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Recycling routes of lithium-ion batteries: A critical review of the development status, the process performance, and life-cycle environmental impacts 锂离子电池的回收途径:对发展现状、工艺性能和生命周期环境影响的批判性回顾
IF 4.3 Q3 ENERGY & FUELS Pub Date : 2022-11-02 DOI: 10.1557/s43581-022-00053-9
Ronja Wagner-Wenz, Albert-Jan van Zuilichem, L. Göllner-Völker, Katrin Berberich, A. Weidenkaff, L. Schebek
This review examines the status of development, process performance and life cycle environmental impact of the three major recycling routes for lithium ion batteries and considers the impact of changes in legislation in the European Union (EU). Today, new lithium-ion battery-recycling technologies are under development while a change in the legal requirements for recycling targets is under way. Thus, an evaluation of the performance of these technologies is critical for stakeholders in politics, industry, and research. We evaluate 209 publications and compare three major recycling routes. An important aspect of this review is that we tackle the need for a critical evaluation of these recycling routes by introducing clear terms and creating a structuring scheme. Our evaluation criteria cover three areas: status of development, process performance, and life-cycle environmental impacts. With respect to development status, we provide an analysis of today’s market. A criterion of process performance is recycling efficiency, which today focuses on the mass of the recovered materials. To include the contributions of critical materials, we add a criterion for the efficiency of recovery of materials. Life-cycle assessments provide information on gross impacts, benefit of substituting virgin material and net impact. Present life-cycle assessments focus on waste management rather than on recovery of critical materials. This review contributes to an understanding of these trade-offs and supports discussion as to what is the “best” recycling route when targets conflict. Graphical Abstract There are three possible process sequences for each lithium-ion battery-recycling route. A distinction is made between pre-treatment steps (gray), direct physical treatment steps (green), pyro-metallurgical treatment (orange), and hydro-metallurgical treatment (blue). The figure is based on a figure from Doose et al. (Joule 3:2622–2646, 2019).
本综述考察了锂离子电池三种主要回收途径的开发状况、工艺性能和生命周期环境影响,并考虑了欧盟(EU)立法变化的影响。如今,新的锂离子电池回收技术正在开发中,而回收目标的法律要求正在改变。因此,对这些技术的性能进行评估对政治、工业和研究中的利益相关者至关重要。我们评估了209种出版物,并比较了三种主要的回收途径。这项审查的一个重要方面是,我们通过引入明确的条款和制定结构方案来解决对这些回收路线进行批判性评估的必要性。我们的评估标准涵盖三个领域:开发状况、工艺性能和生命周期环境影响。关于发展现状,我们对当今市场进行了分析。工艺性能的一个标准是回收效率,今天的回收效率侧重于回收材料的质量。为了包括关键材料的贡献,我们增加了材料回收效率的标准。生命周期评估提供了关于总影响、替代原始材料的效益和净影响的信息。目前的生命周期评估侧重于废物管理,而不是关键材料的回收。这篇综述有助于理解这些权衡,并支持在目标冲突时讨论什么是“最佳”回收路线。图形摘要每个锂离子电池回收路线有三种可能的工艺顺序。对预处理步骤(灰色)、直接物理处理步骤(绿色)、热冶金处理(橙色)和湿法冶金处理(蓝色)进行了区分。该数字基于Doose等人的数字(Joule 3:2622–26462019)。
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引用次数: 6
High-rate NaMo_0.05Ti_1.95(PO_4)_3 for aqueous sodium-ion battery anode material 高倍率NaMo_0.05Ti_1.95(PO_4)_3水溶液钠离子电池正极材料
IF 4.3 Q3 ENERGY & FUELS Pub Date : 2022-09-01 DOI: 10.1557/s43581-022-00041-z
Cheng-Yen Wu, Shao-Chu Huang, Jagabandhu Patra, Chia‐Ching Lin, Chung-Sheng Ni, Jeng‐Kuei Chang, Han-Yi Chen, Cheng‐Zhang Lu
