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How ozone traces degrade polyimide humidifier membranes for fuel cells 臭氧痕迹如何降解燃料电池用聚酰亚胺加湿器膜
Pub Date : 2024-05-22 DOI: 10.1016/j.nxener.2024.100138
Daniel Ilk , Viktoria Frick , Christopher Hänel , Tobias Götz , Thomas Schiestel , Michael Schoemaker , Harry E. Hoster

Humidification of polymer electrolyte membranes in fuel cells is essential for high proton conductivity and lifetime, therefore often membrane humidifier modules are used. We report about the degradation of polyimide humidifier membranes under the influence of airborne ozone traces: during operation we tracked the membranes humidifier performance in 5 modules for up to 1000 h with trace levels of ozone (100 ppb) and conducted characterization tests at 200 h intervals. Operating the humidifier with ozone resulted in a linear decrease in the membrane's ability to transfer moisture over time. Moreover, the glass transition temperature of the membrane material decreases linearly with longer exposure to ozone, while the mechanical strength in terms of breaking force and elongation at break decreases too. Infrared spectra of the tested fibers showed no changes. The reduced water vapor flux would limit fuel cell performance, while the reduced mechanical properties of the membrane can lead to rupture.

燃料电池中聚合物电解质膜的加湿对高质子传导性和使用寿命至关重要,因此通常使用膜加湿器模块。我们报告了聚酰亚胺加湿器膜在空气中臭氧痕量影响下的降解情况:在运行过程中,我们对 5 个模块的膜加湿器性能进行了长达 1000 小时的痕量臭氧(100 ppb)跟踪,并每隔 200 小时进行一次特性测试。在臭氧环境下运行加湿器时,随着时间的推移,膜转移水分的能力呈线性下降。此外,膜材料的玻璃化温度随着暴露在臭氧中的时间延长而线性降低,而机械强度(断裂力和断裂伸长率)也随之降低。测试纤维的红外光谱没有变化。水蒸气通量的降低会限制燃料电池的性能,而膜的机械性能降低则会导致破裂。
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引用次数: 0
Recent advances of vanadium-based cathodes toward aqueous Zn-ion batteries 钒基阴极在水性 Zn 离子电池方面的最新进展
Pub Date : 2024-05-21 DOI: 10.1016/j.nxener.2024.100119
Yuyan Wang, Huaqing Chen, Shujia Zhang, Linrui Hou, Xuting Li, Changzhou Yuan

Benefiting from the advantageous features of low manufacturing cost, inherent safety and resource renewability, aqueous Zn-ion batteries (AZIBs) are considered as one of the most promising candidates for energy storage systems. Unfortunately, problems of AZIBs such as cathode dissolution, Zn dendrite growth, and irreversible electrochemical side reactions have restricted the implementation for practical applications. Vanadium-based are deemed as hopeful cathode materials for AZIBs owing to diverse crystal structures and multiple valence states. Therefore, it is necessary to comprehensively summarize the advance facing vanadium-based cathodes and the corresponding progress to create roadmaps for the development of high-stability AZIBs. This review starts with a discussion of the storage and failure mechanisms of AZIBs and their related affects. Then, enormous up-to-date achievements of vanadium-based cathode materials are highlighted, including vanadium-based oxides and metal vanadium-based oxides. The challenges associated with the application of vanadium-based compounds in AZIBs are also highlighted, and effective strategies to overcome them are proposed. Finally, perspectives and directions on further optimizing vanadium-based cathode materials to improve the performance of AZIBs are discussed.

锌离子水电池(AZIBs)具有制造成本低、固有安全性和资源可再生性等优点,被认为是最有前途的储能系统之一。遗憾的是,AZIBs 存在阴极溶解、锌枝晶生长和不可逆电化学副反应等问题,限制了其实际应用。由于钒基具有多种晶体结构和多价态,因此被认为是有希望的 AZIB 阴极材料。因此,有必要全面总结钒基阴极所面临的挑战和相应的进展,为开发高稳定性 AZIB 绘制路线图。本综述首先讨论了 AZIB 的储存和失效机制及其相关影响。然后,重点介绍了钒基阴极材料的最新巨大成就,包括钒基氧化物和金属钒基氧化物。此外,还强调了钒基化合物在 AZIB 中应用所面临的挑战,并提出了克服这些挑战的有效策略。最后,讨论了进一步优化钒基阴极材料以提高 AZIB 性能的前景和方向。
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引用次数: 0
Stabilizing high temperature operation and calendar life of LiNi0.5Mn1.5O4 稳定 LiNi0.5Mn1.5O4 的高温运行和日历寿命
Pub Date : 2024-05-13 DOI: 10.1016/j.nxener.2024.100136
Weiliang Yao , Yixuan Li , Marco Olguin , Shuang Bai , Marshall A. Schroeder , Weikang Li , Alex Liu , Na Ri Park , Bhargav Bhamwala , Baharak Sayahpour , Ganesh Raghavendran , Oleg Borodin , Minghao Zhang , Ying Shirley Meng

