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Connecting adjacent active layers with structural pillars for high-performance Li-organic batteries 用结构柱连接相邻有源层，用于高性能有机锂电池

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-11-01 Epub Date: 2025-03-18 DOI: 10.1016/j.esci.2025.100401

Kun Zhang , You Pan , Xingyu Guo , Jifeng Wang , Chuanfa Li , Jiaxin Li , Meng Liao , Yi Jiang , Wenjun Li , Kailin Zhang , Qian Ye , Longmei Ma , Xiaocheng Gong , Kai Li , Ying Wang , Yue Gao , Xin-Gao Gong , Huisheng Peng , Bingjie Wang

Organic electrode materials with the versatility of molecular engineering emerge as promising alternatives to construct high-performance batteries. However, a weak binding force between active layers leads to poor structural stability accompanied by a multi-electron redox, thus hindering the construction of practical devices based on organic materials. Herein, we report a structural engineering approach to improve the structural stability of organic molecules by pre-intercalating potassium ions (K⁺) as pillars into the adjacent rhodizonate (C₆O₆²⁻) layers. This enhanced binding, with increased coordination sites of K-O, effectively prevents the exfoliation of C₆O₆²⁻ layers and provides stable diffusion channels for lithium ions (Li⁺). The resulting batteries exhibit accelerated reaction kinetics and enhanced Li⁺ diffusion, leading to a high energy density of 722 Wh kg⁻¹ (based on active materials) and reversible capacity of 315 mAh g⁻¹ at 1.0 C, with a capacity retention of 225 mAh g⁻¹ after 500 cycles. In addition, by virtue of the flexible nature, a Li-K₂C₆O₆ battery has been made into flexible fibers for next-generation wearable systems, offering a new avenue for realizing practical devices based on organic single molecules. This work presents a general and efficient strategy to unlock theoretically high-performance organic electrode materials for advanced Li-organic batteries.

有机电极材料具有分子工程的多功能性，是构建高性能电池的有希望的替代品。然而，由于活性层之间的结合力较弱，导致结构稳定性差，并伴有多电子氧化还原，从而阻碍了基于有机材料的实用器件的构建。在此，我们报告了一种结构工程方法，通过将钾离子（K+）作为支柱预插到相邻的rhodizonate （C6O62−）层中来提高有机分子的结构稳定性。随着K-O配位位点的增加，这种增强的结合有效地防止了C6O62−层的脱落，并为锂离子（Li+）提供了稳定的扩散通道。所得电池表现出加速的反应动力学和增强的Li+扩散，导致722 Wh kg−1的高能量密度（基于活性材料）和315 mAh g−1的可逆容量，在1.0℃下循环500次后容量保持为225 mAh g−1。此外，凭借其柔性特性，Li-K2C6O6电池已被制成用于下一代可穿戴系统的柔性纤维，为实现基于有机单分子的实用设备提供了新的途径。这项工作提出了一种通用而有效的策略来解锁理论上高性能的有机锂有机电池电极材料。

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引用次数: 0

External field-assisted catalysis 外场辅助催化

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-11-01 Epub Date: 2025-03-01 DOI: 10.1016/j.esci.2025.100398

Linbo Jiang, Lintao Jiang, Xu Luo, Ruidong Li, Qingqu Zhou, Weihao Zeng, Jun Yu, Lei Chen, Shichun Mu

In recent years, substantial effort has been dedicated to improving the intrinsic catalytic activity of catalysts through structural modification, component regulation, and chemical state optimization. However, complexity in the design and construction of catalysts, and the possibility of encountering performance ceilings, may constrain their widespread use. Currently, the introduction of in situ external fields, such as force, electric, magnetic, acoustic, light, and thermal fields, is an attractive approach to enhance the catalytic efficiency of catalysts. Such in situ physical fields feature continuity, reversibility, and controllability, and can exert external force or energy on catalysts, thereby affecting their microscopic structures and electron arrangements, accelerating their mass transfer and reaction kinetics. Mutual coupling and conversion among different external fields are also worth exploring. Various in situ external field effects work in multifaceted ways to promote catalysis in energy-environment systems by optimizing mass/energy transfer processes, modifying structures, and accelerating catalytic reaction kinetics, thereby significantly improving the catalytic properties of materials. This review summarizes and analyzes the latest developments in external field-assisted methods for boosting catalyst performance. The external field effect, related catalysis mechanism, and external field-enhanced catalysis are highlighted, and we discuss future challenges, countermeasures, and opportunities for external field-assisted catalysis and beyond.