Aqueous sodium-ion batteries (ASIBs) are currently being developed as low-cost candidates for large-scale energy storage of green energy. Na superionic conductor-type NaTi_2(PO_4)_3 is a promising anode material for ASIBs owing to its excellent theoretical capacity, open three-dimensional framework, and sufficiently low-redox potential. However, its retention rate is restricted by its poor electronic conductivity. In this study, Mo-doped NTPs, NaMo_ x Ti_2− x (PO_4)_3 ( x  = 0, 0.01, 0.03, 0.05, 0.07), are synthesized using a facile sol–gel method to enhance its electronic conductivity. X-ray diffraction analysis reveals that composites doped with high-valence Mo retain rhombohedral crystal structure. Owing to the improved electronic conductivity and sodium-ion kinetics, NaMo_0.05Ti_1.95(PO_4)_3 exhibits superior capacity of 100.9 mAh g^−1 at 50 mA g^−1 and excellent rate performance of 71.9 mAh g^−1 at 10 A g^−1. Moreover, Mo-doped composites retain 82.7% of their original capacity after 500 cycles at 1 A g^−1, indicating the excellent cycling stability of NaMo_0.05Ti_1.95(PO_4)_3. Full cell with Mg-doped Na_3V_1.95Mg_0.05(PO_4)_2F_3/C cathode exhibits a high voltage window of 1.5 V and a sustained high energy density of 28.7 Wh kg^−1 at 512.7 W kg^−1 and 22.1 Wh kg^−1 at 2405.1 W kg^−1. These results demonstrate that NaMo_0.05Ti_1.95(PO_4)_3 exhibits high rate capability and long cycle life, making it a promising ASIB anode material for grid-scale energy storage. Graphical abstract
水性钠离子电池(ASIBs)目前正被开发为大规模绿色能源储能的低成本候选电池。钠超离子导体型NaTi_2(PO_4)_3具有优异的理论容量、开放的三维骨架和足够低的氧化还原电位,是一种很有前途的ASIBs阳极材料。然而,其保留率受到其较差的电子导电性的限制。在本研究中,Mo掺杂的NTPs,NaMo_xTi_2−x(PO_4)_3(x = 0,0.01,0.03,0.05,0.07),以提高其电子导电性。X射线衍射分析表明,高价Mo掺杂的复合材料保持了菱形晶体结构。NaMo_0.05Ti_1.95(PO_4)_3由于其电子电导率和钠离子动力学的改善,在50 mA g^−1时表现出100.9 mAh g^−的优异容量,在10 A g^−2时表现出71.9 mAh g ^−1的优异倍率性能。此外,Mo掺杂复合材料在1A g^−1下循环500次后仍保持了82.7%的原始容量,表明NaMo_0.05Ti_1.95(PO_4)_3具有优异的循环稳定性。Mg掺杂Na_3V_1.95Mg_0.05(PO_4)_2F_3/C阴极的全电池在512.7W kg^−1时表现出1.5V的高电压窗口,在2405.1W kg^-1时表现出28.7Wh kg^−1的持续高能量密度。这些结果表明,NaMo_0.05Ti_1.95(PO_4)_3具有较高的倍率性能和较长的循环寿命,是一种很有前途的电网储能ASIB阳极材料。图形摘要
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引用次数: 0
Recent progress in the synthesis of metal-organic-framework-derived carbon materials 金属-有机骨架衍生碳材料的合成进展
IF 4.3 Q3 ENERGY & FUELS Pub Date : 2022-09-01 DOI: 10.1557/s43581-022-00049-5
Zilin Yang, Shuai Cao, Ting-ting Lv, Guangxun Zhang, Xiaotian Guo, Songtao Zhang, H. Pang
Metal–organic frameworks (MOFs), as a coordination polymer, has developed rapidly in recent years. Meanwhile, carbon materials (CMs) derived from MOFs have attracted extensive attention due to their high specific surface area nanoporous structures and tunable chemical and physical properties, which are widely used in energy storage and conversion, electrocatalysis and other fields. Nowadays, how to efficiently prepare MOFs-derived carbon materials on a large scale for industrial application is the focus of current research. This paper reviews the different forms and preparation methods of metal–organic framework carbon materials. At the same time, the current defects and future development trends of MOFs-derived carbon materials synthesis are discussed. Graphical abstract
金属-有机框架(MOFs)作为一种配位聚合物,近年来发展迅速。同时,MOFs衍生的碳材料因其高比表面积的纳米多孔结构和可调的化学和物理性能而受到广泛关注,广泛应用于储能与转换、电催化等领域。目前,如何有效地大规模制备MOFs衍生的碳材料用于工业应用是当前研究的重点。本文综述了金属-有机骨架碳材料的不同形式和制备方法。同时,讨论了MOFs衍生碳材料合成的现状和发展趋势。图形摘要
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引用次数: 1
