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Creating continuously graded microstructures via electrochemically altering grain boundary complexions 通过电化学改变晶界复合体创建连续分级微结构
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-03-01 DOI: 10.1016/j.mattod.2024.01.008
Qizhang Yan , Chongze Hu , Jian Luo

Tailoring microstructures represents a daunting goal in materials science. Here, an innovative proposition is to utilize grain boundary (GB) complexions (a.k.a. interfacial phases) to manipulate microstructural evolution, which is challenging to control via only temperature and doping. Herein, we use ZnO as a model system to tailor microstructures using applied electric fields as a new “knob” to control GB structures locally via field-driven defects polarization. Specifically, continuously graded microstructures are created under applied electric fields. By employing aberration-corrected scanning transmission electron microscopy (AC STEM) in conjunction with density functional theory (DFT) and ab initio molecular dynamics (AIMD), we discover cation-deficient, oxygen-rich GBs near the anode with enhanced GB diffusivities. In addition, the field-driven redistribution of cation vacancies is deduced from a defect chemistry model, and subsequently verified by spatially resolved photoluminescence spectroscopy. This bulk defects polarization leads to preferential formation of cation-deficient (oxidized) GBs near the anode to gradually promote grain growth towards the anode. This mechanism can be utilized to create continuously graded microstructures without abnormal grain growth typically observed in prior studies. This study exemplifies a case of tailoring microstructural evolution via altering GB complexions locally with applied electric fields, and it enriches fundamental GB science.

定制微结构是材料科学领域的一个艰巨目标。在这里,一个创新性的主张是利用晶界(GB)复合(又称界面相)来操纵微结构演化,而仅通过温度和掺杂来控制微结构演化是具有挑战性的。在此,我们以氧化锌为模型系统,利用外加电场作为新的 "旋钮 "来定制微结构,通过电场驱动的缺陷极化来局部控制 GB 结构。具体来说,就是在外加电场下创建连续分级的微结构。通过将像差校正扫描透射电子显微镜(AC STEM)与密度泛函理论(DFT)和非初始分子动力学(AIMD)相结合,我们在阳极附近发现了阳离子缺乏、富含氧的 GB,并增强了 GB 的扩散性。此外,我们还从缺陷化学模型中推导出了场驱动的阳离子空位再分布,并随后通过空间分辨光致发光光谱进行了验证。这种块体缺陷极化导致阳极附近优先形成阳离子缺失(氧化)的 GB,从而逐渐促进晶粒向阳极生长。利用这种机制可以产生连续分级的微结构,而不会出现之前研究中通常观察到的异常晶粒生长。这项研究是通过外加电场局部改变 GB 复合物来定制微结构演变的一个实例,它丰富了 GB 的基础科学。
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引用次数: 0
Metallic meshes for advanced flexible optoelectronic devices 用于先进柔性光电器件的金属网格
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-03-01 DOI: 10.1016/j.mattod.2024.01.006
Yufan Zhang , Zeren Lu , Xinran Zhou , Jiaqing Xiong

Metallic meshes (MMs) are promising for replacement of traditional brittle metal oxide conductors to serve as flexible transparent devices for applications such as environment, energy, display, and human–machine-environment interface. The diversities of MMs in materials, fabrication mechanisms, geometrics and performances extend their applications, however the systematization of this field is rarely concerned. Here, this article summarizes fabrication strategies of MMs in terms of using hard or soft templates, which produce regular-patterned meshes or random-patterned meshes, emphasizing large scale production technology free of templates would lead the development of MMs. Secondly, mechanisms and strategies are highlighted in terms of enhancement of MMs in optoelectronic properties, thermal, chemical, and mechanical stability that are crucial for adapting different application scenarios. Accordingly, the representative applications of MMs in filters, shielding materials, nanogenerators, supercapacitors, solar cells, light-emitting devices, electroluminescent devices, smart windows, thermal management equipment, sensors, and touch panels are introduced, reflecting their respective advantages in diverse applications. Finally, promising solutions to balance the optoelectronic properties and the stability and durability of MMs are proposed to adapt to complex and extreme applications. It is convinced that this review can provide a comprehensive understanding to guide and promote the future development of flexible optoelectronic devices.