Severe capacity degradation at high operating voltages and poor interphase stability at elevated temperature have thus far precluded the practical application of LiNi0.5Mn1.5O4 (LNMO) as a cathode material for lithium-ion batteries. Addressing these challenges through a combination of experimental and theoretical methods in this work, we demonstrate how a fluorinated carbonate electrolyte enables both high-voltage and high temperature operation by mitigating the traditional interfacial reactions observed in electrolytes with conventional carbonate solvents. Computational studies confirm the exceptional oxidation stability of fluorinated carbonate electrolyte which reduces deprotonation at high voltage. The mitigated deprotonation will then minimize the formation of HF acid which corrodes the LNMO surface and leads to phase transformation and poor interphases. With fluorinated carbonate electrolyte at elevated temperature, it was found on LNMO’s subsurface a reduced amount of Mn3O4 phase which can block Li+ transfer and result in drastic cell failure. Leveraging this approach, LNMO/graphite full cells with a high loading of 3.0 mAh/cm2 achieve excellent cycling stability, retaining ∼84 % of their initial capacity at room temperature (25 °C) after 200 cycles and ∼68 % after 100 cycles at 55 °C. This advanced electrolyte also shows promise for improving calendar life, retaining >30 % more capacity than the carbonate baseline after high temperature storage. These results indicate that electrolytes based on fluorinated carbonates are a promising strategy for overcoming the remaining challenges toward practical commercial application of LNMO.

迄今为止,锂离子电池正极材料镍钴锰酸锂(LiNi0.5Mn1.5O4,LNMO)在高工作电压下的严重容量衰减和在高温下的相间稳定性差,阻碍了它的实际应用。为了应对这些挑战,我们在这项工作中结合了实验和理论方法,展示了含氟碳酸盐电解质如何通过减轻传统碳酸盐溶剂电解质中出现的传统界面反应来实现高压和高温运行。计算研究证实,含氟碳酸盐电解质具有优异的氧化稳定性,可减少高压下的去质子化反应。减轻的去质子化将最大程度地减少氟化氢酸的形成,而氟化氢酸会腐蚀 LNMO 表面,导致相变和相间不良。在高温下使用含氟碳酸盐电解液时,在 LNMO 的亚表面发现了数量减少的 Mn3O4 相,这会阻碍 Li+ 的转移,导致电池严重失效。利用这种方法,装载量高达 3.0 mAh/cm2 的 LNMO/ 石墨全电池实现了出色的循环稳定性,在室温(25 °C)下循环 200 次后,其初始容量仍保持在 84% 左右,在 55 °C下循环 100 次后,其初始容量仍保持在 68%左右。这种先进的电解质还显示出提高日历寿命的前景,在高温储存后,其容量比碳酸盐基线电解质多 30%。这些结果表明,基于含氟碳酸盐的电解质是克服 LNMO 实际商业应用所面临的其余挑战的一种有前途的策略。
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引用次数: 0
Smart investment framework for energy resilience: A case study of a campus microgrid research facility 能源复原力智能投资框架:校园微电网研究设施案例研究
Pub Date : 2024-05-09 DOI: 10.1016/j.nxener.2024.100131
S.M. Safayet Ullah , Samuel Yankson , Shayan Ebrahimi , Farzad Ferdowsi , Terrence Chambers

Energy resilience is a vital consideration for ensuring the survivability of modern infrastructure systems. Achieving 100% resilience, however, is often impractical and economically burdensome. In this paper, we propose a smart investment framework that enables decision-makers to determine optimal investments in energy resilience based on available resources and desired levels of resilience. To illustrate the effectiveness of this framework, we present a case study of a campus microgrid research and testing facility. Using a real-time simulation approach conducted with Typhoon Hardware In Loop (HIL), we evaluate the performance of the microgrid system over 24 hours following 4 historically significant hurricanes that have affected Louisiana in the past few years. The microgrid is designed to power local loads during outages, providing an effective solution for enhancing energy resilience. Real solar data collected from our 1.1 Megawatt (MW) solar facility on the University of Louisiana at Lafayette campus is integrated into the simulation, enabling a realistic evaluation of the system’s performance under hurricane-induced disruptions. By employing the proposed smart investment framework, decision-makers can better identify and address resilience challenges. The framework facilitates informed investment decisions by considering available resources and aligning them with the desired level of resilience. This approach avoids over-investment in unnecessary redundancy while ensuring critical systems are adequately protected. Our research contributes to the field by demonstrating the practicality and benefits of a smart investment framework for energy resilience in a real-world scenario. The case study of the campus microgrid research facility provides valuable insights for decision-makers in similar contexts, highlighting the potential of this framework to guide resilient energy infrastructure planning and investment strategies.