A perspective on the design and scale up of a novel redox flow battery 新型氧化还原液流电池的设计与规模化研究
IF 4.3 Q3 ENERGY & FUELS Pub Date : 2022-09-01 DOI: 10.1557/s43581-022-00046-8
N. Sinclair, R. Savinell, J. Wainright
Abstract Government funding is critical for testing concepts and ideas of technical approaches to demonstrate their value to attract attention for commercial development. In the US for energy projects, this funding often comes from ARPA-E, but similar types of funding agencies exist in other countries as well. However, independent of the funding sources, government or private, often unanticipated challenges arise that require pivots and flexibility, and leap-frogging scale-up levels can hinder achieving the knowledge needed for technology development. By incorporating a conducting carbon slurry in the negative electrolyte of an all iron flow battery, the decoupling of power from energy design becomes possible for this normally hybrid flow battery system. This approach offers the potential for very low cost large-scale energy storage with safe and sustainable materials. Government funding of this project allowed the demonstration of the concept during the seedling stage, but with the use of carbon nanotubes that would not meet cost targets. The second phase of the project demonstrated that low cost carbons with certain properties could also be used effectively. The third phase of the project then sought to scale-up the lab cells to a full-size stack. This paper summarizes some of the technical challenges encountered and pivots in approach that were taken. This project was sponsored by a commercialization-focused government agency (US ARPA-E in this case) and we point out some constraints and expectations of attracting commercial funding sources that hindered the development, or complicated solving the necessary design and materials issues to make the technology interesting for further investment. The lessons learned here will be applicable to other commercialization driven projects sponsored by government agencies in the US and elsewhere. Graphical abstract
政府资助对于测试技术方法的概念和想法以证明其价值以吸引商业开发的关注至关重要。在美国,能源项目的资金通常来自ARPA-E,但其他国家也存在类似的资助机构。然而,独立于政府或私人的资金来源之外,往往会出现意想不到的挑战,这些挑战需要支点和灵活性,而跨越式的规模扩大水平可能会阻碍获得技术开发所需的知识。通过在全铁液流电池的负电解质中加入导电碳浆,这种通常的混合液流电池系统的功率与能量设计的解耦成为可能。这种方法为使用安全和可持续材料的低成本大规模储能提供了潜力。政府资助的这个项目允许在幼苗阶段展示这个概念,但是使用的碳纳米管无法达到成本目标。该项目的第二阶段表明,具有某些特性的低成本碳也可以有效利用。该项目的第三阶段是将实验室细胞扩大到全尺寸堆叠。本文总结了所遇到的一些技术挑战和所采取的方法的要点。这个项目是由一个以商业化为重点的政府机构(在这个案例中是美国ARPA-E)赞助的,我们指出了一些限制和期望,吸引商业资金来源,阻碍了发展,或者复杂的解决必要的设计和材料问题,使技术对进一步的投资感兴趣。这里的经验教训将适用于美国和其他地方政府机构资助的其他商业化项目。图形抽象
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引用次数: 0
Ti_4O_7 as conductive additive in sulfur and graphene-sulfur cathodes for high-performance Lithium-sulfur batteries with a facile preparation method Ti_4O_7在高性能锂硫电池硫和石墨烯硫阴极中的导电添加剂的简易制备方法
IF 4.3 Q3 ENERGY & FUELS Pub Date : 2022-09-01 DOI: 10.1557/s43581-022-00052-w
Chun-Wei yu, Cho-Jen Tsai