金属网格(MMs)有望取代传统的脆性金属氧化物导体,成为环境、能源、显示和人机环境界面等应用领域的柔性透明器件。MMs 在材料、制造机制、几何形状和性能方面的多样性扩展了其应用范围,但这一领域的系统化研究却很少受到关注。本文从使用硬模板或软模板、产生规则图案网格或随机图案网格的角度,总结了 MMs 的制造策略,强调无模板的大规模生产技术将引领 MMs 的发展。其次,强调了 MMs 在光电特性、热稳定性、化学稳定性和机械稳定性方面的增强机制和策略,这对于适应不同的应用场景至关重要。因此,介绍了 MMs 在滤波器、屏蔽材料、纳米发电机、超级电容器、太阳能电池、发光器件、电致发光器件、智能窗户、热管理设备、传感器和触摸屏中的代表性应用,反映了它们在不同应用中的各自优势。最后,还提出了在 MMs 的光电特性与稳定性和耐用性之间取得平衡的可行方案,以适应复杂和极端的应用。相信这篇综述能为指导和促进柔性光电器件的未来发展提供一个全面的认识。
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引用次数: 0
Ultrasensitive quantum capacitance detector at the edge of graphene 石墨烯边缘超灵敏量子电容探测器
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-03-01 DOI: 10.1016/j.mattod.2023.12.011
Yujia Huang , Lei Bao , Yi Li , Xuefei Zhang , Zijian Zhang , Ruopeng Cui , Hongwei Zhu , Chunlei Wan , Wangyang Fu

Graphene, with its outstanding electrical properties, has appealed to the attention of researchers all over the world for biosensing applications. So far, much of the research has been conducted on the field-effect modulations of carriers in the basal plane of graphene after adsorbing charged biomolecules. However, another essential aspect--the graphene edge--has been largely ignored due to the difficulties in both manufacture and characterization. Here, we propose a facile intercalation and pressure sintering approach that enables the fabrication and exposure of only graphene edges. The quantum capacitance of the exposed edges is proportional to the local density of state (DOS) and can be harvested for biochemical sensing. Notably, due to fringe electric field enhancement and biomolecular convergence at the one-dimensional graphene edges, we are able to detect four representative amino acids at 0.01 fg/mL concentrations within several minutes. These achievements in innovative quantum capacitance measurements of graphene edges, combined with simple and robust device fabrication by eliminating complex micro-nano processing, offer a new avenue for the next generation of biochemical sensors with ever-demanding sensitivities.

石墨烯具有出色的电学特性,在生物传感应用方面吸引了全世界研究人员的关注。迄今为止,大部分研究都是针对石墨烯吸附带电生物分子后基底面载流子的场效应调制。然而,由于制造和表征方面的困难,石墨烯边缘这一重要方面在很大程度上被忽视了。在这里,我们提出了一种简便的插层和压力烧结方法,这种方法可以只制造和暴露石墨烯边缘。暴露边缘的量子电容与局部状态密度(DOS)成正比,可用于生化传感。值得注意的是,由于一维石墨烯边缘的边缘电场增强和生物分子会聚,我们能够在几分钟内检测到浓度为 0.01 fg/mL 的四种代表性氨基酸。这些石墨烯边缘创新量子电容测量方面的成就,再加上通过消除复杂的微纳加工而实现的简单而稳健的器件制造,为灵敏度要求不断提高的下一代生化传感器提供了一条新途径。
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引用次数: 0
MXene guides microwaves through 3D polymeric structures MXene 引导微波穿过三维聚合物结构
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-03-01 DOI: 10.1016/j.mattod.2023.12.013
Omid Niksan , Lingyi Bi , Kasra Khorsand Kazemi , Roman Rakhmanov , Yury Gogotsi , Mohammad H. Zarifi