近年来，人们通过结构修饰、组分调节和化学态优化等方法来提高催化剂的内在催化活性。然而，催化剂设计和结构的复杂性，以及遇到性能上限的可能性，可能会限制它们的广泛应用。目前，引入原位外场，如力场、电场、磁场、声场、光场和热场，是提高催化剂催化效率的一种有吸引力的方法。这种原位物理场具有连续性、可逆性和可控性，可以对催化剂施加外力或能量，从而影响催化剂的微观结构和电子排列，加速催化剂的传质和反应动力学。不同外场之间的相互耦合和转换也值得探讨。各种原位外场效应通过优化质量/能量传递过程、修饰结构、加速催化反应动力学等方式，以多方面的方式促进能量-环境系统中的催化，从而显著提高材料的催化性能。本文综述和分析了外场辅助方法在提高催化剂性能方面的最新进展。重点介绍了外场效应、相关的催化机理和外场增强催化，并讨论了外场辅助催化未来的挑战、对策和机遇。

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引用次数: 0

Multifunctional robotic electrofluid for soft fluidic actuation 用于软流体驱动的多功能机器人电流体

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-11-01 Epub Date: 2025-07-04 DOI: 10.1016/j.esci.2025.100448

Wei Tang , Pingan Zhu , Yu Hu, Xinyu Guo, Yonghao Wang, Kecheng Qin, Yiding Zhong, Qincheng Sheng, Huxiu Xu, Zhaoyang Li, Huayong Yang, Jun Zou

Like the vital role that multifunctional biological fluids play in living organisms, leveraging fluid multifunctionality offers a promising approach to enhance system capabilities without overcomplicating the hardware. However, creating a multifunctional fluid for soft fluidic systems remains a persistent challenge. Here, we report a multifunctional electrofluid that integrates actuation, sensing, self-healing, damage detection, and triboelectricity powering for the various function requirements of soft fluidic systems. We demonstrate that actuation, sensing, and damage detection can be achieved by activating electrons in the working fluid, and the system enables underwater self-healing through the incorporation of water-reactive self-healing agents into the working fluid. In addition, we achieve the fluid flow by transporting the electrons gathered by the triboelectric nanogenerator into the fluid, thereby making the system become a triboelectricity-powered machine. The fluid module developed based on electrofluids is self-contained and plug-and-play, providing good convenience for rapid construction of soft fluidic systems. We validate the effectiveness of the electronic fluids through soft robotic fish, soft octobot, and wearable devices, demonstrating that the proposed fluid enables multiple functions of the system without added weight or volume. As such, the proposed electrofluid provides a promising platform to achieve high integration and lightweight of multifunctional soft fluidic actuation by expanding the functionalities of the fluid itself.

就像多功能生物流体在生物体中发挥的重要作用一样，利用流体的多功能提供了一种很有前途的方法，可以在不使硬件过度复杂化的情况下增强系统功能。然而，为软流体系统创造多功能流体仍然是一个持续的挑战。在这里，我们报道了一种多功能电流体，它集成了驱动、传感、自愈、损伤检测和摩擦电供电，可满足软流体系统的各种功能要求。我们证明，通过激活工作流体中的电子，可以实现驱动、传感和损伤检测，并且通过在工作流体中加入水反应性自修复剂，该系统可以实现水下自修复。此外，我们通过将摩擦电纳米发电机收集的电子传输到流体中来实现流体的流动，从而使系统成为摩擦电驱动的机器。基于电流体开发的流体模块具有自成一体、即插即用的特点，为软流体系统的快速构建提供了良好的便利。我们通过软机器鱼、软章鱼机器人和可穿戴设备验证了电子流体的有效性，证明了所提出的流体可以在不增加重量或体积的情况下实现系统的多种功能。因此，所提出的电流体通过扩展流体本身的功能，为实现多功能软流体驱动的高集成度和轻量化提供了一个有前途的平台。