Lithium-sulfur batteries have significant potential to be applied in next-generation energy storage systems. However, polysulfide dissolution and redeposition have contributed to poor cycling stability, low sulfur utilization, and poor rate performance, thereby limiting their practical applications. Herein, we used a sol-gel method to fabricate a Ti_4O_7 conductive metal oxide, which was partially added to a Lithium-sulfur battery cathode. The results demonstrated that the addition of 7.5 wt% to 10 wt% Ti_4O_7 as the conductive additive resulted in a better rate capability and reversible cycling performance owing to its high electronic conductivity and surface adsorption of polysulfides. Compared to complex architectures and complicated synthesis methods, we report a more effective way to overcome the drawbacks of Lithium-sulfur batteries. Graphical abstract
锂硫电池在下一代储能系统中具有巨大的应用潜力。然而,多硫溶解和再沉积导致循环稳定性差,硫利用率低,速率性能差,从而限制了它们的实际应用。本文采用溶胶-凝胶法制备了Ti_4O_7导电金属氧化物,并将其部分添加到锂硫电池正极中。结果表明,添加7.5 wt% ~ 10 wt%的Ti_4O_7作为导电添加剂,由于Ti_4O_7具有较高的电子导电性和对多硫化物的表面吸附能力,具有较好的速率性能和可逆循环性能。与复杂的结构和复杂的合成方法相比,我们报告了一种更有效的方法来克服锂硫电池的缺点。图形抽象
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引用次数: 2
Energy and sustainability: A historical moment for the nation and the world 能源和可持续性:美国和世界的历史性时刻
IF 4.3 Q3 ENERGY & FUELS Pub Date : 2022-09-01 DOI: 10.1557/s43581-022-00051-x
Yue Meng
Last month, we were elated to learn that the climate and energy provisions of the Inflation Reduction Act will speed greenhouse gas mitigation and put the US on track to deliver the intended target for 2035. The bill includes $369 billion in climate and energy provisions that will transform how the nation gets its energy and shape the country’s climate and industrial policy for decades. It is indeed a historical moment. MRS Energy & Sustainability was launched as a reviews-only journal in 2014. The Materials Research Society (MRS) has a long track record of recognizing the scientific, technological, and sociological complexity relating to energy, the environment, and sustainability. The birth of the journal 8 years ago was motivated by the Society’s vision as a global organization of materials researchers that promotes communication for the advancement of interdisciplinary materials research and technology to improve the quality of life. Naturally, energy and sustainability are at the core of our quality of life. Since I became the Editor-in-Chief of the journal in 2018, my goal has been to broaden its scope by introducing more original research and focused topics to the journal’s coverage. (Original research represents 39% of published content since 2020). Despite the lack of in-person meetings in 2020 and 2021 due to the pandemic, I am delighted to see the enthusiastic engagement from the materials science community at large. Remarkably, we have increased numbers of downloads all over the world and submissions are steadily increasing. The journal has subscriptions on all six habitable continents, and the variety of content has made it a destination for the most cutting-edge research in the field. In 2021, MRS entered a new publishing alliance with Springer-Nature, one of the world’s powerhouses for scientific publications. At this critical moment of energy transition in the world, MRS Energy & Sustainability will continue to serve the MRS community and society at large by publishing the convergent research among science, technology, economics, and policy. The journal published some of its most highly cited papers addressing recycling, critical materials supply chain, life cycle analysis for renewables, materials circularity, etc., long before those issues caught the public’s attention. Our readers include a broad spectrum of scientists, academics, policy makers, and industry professionals, all interested in the interdisciplinary nature of the science, technology, and policy aspects of energy and sustainability. Looking ahead when EDITORIAL