With the advances in space technology, weight reduction of components has been a paramount, yet challenging task. Additive manufacturing with high-performance polymers can realize lightweight and complex geometries that can also be manufactured on board. Yet polymers are electromagnetically inefficient for applications requiring electrical conductivity, such as guiding microwave signals. This work presents high-efficiency and lightweight additively-manufactured microwave components enabled by MXene coating. The waveguiding functionality was observed from 8 to 33 GHz, covering low earth orbit (LEO) frequencies, with a power-handling capability of up to 10 dB and a transmission coefficient of 93 %. After a single dip-coating cycle, the polymer waveguide performed only 2 % below an eight times heavier metallic equivalent. Frequency/polarization filtering was enabled by implementing special geometries, and a range of microwave functionalities, including resonance, was demonstrated. The MXene-coated components can replace 3D-printed and bulk metals, greatly decreasing weight and cost in space, and also in various terrestrial applications.

随着航天技术的发展,减轻部件重量一直是一项至关重要但又极具挑战性的任务。使用高性能聚合物进行增材制造可以实现轻质、复杂的几何形状,而且还可以在船上制造。然而,对于需要导电性的应用(如引导微波信号)而言,聚合物的电磁效率较低。这项研究通过 MXene 涂层实现了高效、轻质的快速制造微波元件。波导功能的频率范围为 8 至 33 GHz,覆盖低地球轨道(LEO)频率,功率处理能力高达 10 dB,传输系数为 93%。经过一个浸涂周期后,聚合物波导的性能仅比重八倍的金属波导低 2%。通过采用特殊的几何结构实现了频率/极化滤波,并展示了包括共振在内的一系列微波功能。MXene 涂层组件可以取代 3D 打印和块状金属,从而大大降低太空以及各种地面应用的重量和成本。
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引用次数: 0
Electrocatalytic upgrading of nitrogenous wastes into value-added chemicals: A review 将含氮废物电催化升级为增值化学品:综述
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-03-01 DOI: 10.1016/j.mattod.2024.01.009
Jiawei Liu , Zeyu Li , Chade Lv , Xian-Yi Tan , Carmen Lee , Xian Jun Loh , Ming Hui Chua , Zibiao Li , Hongge Pan , Jian Chen , Qiang Zhu , Jianwei Xu , Qingyu Yan

In response to the ever-increasing global population and the growing demand for energy and food, human activities have exerted a substantial impact on the global nitrogen cycles. In this context, the electrocatalytic upgrading of nitrogenous wastes into high-value chemicals under ambient conditions, ideally powered by renewable electricity, emerges as a promising approach to concurrently manage nitrogen-containing wastes and facilitate sustainable production of valuable chemicals. This review presents the electrochemical “waste-to-valuables” concept by discussing its practicality in terms of waste removal efficiency, valuable production efficiency, downstream recovery of valuables, potential applications, and economic feasibility. Specifically, the electrocatalytic upgrading of nitrogenous wastes, i.e., nitric oxide and nitrate as representative air and aqueous pollutants, respectively, into high-value-added chemicals, i.e., ammonia via nitric oxide/nitrate reduction and urea/amide/amine via nitrogen-integrated carbon dioxide reduction is focused. Targeting nitrogenous waste exhausts/streams with low/high concentrations, reactor design and catalyst design principles are reviewed with representative examples. Finally, the major challenges and opportunities associated with the practical applications of the “waste-to-valuables” concept are discussed.