能源复原力是确保现代基础设施系统生存能力的重要考虑因素。然而,要实现 100% 的复原力往往并不现实,而且经济负担很重。在本文中,我们提出了一个智能投资框架,使决策者能够根据可用资源和所需的复原力水平,确定能源复原力方面的最佳投资。为了说明该框架的有效性,我们介绍了一个校园微电网研究和测试设施的案例研究。通过使用台风硬件环路(HIL)进行实时模拟,我们评估了微电网系统在过去几年中影响路易斯安那州的四次历史性重大飓风后 24 小时内的性能。微电网的设计目的是在断电期间为本地负载供电,为提高能源恢复能力提供有效的解决方案。从路易斯安那大学拉斐特校区 1.1 兆瓦(MW)太阳能设施收集的真实太阳能数据被集成到模拟中,从而能够对系统在飓风引起的中断情况下的性能进行真实评估。通过采用拟议的智能投资框架,决策者可以更好地识别和应对抗灾挑战。该框架通过考虑可用资源并将其与期望的复原力水平相匹配,有助于做出明智的投资决策。这种方法可避免对不必要的冗余进行过度投资,同时确保关键系统得到充分保护。我们的研究为该领域做出了贡献,在实际场景中展示了能源复原力智能投资框架的实用性和益处。校园微电网研究设施的案例研究为类似情况下的决策者提供了宝贵的见解,突出了该框架在指导弹性能源基础设施规划和投资战略方面的潜力。
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引用次数: 0
Phase-field determination of NaSICON materials in the quaternary system Na2O-P2O5-SiO2-ZrO2: II. Glass-ceramics and the phantom of excessive vacancy formation 四元系 Na2O-P2O5-SiO2-ZrO2 中 NaSICON 材料的相场测定:II.玻璃陶瓷和过量空位形成的模型
Pub Date : 2024-05-08 DOI: 10.1016/j.nxener.2024.100130
Enkhtsetseg Dashjav , Marie-Theres Gerhards , Felix Klein , Daniel Grüner , Thomas C. Hansen , Jochen Rohrer , Karsten Albe , Dina Fattakhova-Rohlfing , Frank Tietz

This work focuses on a very narrow region in the quaternary system Na2O-P2O5-SiO2-ZrO2 to explore the occasionally proposed deficiency in zirconium and oxygen content of Na+ super-ionic conductor (NaSICON) materials. In addition, this region is known for the formation of glass-ceramics, but a systematic study of such materials has not been carried out yet. For this purpose, 2 series of compositions were defined and synthesized: Na3.4Zr2-3x/4Si2.4-x/4P0.6+x/4O12-11x/8 and Na3.4Zr2-3x/4Si2.4+x/4P0.6+1.5x/4O12-x/16. They only differ in the silicate and phosphate content. In the first series the molar content is constant, nSi + nP = 3. The latter series allows an excess of the 2 cations to meet the composition Na3.1Zr1.55Si2.3P0.7O11 or alternatively re-written as Na3.4Zr1.7Si2.52P0.77Ol2, which was formerly regarded as a superior material to the frequently reported composition Na3Zr2Si2POl2.

Several characterization techniques were applied to better understand the relationships between phase formation, processing, and properties of the obtained glass ceramics in the context of the quasi-quaternary phase diagram. The investigations gave clear evidence that a glass phase is progressively formed with increasing x. Therefore, compounds with x > 0.2 have to be regarded as glass-ceramic composites. The resulting NaSICON materials revealed a very limited Zr deficiency with charge compensation by Na ions and a non-detectable amount of oxygen vacancies verified by neutron scattering and atomistic simulations.

Hence, this work is the first systematic investigation of pretended Zr-deficient NaSICON materials, which clearly show the chemistry of a 2-phase region. The 2 investigated series are directed toward a region that is orthogonal to the series Na3Zr3-ySi2PyO11.5+y/2 reported in the first part of this series of publications.