上个月,我们高兴地获悉,《通货膨胀削减法案》(Inflation Reduction Act)中的气候和能源条款将加速温室气体减排,使美国走上实现2035年预期目标的轨道。该法案包括3690亿美元的气候和能源条款,这些条款将改变美国获得能源的方式,并塑造美国未来几十年的气候和产业政策。这确实是一个历史性的时刻。《MRS能源与可持续发展》杂志于2014年创刊,仅限评论。材料研究学会(MRS)在认识与能源、环境和可持续性相关的科学、技术和社会学复杂性方面有着悠久的历史。该杂志于8年前诞生,其动机是该协会的愿景,即作为一个全球性的材料研究人员组织,促进跨学科材料研究和技术的进步,以提高生活质量。自然,能源和可持续性是我们生活质量的核心。自2018年担任主编以来,我的目标一直是通过在期刊报道中引入更多原创研究和重点主题来扩大其范围。(自2020年以来,原创研究占已发表内容的39%)。尽管由于疫情的影响,2020年和2021年没有面对面的会议,但我很高兴看到材料科学界的热情参与。值得注意的是,我们在全球范围内的下载量和提交量都在稳步增长。该杂志在所有六个可居住的大洲都有订阅,其内容的多样性使其成为该领域最尖端研究的目的地。2021年,MRS与世界科学出版物巨头之一的施普林格-自然(Springer-Nature)建立了新的出版联盟。在这个世界能源转型的关键时刻,《MRS能源与可持续发展》将继续通过发表科学、技术、经济和政策的融合研究,为MRS社区和整个社会服务。早在这些问题引起公众注意之前,该杂志就发表了一些被引用率最高的论文,涉及回收、关键材料供应链、可再生能源生命周期分析、材料循环等问题。我们的读者包括广泛的科学家、学者、政策制定者和行业专业人士,他们都对能源和可持续发展的科学、技术和政策方面的跨学科性质感兴趣。展望未来
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引用次数: 0
A review on electric vehicle transport policy of India with certain recommendations 印度电动汽车运输政策综述及若干建议
IF 4.3 Q3 ENERGY & FUELS Pub Date : 2022-09-01 DOI: 10.1557/s43581-022-00048-6
K. Yadav, A. Sircar
India is forging ahead on the journey of adopting electric vehicles in the country with all EV fleets targeting by 2030. It seems to be quite optimistic considering that the EV fleet is still smaller than 1%. Successful market penetration of electric vehicles may not only rely on the characteristics of the technology, but also on the business models available on the market. This study is a review of Indian EV policy in order to change Indian mobility sector. It discusses the journey of Indian EV sector and how it evolved. It talks about the six key growth drivers which are responsible for EV development in India. This paper also narrates the electric vehicle policy development cycle of India with its parameters and functions. It also explains the life cycle assessment of EV for the development of economic perspective of EV in India. The Indian government needs to implement policies aimed at reducing air pollution by introducing EV’s that raise the sale of electric vehicles, increase the percentage of green energy in the Indian power mix and prevent battery production air pollution. The suggested strategies can be adapted to reduce air emissions by increasing the introduction of electric vehicles in any sector globally. Graphical abstract
印度正在推进采用电动汽车的道路,所有电动汽车车队的目标是到2030年。考虑到电动汽车车队仍不足1%,这似乎相当乐观。电动汽车能否成功渗透市场,不仅取决于技术的特点,还取决于市场上可用的商业模式。这项研究是对印度电动汽车政策的回顾,旨在改变印度的出行行业。它讨论了印度电动汽车行业的发展历程及其演变过程。它谈到了印度电动汽车发展的六个关键增长驱动因素。本文还叙述了印度电动汽车政策的发展周期及其参数和功能。它还解释了电动汽车的生命周期评估,以发展印度电动汽车的经济前景。印度政府需要实施旨在减少空气污染的政策,引入电动汽车,提高电动汽车的销量,提高绿色能源在印度电力结构中的比例,并防止电池生产空气污染。建议的策略可以通过在全球任何行业增加电动汽车的引入来减少空气排放。图形摘要
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引用次数: 0
Synthesis of size-selected Pt/GONR nanocomposites for visible-light-enhanced methanol oxidation reaction in an alkaline solution 用于碱性溶液中可见光增强甲醇氧化反应的尺寸选择的Pt/GONR纳米复合材料的合成
IF 4.3 Q3 ENERGY & FUELS Pub Date : 2022-09-01 DOI: 10.1557/s43581-022-00054-8
Chia-Liang Sun, Yu-Chih Chen, Cheng-Hsuan Lin, Hung-Yu Chen