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引用次数: 0

Li-rich oxide micro-bricks with exposed {010} planes to construct ultrahigh-compaction hierarchical cathodes for Li-ion batteries 具有暴露{010}平面的富锂氧化物微砖用于构建锂离子电池的超高压实分层阴极

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-09-01 Epub Date: 2025-04-03 DOI: 10.1016/j.esci.2025.100405

Yongjian Li , Tong Sun , Chenxing Yang , Yuefeng Su , Cai Liu , Xinyu Zhu , Yihong Wang , Siyuan Ma , Xinyu Wang , Yizhi Zhai , Wenlong Kang , Lai Chen , Meng Wang , Liang Zhang , Bin Wang , Qing Huang , Yibiao Guan , Feng Wu , Ning Li

Although lithium-rich manganese-based (LRM) cathode materials have high capacity (> 250 mAh g⁻¹) due to their multi-electron redox mechanisms and offer cost advantages due to their high Mn content, challenges remain before they can achieve commercialization as replacements for lithium cobalt oxides which have high volumetric energy density. Here, we construct a hierarchically structured LRM cathode, featuring primary micro-bricks and abundant exposure of lithium-ion active transport facets ({010} planes). Benefiting from these densely packed bricks and rapid lithium-ion active planes, the hierarchical material achieves an optimal compaction density of 3.4 g cm⁻³ and an ultrahigh volumetric energy density of 3431.0 Wh L⁻¹, which is the highest performance level to date. Advanced characterizations, including hard X-ray absorption spectra and wide-angle X-ray scattering spectra, combined with density functional theory calculations, demonstrate that the hierarchical material shows a highly reversible charge compensation process and low-strain structural evolution. In addition, when the material has appropriate Li/Ni intermixing, it is not prone to shearing or sliding along the two-dimensional lithium-ion diffusion planes, which promotes robust architectural stability under high-pressure calendering and long-term cycling. This work should promote the development of advanced cathode materials for rechargeable batteries with high volumetric energy density.

尽管富锂锰基（LRM）正极材料由于其多电子氧化还原机制而具有高容量（> 250 mAh g - 1），并且由于其高锰含量而具有成本优势，但在它们作为具有高体积能量密度的锂钴氧化物的替代品实现商业化之前仍然存在挑战。在这里，我们构建了一个分层结构的LRM阴极，具有初级微砖和大量暴露的锂离子主动输运面（{010}平面）。得益于这些密集堆积的砖块和快速锂离子活性层，分层材料实现了3.4 g cm−3的最佳压实密度和3431.0 Wh L−1的超高体积能量密度，这是迄今为止的最高性能水平。通过硬x射线吸收光谱和广角x射线散射光谱的高级表征，结合密度泛函理论计算，表明分层材料表现出高度可逆的电荷补偿过程和低应变的结构演化。此外，当材料具有适当的Li/Ni混合时，它不容易沿着二维锂离子扩散面剪切或滑动，从而在高压压延和长期循环下促进了强大的结构稳定性。这项工作将促进高体积能量密度可充电电池正极材料的发展。

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引用次数: 0

Adsorption-attraction electrolyte addressing anion-deficient interface for lithium metal batteries 锂金属电池阴离子缺乏界面的吸附-吸引电解质

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-09-01 Epub Date: 2025-03-08 DOI: 10.1016/j.esci.2025.100399

Pengbin Lai , Yaqi Zhang , Junhao Wang , Minghui Chen , Xinyu Li , Xiaodie Deng , Qichen Chen , Boyang Huang , Chaolun Gan , Yeguo Zou , Yu Qiao , Peng Zhang , Jinbao Zhao