随着全球人口的不断增加以及对能源和食品需求的不断增长,人类活动对全球氮循环产生了重大影响。在这种情况下,在环境条件下,以可再生电力为理想动力,将含氮废物电催化升级为高价值化学品,不失为一种既能管理含氮废物,又能促进有价值化学品可持续生产的有效方法。本综述介绍了电化学 "从废物到有价物品 "的概念,从废物去除效率、有价物品生产效率、有价物品下游回收、潜在应用和经济可行性等方面讨论了这一概念的实用性。具体而言,重点讨论了电催化将含氮废物(即分别作为代表性空气污染物和水污染物的一氧化氮和硝酸盐)升级为高附加值化学品的问题,即通过一氧化氮/硝酸盐还原法将氨转化为高附加值化学品,以及通过氮整合二氧化碳还原法将尿素/酰胺/胺转化为高附加值化学品。针对低浓度/高浓度含氮废气/废流,通过代表性实例回顾了反应器设计和催化剂设计原则。最后,讨论了与 "变废为宝 "概念的实际应用相关的主要挑战和机遇。
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引用次数: 0
Self-assembled liquid metal nanoporous film with durability for efficient phase-change thermal energy management via surface and interface engineering 通过表面和界面工程实现具有耐久性的自组装液态金属纳米多孔膜,用于高效相变热能管理
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-03-01 DOI: 10.1016/j.mattod.2024.01.007
Ben Chu , Bo Liu , Benwei Fu , Ruitong Wang , Weizheng Cheng , Peng Tao , Chengyi Song , Wen Shang , Michael D. Dickey , Tao Deng

Films with nanoengineered surfaces have found extensive utilization in versatile applications, such as freshwater harvesting, water purification, steam generation and thermal energy management. Herein, we develop a liquid metal (LM) nanoporous film on a copper substrate via a simple and scalable bubble-induced self-assembly method. The LM nanoporous film not only provides abundant nucleation sites of bubbles due to nanoscale pores, but also generates CuGa2 intermetallic compound (IMC) as a thermal interface layer with low interfacial resistance due to in situ alloying with the copper substrate. When the film is used in ethanol-based boiling system, it shows a 172% enhanced heat transfer coefficient compared to the pristine copper. In addition, the metallic wetting force between the LM nanoporous film and CuGa2 IMC results in a durable nanoporous film. When the LM nanoporous film is utilized for the phase-change thermal energy management of a high-power-density light emitting diode, it leads to a distinct decrease in temperature by 20.7 ℃ relative to the pristine copper. This work provides a strategy to combine nanoengineered surfaces with interface engineering to enhance phase-change heat transfer, which can result in efficient energy transport in various energy-related applications.

具有纳米工程表面的薄膜已被广泛应用于多种领域,如淡水收集、水净化、蒸汽发电和热能管理。在此,我们通过一种简单且可扩展的气泡诱导自组装方法,在铜基底上开发了一种液态金属(LM)纳米多孔薄膜。液态金属纳米多孔膜不仅因其纳米级孔隙而提供了丰富的气泡成核位点,而且由于与铜基底的原位合金化,还生成了 CuGa2 金属间化合物(IMC)作为热界面层,具有较低的界面电阻。当薄膜用于乙醇沸腾体系时,其传热系数比原始铜提高了 172%。此外,LM 纳米多孔薄膜与 CuGa2 IMC 之间的金属润湿力使纳米多孔薄膜经久耐用。将 LM 纳米多孔膜用于高功率密度发光二极管的相变热能管理时,与原始铜相比,温度明显降低了 20.7 ℃。这项工作提供了一种将纳米工程表面与界面工程相结合以增强相变传热的策略,从而在各种能源相关应用中实现高效的能量传输。
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引用次数: 0
Asymmetric structural design of a highly oriented multi-resonance emitter enables a record 41.5% external quantum efficiency in deep-blue OLED 高度定向多共振发射器的不对称结构设计使深蓝色有机发光二极管的外部量子效率达到创纪录的 41.5
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-03-01 DOI: 10.1016/j.mattod.2024.01.003
Guomeng Li , Mingxu Du , Tianjiao Fan , Xiaofeng Luo , Lian Duan , Yuewei Zhang

Narrowband emitters offer significant advantages in the fabrication of next-generation deep-blue organic light-emitting diodes (OLEDs) due to their wide color gamut, high stability, and high efficiency. It is a pressing challenge to increase the light outcoupling efficiency to further boost device performance, even though 100% internal quantum efficiency is already achievable through rational molecular design. Here, we strategically propose a novel asymmetric structure design strategy aimed at simultaneously optimizing the horizontal emitting dipole orientation and aggregation state properties of the deep-blue multi-resonance (MR) emitters. This proof-of-concept emitter A-BN is capable of displaying ultrapure deep-blue emission with a peak of ∼461 nm, a small full-width-at-half-maximum of ∼25 nm, a CIEy coordinate of ∼0.08, a high horizontal dipole ratio of ∼90 %, and a near-unity photoluminescence quantum yield of ∼98 % in the practical mass-production concentration range (1–3 wt%). The corresponding non-sensitized device achieves a maximum external quantum efficiency of 41.5% without any external light extraction techniques, representing state-of-the-art performance for deep-blue OLEDs. These findings will help drive the development of highly efficient and stable narrowband deep-blue emitters and lead to a revolution in OLED technology.