Abstract In this study, we prepared size-selected Pt/graphene oxide nanoribbon (GONR) composites as fuel-cell anode photoelectrocatalysts for methanol oxidation reaction (MOR) in an alkaline solution. Additionally, we used a light-emitting diode (LED) and a Xeon (Xe) lamp to increase the current densities of methanol oxidation reaction while photoelectrochemical phenomenon occurred upon our catalysts. The major parameter of our research is microwave powers for unzipping GONRs for electrochemical and photoeletrochemical measurements. Firstly, we utilized microwave heating to fabricate GONRs and load Pt nanoparticles made by chemical reduction methods. Secondly, we carried out the electrochemical and photoeletrochemical measurements using electrocatalyst-modified screen-printed carbon electrodes. The size distribution of Pt colloidal nanoparticles was characterized by transmission electron microscopy. The compositions of composite catalysts were determined by scanning electron microscopy and energy-dispersive X-ray spectroscopy. The MOR photocurrent density of Pt/GONR (200 W) in cyclic voltammograms is 458 mA/mg_Pt under LED illumination. The photocurrent increase of this condition is 38.0% which is better than its dark one. Furthermore, we can obtain the MOR photocurrent density of 608, 696, and 794 mA/mg_Pt using Xe lamp with a power of 500, 750, and 1000 mW/cm^2. Graphical abstract Highlights The Pt/graphene oxide nanoribbon composites was used as electrocatalysts for the methanol oxidation reaction in an alkaline solution. The visible light sources help to improve the peak oxidation currents of the reaction using our electrocatalysts. Discussion The requirements for a best carbon support for a specific photoelectrochemical reaction remain an issue. The quantitative analyses of the current increase induced by photon energy in a specific electrochemical reaction are not well resolved yet.
摘要在本研究中,我们制备了尺寸选择的Pt/氧化石墨烯纳米带(GONR)复合材料,作为碱性溶液中甲醇氧化反应(MOR)的燃料电池阳极光电催化剂。此外,我们使用发光二极管(LED)和至强(Xe)灯来增加甲醇氧化反应的电流密度,同时在我们的催化剂上发生光电化学现象。我们研究的主要参数是用于电化学和光电化学测量的GONR解压缩的微波功率。首先,我们利用微波加热制备了GONR,并负载了化学还原法制备的Pt纳米颗粒。其次,我们使用电催化剂修饰的丝网印刷碳电极进行了电化学和光电化学测量。用透射电子显微镜对Pt胶体纳米粒子的粒径分布进行了表征。用扫描电子显微镜和能谱仪测定了复合催化剂的组成。在LED照明下,Pt/GONR(200W)在循环伏安图中的MOR光电流密度为458mA/mg_Pt。该条件下的光电流增幅为38.0%,优于暗条件下的增幅。此外,我们可以使用功率为500、750和1000mW/cm^2的Xe灯获得608、696和794mA/mg_Pt的MOR光电流密度。图形摘要亮点Pt/氧化石墨烯纳米带复合材料被用作碱性溶液中甲醇氧化反应的电催化剂。使用我们的电催化剂,可见光源有助于提高反应的峰值氧化电流。讨论对特定光电化学反应的最佳碳载体的要求仍然是一个问题。对特定电化学反应中光子能量引起的电流增加的定量分析尚未得到很好的解决。
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引用次数: 0
The role of modeling battery degradation in bulk power system optimizations 电池退化建模在大容量电力系统优化中的作用
IF 4.3 Q3 ENERGY & FUELS Pub Date : 2022-09-01 DOI: 10.1557/s43581-022-00047-7
Bolun Xu
Battery energy storage is critical to decarbonizing future power systems, and the cost of battery degradation within power system operations is crucial to ensure economic utilization of battery resources and provide a fair return to their investors. Power system operators dispatch assets by solving optimization problems of extreme complexity that include thousands of generators and transmission lines, and degradation models to be incorporated into power system optimization must be efficient to compute while capturing key degradation factors relevant to grid operations. This paper will compare various degradation models that are incorporable into power system optimization; each has different computation complexities and modeling focuses. This paper will summarize the pros and cons of different models, and how they may suit different battery technologies or configurations. Besides modeling, the paper discusses the opportunity cost of degradation and the battery warranty terms, both will impact the design and implementation of degradation models in power systems. The paper summarizes the comparison and future directions for designing degradation models for grid-scale batteries. Graphical abstract