Constructing an optimal solid–electrolyte interphase (SEI) through electrolyte strategies is an effective approach to suppress lithium dendrites and improve deposition/stripping reversibility. Specifically, increasing the proportion of anion coordination in the inner Li⁺ solvation sheath promotes the formation of an anion-derived SEI that features a high content of inorganic components favoring Li⁺ diffusion. However, whether this anion-rich structure can persist during cycling has not been dynamically investigated. In this work, we not only construct a favorable solvation structure but also study its evolution in both bulk and interface regions across varying temperatures. Additionally, we employ the unique “adsorption-attraction” mechanism of trifluoromethoxybenzene (PhOCF₃) solvent to inhibit the undesirable transition from an “anion-rich” to “anion-deficient” structure at the anode interface, which is confirmed by 2D NMR and in situ infrared spectroscopy. In summary, this work explores the solvation structure in depth and proposes new perspectives on designing electrolytes for lithium metal batteries.

通过电解质策略构建最佳固-电解质间相（SEI）是抑制锂枝晶和提高沉积/剥离可逆性的有效途径。具体来说，增加内部Li+溶剂化鞘中阴离子配位的比例，促进阴离子衍生SEI的形成，该SEI具有高含量的无机成分，有利于Li+的扩散。然而，这种富含阴离子的结构是否能在循环过程中持续存在尚未得到动态研究。在这项工作中，我们不仅构建了一个有利的溶剂化结构，而且研究了它在不同温度下在体区和界面区的演变。此外，我们利用三氟甲氧基苯（PhOCF3）溶剂独特的“吸附-吸引”机制，抑制了阳极界面从“富阴离子”到“缺阴离子”结构的不良转变，这一点得到了二维核磁共振和原位红外光谱的证实。综上所述，本研究深入探讨了溶剂化结构，为锂金属电池电解质的设计提供了新的视角。

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引用次数: 0

Advanced implantable energy storage for powering medical devices 为医疗设备供电的先进植入式能量存储

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-09-01 Epub Date: 2025-04-18 DOI: 10.1016/j.esci.2025.100409

Shasha Wang , Leqian Wei , Fujun Wang , Lu Wang , Jifu Mao

Implantable electronic medical devices (IEMDs) are revolutionary advancements in healthcare, enabling continuous health monitoring and disease treatments. To support their further development, IESDs that include supercapacitors (SCs) and batteries are now garnering intensive worldwide research efforts. In this review, we discuss and analyze the research advancements and challenges associated with batteries and SCs in the realm of IESDs. First, we summarize the main components of IESDs, including electrodes, electrolytes, and encapsulation materials. Subsequently, we elucidate the main application scenarios of multifunctional energy storage devices, specifically biosafe, stretchable/self-healing, biodegradable, miniaturized, injectable, and edible IESDs. We then summarize research progress to date on the integration of IESDs with energy harvesters and wireless charging. State-of-the-art studies of IESDs categorized by human organ systems are covered in depth, including cardiovascular, nervous, gastrointestinal, musculoskeletal, vision, and systemic recording and stimulation. We close by briefly outlining the challenges and future prospects for IESDs.

植入式电子医疗设备（iemd）是医疗保健领域的革命性进步，能够实现持续的健康监测和疾病治疗。为了支持它们的进一步发展，包括超级电容器（sc）和电池在内的iesd目前正在全球范围内进行密集的研究。在本文中，我们讨论和分析了与iesd领域的电池和sc相关的研究进展和挑战。首先，我们总结了iesd的主要组成部分，包括电极、电解质和封装材料。随后，我们阐述了多功能储能器件的主要应用场景，特别是生物安全、可拉伸/自修复、可生物降解、小型化、可注射和可食用的iesd。然后总结了迄今为止iesd与能量收集器和无线充电集成的研究进展。以人体器官系统分类的IESDs的最新研究深入涵盖，包括心血管，神经，胃肠道，肌肉骨骼，视觉和系统记录和刺激。最后，我们简要概述了可持续发展领域面临的挑战和未来前景。

