermal localization. This breakthrough not only enables efficient use of waste biomass but also advances the field of sustainable materials, opening new avenues in solar-driven steam generation.

受竹子和蘑菇等天然植物的启发,仿生蒸发器通过毛细管蒸发成为高效的发电机。然而,原始的天然蒸发器目前不能满足日益增长的需求,其性能限制在很大程度上仍未被探索,提出了实质性的挑战。通过大量的实验和详细的仿真分析,本研究提出了一种精确设计的h型竹蒸汽发生器。这种创新的设计结合了嵌入石墨片的独特节点结构和以微孔和纳米孔通道为特征的节点间,所有这些都通过流线型碳化实现。结果是惊人的:在一次太阳照射下,水蒸发率为2.28 kg m-2 h-1,光热转换效率为90.2%,优于同类替代品。该研究也标志着COMSOL模拟水毛细蒸发的第一个综合模拟,由光热石墨层、广谱太阳吸收和毛细微结构的协同效应驱动。烟囱辅助的封闭腔体结构进一步促进了水的毛细蒸发和热局部化。这一突破不仅使废弃生物质的有效利用成为可能,而且推动了可持续材料领域的发展,为太阳能驱动的蒸汽产生开辟了新的途径。
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引用次数: 0
Long-chain crosslinker-induced patterning on an elastic polymer film for robust and reversible information encryption/decryption. 弹性聚合物薄膜上的长链交联剂诱导图图化用于稳健可逆的信息加密/解密。
IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-13 DOI: 10.1039/d4mh01828a
Qitong He, Qiuhua Zhao, Lidong Zhang

While reversible information encryption and decryption are readily achievable with hydrogels, this process presents a significant challenge when applied to elastic polymer films. This is due to the inherent chemical stability of anhydrous polymer films which significantly increases the difficulty of information writing. In this study, we propose a solvent-free radical polymerization method for chemical patterning on the elastic film of poly(styrene-butadiene-styrene) (SBS). Unlike short chain crosslinkers-induced patterning, which increases the brittleness of the film, the long-chain crosslinkers are chemically bonded with the chains of SBS. This not only enhances the mechanical stability of film, but also improves its softness and robustness (the strength increases 1.8 times and the toughness increases 2.3 times), thereby greatly extending its durability for information encryption and decryption. When patterned with a photomask, the crosslinked regions maintain transparency upon acetone absorption, while the non-crosslinked regions become opaque due to an acetone-induced phase change. Upon removal of acetone, these opaque regions can be restored to transparency. Compared with hydrogels liable to water loss and deformation, the patterned films show greater stability, retaining pattern encryption/decryption functions after 30 days in a natural environment without special storage. The rate of this phase transition is directly related to the degree of crosslinking. Therefore, by adjusting the degree of crosslinking, the patterned films can undergo multistage encryption/decryption in response to acetone, providing a promising method for information security and storage.

虽然水凝胶可以很容易地实现可逆的信息加密和解密,但当应用于弹性聚合物薄膜时,这一过程面临着重大挑战。这是由于无水聚合物薄膜固有的化学稳定性,这大大增加了信息书写的难度。在这项研究中,我们提出了一种无溶剂自由基聚合方法在聚苯乙烯-丁二烯-苯乙烯(SBS)弹性膜上进行化学图案。与短链交联剂诱导的图案化(增加薄膜的脆性)不同,长链交联剂与SBS链化学键合。这不仅增强了薄膜的机械稳定性,而且提高了薄膜的柔软性和坚固性(强度提高1.8倍,韧性提高2.3倍),从而大大延长了薄膜的信息加密和解密的耐久性。当使用光掩膜时,交联区域在丙酮吸收时保持透明,而非交联区域由于丙酮诱导的相变而变得不透明。除去丙酮后,这些不透明的区域可以恢复透明。与易失水和变形的水凝胶相比,图案膜表现出更大的稳定性,在自然环境中无需特殊储存30天后仍能保持图案加密/解密功能。这种相变的速率与交联的程度直接相关。因此,通过调节交联度,图案膜可以响应丙酮进行多级加密/解密,为信息安全和存储提供了一种很有前途的方法。
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引用次数: 0
Dual functional coordination interactions enable fast polysulfide conversion and robust interphase for high-loading lithium-sulfur batteries. 双功能配位相互作用可实现高负载锂硫电池的快速多硫化物转化和坚固的界面相。
IF 12.2 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-10 DOI: 10.1039/d4mh01504e
Wenchang Han, Jiyue Hou, Fei Wang, Bao Zhang, Enfeng Zhang, Yongqi Wang, Chunman Yang, Peng Dong, Weili Song, Xue Li, Yannan Zhang, Shuaifeng Lou, Yingjie Zhang, Yiyong Zhang

The stable operation of high-capacity lithium-sulfur batteries (LSBs) has been hampered by slow conversion kinetics of lithium polysulfides (LiPSs) and instability of the lithium metal anodes. Herein, 6-(dibutylamino)-1,3,5-triazine-2,4-thiol (DTD) is introduced as a functional additive for accelerating the kinetics of cathodic conversion and modulating the anode interface. We proposed that a coordination interaction mechanism drives the polysulfide conversion and modulates the Li+ solvated structure during the binding of the N-active site of DTD to LiPSs and lithium salts. The results show that DTD effectively promotes the redox of LiPSs and the formation of an inorganic-organic synergistic solid electrolyte interface (SEI). This suppresses the parasitic reaction of LiPSs and confers uniform lithium deposition. Therefore, the capacity decay rate per cycle of the DTD-added LSBs is only 0.066% after 600 cycles at 1C. Moreover, Li-Li symmetric batteries exhibited smaller overpotentials during long cycling and a 41% increment in cycle life. Even with high sulfur loading (5.38 mg cm-2) and a depleted electrolyte sulfur ratio (E/S = 5 μL mg-1), the capacity retention of the battery is 71.5%. This work provides a new reference for elucidating the mechanisms of polysulfide conversion and SEI interface regulation for high-energy-density lithium-sulfur batteries.

高容量锂硫电池(LSBs)的稳定运行一直受到多硫化锂(LiPSs)转化动力学缓慢和锂金属阳极不稳定的影响。本文介绍了6-(二丁胺)-1,3,5-三嗪-2,4-硫醇(DTD)作为加速阴极转化动力学和调节阳极界面的功能添加剂。我们提出了一种配位相互作用机制驱动多硫化物转化,并在DTD的n活性位点与LiPSs和锂盐结合时调节Li+溶剂化结构。结果表明,DTD有效地促进了LiPSs的氧化还原和无机-有机协同固体电解质界面(SEI)的形成。这抑制了LiPSs的寄生反应,并保证了均匀的锂沉积。因此,添加dtd的lsb在1C下循环600次后,每周期的容量衰减率仅为0.066%。此外,锂离子对称电池在长周期循环中表现出较小的过电位,循环寿命增加41%。即使在高硫负荷(5.38 mg cm-2)和耗尽电解液硫比(E/S = 5 μL mg-1)下,电池的容量保持率为71.5%。本研究为阐明高能量密度锂硫电池多硫转化机理和SEI界面调控提供了新的参考。
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Materials Horizons
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