电池储能对于未来电力系统的脱碳至关重要,而电力系统运营中电池退化的成本对于确保电池资源的经济利用和为投资者提供公平回报至关重要。电力系统运营商通过解决包括数千台发电机和输电线路在内的极端复杂的优化问题来调度资产,要纳入电力系统优化的退化模型必须能够高效计算,同时捕捉与电网运营相关的关键退化因素。本文将比较可纳入电力系统优化的各种退化模型;每种方法都有不同的计算复杂性和建模重点。本文将总结不同型号的优缺点,以及它们如何适合不同的电池技术或配置。除建模外,本文还讨论了退化的机会成本和电池保修条款,这两个问题都将影响电力系统退化模型的设计和实施。本文总结了电网规模电池退化模型设计的比较和未来方向。图形摘要
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引用次数: 4
Unilateral modified composite electrolyte by high modulus ceramics filling 高模量陶瓷填充单向改性复合电解质
IF 4.3 Q3 ENERGY & FUELS Pub Date : 2022-08-30 DOI: 10.1557/s43581-022-00045-9
Pu Chen, Rui-Tung Kuo, Tzu-Ying Lin
Abstract Replacing liquid electrolytes with solid-state electrolytes allows all-solid-state lithium batteries (SSBs) to exhibit excellent safety and high volumetric energy density. Since the large-scale processing of electrolytes might encounter a brittleness issue on the ceramic solid-state electrolytes, the solid polymer electrolytes (SPEs) such as poly(ethylene oxide) (PEO)-based polymer-ceramic composite may present a solution due to its great strength and bendable characteristics. While being inherently flexible, PEO-based electrolyte has relatively low ionic conductivity at room temperature and poor resistance against the hazard of dendrite formation and growth. Although ceramic filler addition has been developed to increase the yield strength and improve the electrochemical properties, high-density fillers lack reinforcement and cause brittle failure. In this work, we propose a unilateral structure that well combines the flexible nature of PEO polymer and low fraction fillers with good inhibition of lithium dendrite growth. In the unilateral structure, the polymer acquires high flatness and wettability to the electrode, and high-density garnet Li_7La_3Zr_2O_12-based filler at the composite surface provides high shear modulus to enhance overall mechanical strength, taking complementary advantages of two kinds of electrolytes. It is further demonstrated that the lithium-ion conductivity strongly depends on the lithium concentration gradient inside the composite electrolyte, and ball-milled ceramics may further disequilibrium the optimum ionic conductivities. Under current density galvanostatic cycling of 0.2 mA/cm^2, a unilateral modified composite electrolyte with merely 15wt% fillers can withstand lithium stripping and plating smoothly for more than 50 h without potential protrusion. Graphical abstract
摘要用固态电解质代替液体电解质可以使全固态锂电池(SSBs)表现出优异的安全性和高体积能量密度。由于电解质的大规模加工可能会遇到陶瓷固体电解质的脆性问题,固体聚合物电解质(SPE),如聚环氧乙烷(PEO)基聚合物-陶瓷复合材料,由于其强大的强度和可弯曲的特性,可能会提供解决方案。PEO基电解质虽然具有固有的柔性,但在室温下具有相对较低的离子导电性,并且对枝晶形成和生长的危险性较差。尽管已经开发了添加陶瓷填料来提高屈服强度和电化学性能,但高密度填料缺乏增强性并导致脆性破坏。在这项工作中,我们提出了一种单侧结构,它很好地结合了PEO聚合物和低分数填料的柔性性质,并对锂枝晶生长有良好的抑制作用。在单侧结构中,聚合物获得了较高的平坦性和对电极的润湿性,复合材料表面的高密度石榴石Li_7La_3Zr_2O_12基填料提供了较高的剪切模量,提高了整体机械强度,这是两种电解质的互补优势。进一步证明,锂离子电导率在很大程度上取决于复合电解质内的锂浓度梯度,球磨陶瓷可能会进一步失衡最佳离子电导率。在0.2mA/cm^2的电流密度恒电流循环下,仅含15wt%填料的单向改性复合电解质可以在没有电位突出的情况下平稳地承受锂剥离和电镀50小时以上。图形摘要
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MRS Energy & Sustainability
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