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引用次数: 0

Precise Pt-skin manipulation of strain and ligand effects for oxygen reduction 精确的Pt-skin操作应变和配体对氧还原的影响

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-09-01 Epub Date: 2025-02-26 DOI: 10.1016/j.esci.2025.100396

Yizhe Chen , Zeyu Jin , Jialin Sun , Shengli Chen , Jiujun Zhang , Shiming Zhang

Nanostructured platinum (Pt)-skin alloys are promising electrocatalysts for oxygen reduction reaction (ORR) due to their tunable strain and ligand effects which essentially regulate the surface electronic structures. In addition to the chemical nature of alloying elements, the layer numbers of Pt-skin crucially determine the strain and ligand effects. So far, the effects of Pt-skin layer numbers have been generally investigated through vapor deposition on bulk metals and alloys with extended surfaces, while the precise Pt-skin control of nanostructured alloy electrocatalysts in wet chemical synthesis remains fairly challenging. Herein, we develop a Pt-skin engineering strategy to construct a family of dendrite-like porous PtCu@Pt_nL nanospheres (NSs) with precisely controlled Pt-skin layers by adjusting the reducibility of Cu ions. Density functional theory calculations and X-ray photoelectron spectroscopy-based valence band spectra results indicate a concave parabolic trend of d-band center with varying the Pt-skin layer from 0 to 5, jointly resulting from the skin layer-dependent electron transfer numbers and compression strain. The two-layer Pt-skin alloy, PtCu@Pt_2L NS, is identified to have the lowest d-band center and therefore locates at the summit of ORR activity volcano. Accordingly, this carbon supported PtCu@Pt_2L NSs catalyst achieves excellent ORR electrocatalysis in H₂–O₂ proton exchange membrane fuel cells.

纳米结构铂皮合金具有应变和配体可调节表面电子结构的特性，是氧还原反应（ORR）的电催化剂。除了合金元素的化学性质外，铂皮的层数也决定了应变和配体效应。到目前为止，Pt-skin层数的影响一般是通过气相沉积在具有扩展表面的大块金属和合金上进行研究，而在湿化学合成中精确控制纳米结构合金电催化剂的Pt-skin仍然是相当具有挑战性的。在此，我们开发了一种Pt-skin工程策略，通过调节Cu离子的还原性，构建了一个具有精确控制Pt-skin层的枝状多孔PtCu@PtnL纳米球（NSs）家族。密度泛函理论计算和基于x射线光电子能谱的价带谱结果表明，随着pt蒙皮层数从0到5的变化，d带中心呈凹抛物线趋势，这是由蒙皮层依赖的电子转移数和压缩应变共同造成的。两层pt皮合金PtCu@Pt2L NS的d波段中心最低，因此位于ORR活火山顶部。因此，该碳负载PtCu@Pt2L NSs催化剂在H2-O2质子交换膜燃料电池中实现了优异的ORR电催化。

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引用次数: 0

Game changers: scavenging materials for nonaqueous rechargeable battery applications 游戏改变者：非水可充电电池应用的清除材料

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-09-01 Epub Date: 2025-04-30 DOI: 10.1016/j.esci.2025.100411

Xing Chen , Huanrui Zhang , Cizhen Luo , Chenhui Gao , Chenghao Sun , Rongxian Wu , Yifan Gong , Pengzhou Mu , Qingfu Wang , Guanglei Cui