窄带发光体具有色域广、稳定性高和效率高等特点,在制造下一代深蓝色有机发光二极管(OLED)方面具有显著优势。尽管通过合理的分子设计已经可以实现 100% 的内部量子效率,但如何提高光外耦合效率以进一步提升器件性能仍是一项紧迫的挑战。在此,我们战略性地提出了一种新型非对称结构设计策略,旨在同时优化深蓝色多共振(MR)发射器的水平发射偶极取向和聚集态特性。这种概念验证型发射器 A-BN 能够发出峰值为 461 nm、全宽半最大值为 25 nm、CIEy 坐标为 0.08,水平偶极比高达 ∼ 90 %,在实际量产浓度范围内(1-3 wt%),光致发光量子产率接近 98 %。相应的非敏化器件在没有任何外部光提取技术的情况下实现了 41.5% 的最大外部量子效率,代表了深蓝色有机发光二极管的最先进性能。这些发现将有助于推动高效、稳定的窄带深蓝发光体的发展,并带来有机发光二极管技术的革命。
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引用次数: 0
8″ wafer-scale, centimeter-sized, high-efficiency metalenses in the ultraviolet 8 英寸晶圆级、厘米级高效紫外线金属透镜
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-03-01 DOI: 10.1016/j.mattod.2024.01.010
Joohoon Kim , Yeseul Kim , Wonjoong Kim , Dong Kyo Oh , Dohyun Kang , Junhwa Seong , Jeong Woo Shin , Dohyun Go , Chanwoong Park , Hyoin Song , Jihwan An , Heon Lee , Junsuk Rho

Metalenses have outstanding light-modulating performances, and studies have been conducted on them to not only replace conventional bulky and heavy refractive lenses but also to expand on them. However, their operating wavelengths have rarely covered the ultraviolet (UV) regime since UV-transparent materials are scarce and nanopatterning techniques have a small patterning area, high cost, and low throughput. These limitations are overcome in this study, and centimeter-scale and highly efficient UV metalenses are successfully mass-produced. The UV metalens is designed to operate at a wavelength of 325 nm, with a numerical aperture of 0.2. Argon fluoride photolithography is used to fabricate an 8-inch master stamp in which 300 metalenses are patterned in an array with a high resolution. The fabricated master stamp can be duplicated repeatedly using wafer-scale nanoimprint lithography. To improve efficiency, we developed a zirconium dioxide–polymer hybrid material that is scalable, easily manufacturable, UV-transparent, and high-index material. The experimental results confirm that the mass-produced metalenses operate as ideal imaging systems, exhibiting an average measured efficiency of 45.1 %.

[显示省略]
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引用次数: 0
Aperiodicity is all you need: Aperiodic monotiles for high-performance composites 非周期性就是您所需要的一切:用于高性能复合材料的非周期性单纺织物
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-03-01 DOI: 10.1016/j.mattod.2023.12.015
Jiyoung Jung , Ailin Chen , Grace X. Gu

Developing mechanical materials with high stiffness, strength, and toughness has been a longstanding pursuit. Conventional engineering materials often experience a trade-off relationship between these properties, motivating researchers to explore composite structures to overcome these limitations. This study introduces a novel approach to composite design by employing aperiodic monotiles, shapes that cover surfaces without any translational symmetry. Using a combined computational and experimental approach, we study the fracture behavior of composites crafted with these monotiles and compare their performance against conventional honeycomb and square patterns. Remarkably, our aperiodic monotile-based composites exhibited superior Young's modulus, strength, and toughness in comparison to other designs under tensile loading conditions. In addition, the aperiodic monotile structures showed consistent mechanical performance with varying crack locations and directions, which implies reliable fracture resistance under complex loadings. This study suggests that leveraging the inherent disorder of aperiodic structures can usher in a new generation of robust and resilient materials.