Many potentially harmful reactive species are either present in nonaqueous rechargeable batteries or generated during their operation, with very negative effects on battery performance and/or safety. Scavenging materials have emerged as game changers, capable of directly eliminating and reducing the negative impact rendered by detrimental reactive species and thereby significantly improving battery performance and/or safety. This discussion introduces the origin of harmful species such as water and hydrofluoric acid, phosphorus pentafluoride, metal dendrites, combustion free radicals, active oxygen species and free radicals, as well as gaseous side products, and their adverse effects on battery performance and/or safety. We then describe and discuss scavenging materials having various structural characteristics and reaction chemistries with detrimental reactive species, as well as their positive role on battery performance and/or safety with respect to prominent nonaqueous rechargeable batteries, including lithium, sodium, zinc, and magnesium batteries. In addition, we outline the limitations of scavenging materials and the analysis techniques used in scavenging chemistry. The paper closes by offering perspectives on future development directions for scavenging chemistries in the realm of nonaqueous rechargeable battery applications. This comprehensive discussion will help to stimulate further advancements in novel scavenging materials for use in nonaqueous rechargeable battery applications.

许多潜在的有害反应物质要么存在于非水可充电电池中，要么在其运行过程中产生，对电池性能和/或安全性产生非常负面的影响。清除材料已经成为游戏规则的改变者，能够直接消除和减少有害反应物质带来的负面影响，从而显著提高电池性能和/或安全性。本讨论介绍了水和氢氟酸、五氟化磷、金属枝晶、燃烧自由基、活性氧和自由基以及气态副产物等有害物质的来源及其对电池性能和/或安全的不利影响。然后，我们描述并讨论了具有各种结构特征和具有有害活性物质的反应化学的清除材料，以及它们对电池性能和/或安全性的积极作用，包括锂、钠、锌和镁电池。此外，我们概述了清除材料的局限性和清除化学中使用的分析技术。论文最后提出了在非水可充电电池应用领域中清除化学物质的未来发展方向。这一全面的讨论将有助于促进用于非水可充电电池应用的新型清除材料的进一步发展。

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引用次数: 0

Pulsed laser-tuned ruthenium@carbon interface for self-powered hydrogen production via zinc–hydrazine battery coupled hybrid electrolysis 脉冲激光调谐ruthenium@carbon接口，通过锌-肼电池耦合混合电解自供电制氢

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-09-01 Epub Date: 2025-04-11 DOI: 10.1016/j.esci.2025.100408

Huieun Ahn , Raja Arumugam Senthil , Sieon Jung , Anuj Kumar , Mohd Ubaidullah , Myong Yong Choi

Herein, we report the synthesis of selectively face-centered cubic structured ruthenium nanospheres covered in graphitic carbon (denoted as Ru@C) using an effective and innovative pulsed laser ablation in liquid strategy. The Ru@C‒200 catalyst exhibited a low overpotential of 48 mV for hydrogen evolution reaction (HER) and an ultralow oxidation potential of −8 mV (vs. reversible hydrogen electrode) for hydrazine oxidation reaction (HzOR) at 10 mA cm⁻², maintaining long-term durability for over 100 h, demonstrating its dual-functional activity. This performance was attributed to the robust synergistic coupling between the Ru core and C shell, as confirmed by in situ electrochemical studies and density functional theory investigations. As a result, overall hydrazine splitting (OHzS) in the Ru@C‒200||Ru@C‒200 system requires only low cell voltages of 0.11 and 0.70 V at 10 and 100 mA cm⁻², respectively. Moreover, a rechargeable zinc–hydrazine (Zn–Hz) battery, fabricated using the Ru@C‒200 catalyst as the cathode and Zn foil as the anode, exhibited a high energy efficiency of 90% and efficient H₂ production, validating its remarkable ability for practical applications. Notably, coupling Zn–Hz battery with OHzS system encourages self-powered H₂ production. This study provides potential guidance for engineering robust electrocatalysts for large-scale H₂ production while purifying hydrazine-containing industrial sewage.

在此，我们报告了使用有效和创新的液体脉冲激光烧蚀策略合成石墨碳覆盖的选择性面心立方结构钌纳米球（表示为Ru@C）。Ru@C -200催化剂在10 mA cm−2下，析氢反应（HER）的过电位为48 mV，肼氧化反应（HzOR）的氧化电位为- 8 mV（相对于可逆氢电极），保持了超过100 h的长期使用寿命，显示了其双功能活性。现场电化学研究和密度泛函理论研究证实，这种性能归因于Ru芯和C壳之间强大的协同耦合。因此，在Ru@C -200 ||Ru@C -200体系中，总肼分裂（OHzS）只需要在10和100 mA cm - 2下分别为0.11 V和0.70 V的低电池电压。此外，以Ru@C -200催化剂为阴极，锌箔为阳极制备的可充电锌-肼（Zn - hz）电池，具有高达90%的高能效和高效的产氢能力，验证了其卓越的实际应用能力。值得注意的是，将Zn-Hz电池与OHzS系统耦合可以促进自供电制氢。该研究为大规模制氢同时净化含肼工业污水的工程稳健电催化剂提供了潜在的指导。

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引用次数: 0

Bridging graphene for films with superior mechanical and electrical performance for electromagnetic interference shielding 桥接石墨烯薄膜具有优越的机械和电气性能，用于电磁干扰屏蔽

IF 36.6 Q1 ELECTROCHEMISTRY

eScience

Pub Date : 2025-09-01 Epub Date: 2025-04-10 DOI: 10.1016/j.esci.2025.100407

Jiawen Zhang , Tianqi Xu , Ling Ding , Jinpeng Ji , Jianxin Geng , Huynh Thien Ngo , Ke Zhou , Xiankai Chen , Fengxia Geng

Macroscopic films assembled from graphene sheets could be ideal for lightweight and flexible electromagnetic interference shielding applications if the excellent mechanical strength and electrical conductivity of individual graphene can be replicated on the macroscale. However, in practice, a large performance gap remains between individual graphene and graphene-based macroscopic films. In this work, we report macroscopic graphene-based films with high mechanical strength and electrical conductivity (1.70 ± 0.05 GPa and 1170 ± 60 S cm⁻¹) obtained by introducing a covalent conjugating aromatic amide group to bridge graphene edges. The bridging was achieved by reacting a doctor-bladed GO film with 1,2,4,5-benzenetetraamine hydrochloride followed by chemical reduction. Impact load tests demonstrated efficient stress transfer in these films, with stress spread uniformly well beyond the impact area. This is in sharp contrast to previously reported films, which showed the immediate initiation of cracks followed by crack extension in random directions. Our conducting films achieved a shielding effectiveness of 114.1 dB for a 120 μm thick film, and the specific shielding effectiveness was calculated to be 67.9 dB cm³ g⁻¹, which significantly exceeds those of currently known shielding materials as well as graphene films synthesized under similar conditions without thermal annealing. Owing to the graphene films’ mechanical robustness, the shielding performance was maintained even after repeated folding.

如果单个石墨烯优异的机械强度和导电性可以在宏观尺度上复制，那么由石墨烯片组装而成的宏观薄膜将是轻质和柔性电磁干扰屏蔽应用的理想选择。然而，在实际应用中，单个石墨烯和石墨烯基宏观薄膜之间仍然存在很大的性能差距。在这项工作中，我们报道了通过引入共价共轭芳酰胺基团来桥接石墨烯边缘而获得的具有高机械强度和电导率（1.70±0.05 GPa和1170±60 S cm−1）的宏观石墨烯基薄膜。桥接是通过将氧化石墨烯薄膜与1,2,4,5-苯四胺盐酸盐反应，然后进行化学还原来实现的。冲击载荷试验表明，在这些薄膜中有效的应力传递，应力均匀地扩散到冲击区域之外。这与先前报道的薄膜形成鲜明对比，后者显示裂纹立即开始，随后裂纹向随机方向扩展。在120 μm厚的薄膜上，我们的导电膜的屏蔽效率达到114.1 dB，比屏蔽效率为67.9 dB cm3 g−1，大大超过了目前已知的屏蔽材料以及在类似条件下未经热处理合成的石墨烯薄膜。由于石墨烯薄膜的机械坚固性，即使经过多次折叠也能保持屏蔽性能。

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引用次数: 0