开发具有高刚度、高强度和高韧性的机械材料是一项长期的追求。传统的工程材料往往在这些性能之间存在权衡关系,这促使研究人员探索复合材料结构来克服这些限制。本研究介绍了一种新颖的复合材料设计方法,即采用无平移对称性的覆盖表面的非周期性单体。我们采用计算和实验相结合的方法,研究了使用这些单片材料制作的复合材料的断裂行为,并将其性能与传统的蜂窝和方形图案进行了比较。值得注意的是,在拉伸加载条件下,与其他设计相比,我们基于非周期性单瓷砖的复合材料表现出更高的杨氏模量、强度和韧性。此外,在不同的裂纹位置和方向上,非周期性单纺织物结构表现出一致的机械性能,这意味着在复杂载荷下具有可靠的抗断裂性。这项研究表明,利用非周期性结构固有的无序性,可以开发出新一代坚固耐用的材料。
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引用次数: 0
Recycling of LiFePO4 cathode materials: From laboratory scale to industrial production 磷酸铁锂阴极材料的回收利用:从实验室规模到工业生产
IF 24.2 1区 材料科学 Q1 Engineering Pub Date : 2024-03-01 DOI: 10.1016/j.mattod.2023.12.012
Minghui Shan , Chenyang Dang , Kai Meng , Yunteng Cao , Xiaoqing Zhu , Jia Zhang , Guiyin Xu , Meifang Zhu

Lithium iron phosphate (LiFePO4) has emerged as one of the most popular cathodes due to its excellent properties of low cost, high safety and stability. However, owing to the limited lifespan caused by degradation, the widespread use of LiFePO4 batteries would generate a large number of spent batteries, the improper disposal of which causes environmental pollution and waste of resources. Therefore, the recycling of these batteries is important for environmental protection, resource conservation and economic efficiency. This review summarises LiFePO4 cathode materials from their development and degradation mechanisms, illustrating the reasons and necessity of their recycling. In addition, battery recycling technologies are systematically discussed from laboratory scale to industrial production in terms of efficiency, economic benefits and environmental impact. Finally, we identify the challenges of LiFePO4 cathode recycling and offer some perspectives on these challenges. These endeavors demonstrate that the degradation of large-scale batteries drives the formation of recycling demand. Therefore, it is necessary to accurately assess the degradation mechanism which is a precondition of cathode recycling. Besides, the cathode recycling mechanism should be paid much attention, simplifying the recycling process. Moreover, it is essential to illustrate the impact of impurities and defects generated during the cycling. As such, this review provides valuable insights in innovating and boosting LiFePO4 cathode recycling technologies on an industrial scale.

磷酸铁锂(LiFePO4)因其低成本、高安全性和稳定性等优良特性,已成为最受欢迎的正极之一。然而,由于磷酸铁锂电池的降解导致其寿命有限,广泛使用会产生大量废旧电池,处理不当会造成环境污染和资源浪费。因此,这些电池的回收利用对环境保护、资源节约和经济效益具有重要意义。本综述从磷酸铁锂正极材料的发展和降解机理等方面进行了总结,说明了其回收利用的原因和必要性。此外,还从效率、经济效益和环境影响等方面系统地讨论了从实验室规模到工业化生产的电池回收技术。最后,我们指出了磷酸铁锂正极回收所面临的挑战,并对这些挑战提出了一些看法。这些努力表明,大规模电池的降解推动了回收需求的形成。因此,准确评估降解机制是阴极回收的前提条件。此外,还应重视正极回收机制,简化回收流程。此外,说明循环过程中产生的杂质和缺陷的影响也很重要。因此,本综述为创新和促进工业规模的磷酸铁锂阴极回收技术提供了宝贵的见解。
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引用次数: 0
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