这项研究的重点是四元系 Na2O-P2O5-SiO2-ZrO2 中一个非常狭窄的区域,以探讨偶尔提出的 Na+ 超离子导体 (NaSICON) 材料中锆和氧含量不足的问题。此外,该区域已知可形成玻璃陶瓷,但尚未对此类材料进行系统研究。为此,我们定义并合成了两个系列的成分:Na3.4Zr2-3x/4Si2.4-x/4P0.6+x/4O12-11x/8 and Na3.4Zr2-3x/4Si2.4+x/4P0.6+1.5x/4O12-x/16.它们只在硅酸盐和磷酸盐含量上有所不同。在第一个系列中,摩尔含量是恒定的,即 nSi + nP = 3。后一个系列允许过量的两种阳离子符合 Na3.1Zr1.55Si2.3P0.7O11 的成分,或者改写为 Na3.4Zr1.7Si2.52P0.77Ol2,这曾被认为是一种优于经常报道的 Na3Zr2Si2POl2 成分的材料。为了在准四元相图的背景下更好地理解所获得的玻璃陶瓷的相形成、加工和性能之间的关系,我们采用了多种表征技术。研究清楚地表明,玻璃相是随着 x 的增加而逐渐形成的,因此,x > 0.2 的化合物必须被视为玻璃陶瓷复合材料。通过中子散射和原子模拟验证,所得到的 NaSICON 材料显示出非常有限的 Zr 缺乏,Na 离子对其进行了电荷补偿,氧空位的数量也无法检测到。所研究的两个系列与本系列出版物第一部分中报告的 Na3Zr3-ySi2PyO11.5+y/2 系列正交。
{"title":"Phase-field determination of NaSICON materials in the quaternary system Na2O-P2O5-SiO2-ZrO2: II. Glass-ceramics and the phantom of excessive vacancy formation","authors":"Enkhtsetseg Dashjav ,&nbsp;Marie-Theres Gerhards ,&nbsp;Felix Klein ,&nbsp;Daniel Grüner ,&nbsp;Thomas C. Hansen ,&nbsp;Jochen Rohrer ,&nbsp;Karsten Albe ,&nbsp;Dina Fattakhova-Rohlfing ,&nbsp;Frank Tietz","doi":"10.1016/j.nxener.2024.100130","DOIUrl":"https://doi.org/10.1016/j.nxener.2024.100130","url":null,"abstract":"<div><p>This work focuses on a very narrow region in the quaternary system Na<sub>2</sub>O-P<sub>2</sub>O<sub>5</sub>-SiO<sub>2</sub>-ZrO<sub>2</sub> to explore the occasionally proposed deficiency in zirconium and oxygen content of Na<sup>+</sup> super-ionic conductor (NaSICON) materials. In addition, this region is known for the formation of glass-ceramics, but a systematic study of such materials has not been carried out yet. For this purpose, 2 series of compositions were defined and synthesized: Na<sub>3.4</sub>Zr<sub>2-3x/4</sub>Si<sub>2.4-x/4</sub>P<sub>0.6+x/4</sub>O<sub>12-11x/8</sub> and Na<sub>3.4</sub>Zr<sub>2-3x/4</sub>Si<sub>2.4+x/4</sub>P<sub>0.6+1.5x/4</sub>O<sub>12-x/16</sub>. They only differ in the silicate and phosphate content. In the first series the molar content is constant, <em>n</em><sub><em>Si</em></sub> <em>+ n</em><sub><em>P</em></sub> = 3. The latter series allows an excess of the 2 cations to meet the composition Na<sub>3.1</sub>Zr<sub>1.55</sub>Si<sub>2.3</sub>P<sub>0.7</sub>O<sub>11</sub> or alternatively re-written as Na<sub>3.4</sub>Zr<sub>1.7</sub>Si<sub>2.52</sub>P<sub>0.77</sub>O<sub>l2</sub>, which was formerly regarded as a superior material to the frequently reported composition Na<sub>3</sub>Zr<sub>2</sub>Si<sub>2</sub>PO<sub>l2</sub>.</p><p>Several characterization techniques were applied to better understand the relationships between phase formation, processing, and properties of the obtained glass ceramics in the context of the quasi-quaternary phase diagram. The investigations gave clear evidence that a glass phase is progressively formed with increasing x. Therefore, compounds with x &gt; 0.2 have to be regarded as glass-ceramic composites. The resulting NaSICON materials revealed a very limited Zr deficiency with charge compensation by Na ions and a non-detectable amount of oxygen vacancies verified by neutron scattering and atomistic simulations.</p><p>Hence, this work is the first systematic investigation of pretended Zr-deficient NaSICON materials, which clearly show the chemistry of a 2-phase region. The 2 investigated series are directed toward a region that is orthogonal to the series Na<sub>3</sub>Zr<sub>3-y</sub>Si<sub>2</sub>P<sub>y</sub>O<sub>11.5+y/2</sub> reported in the first part of this series of publications.</p></div>","PeriodicalId":100957,"journal":{"name":"Next Energy","volume":"4 ","pages":"Article 100130"},"PeriodicalIF":0.0,"publicationDate":"2024-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949821X24000358/pdfft?md5=cc10a3a0bc5bf99a59fd6f724affc8ff&pid=1-s2.0-S2949821X24000358-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140880490","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Flame modified carbon-based electrodes as positive electrode for high performance of hydrogen/iron battery 火焰改性碳基电极作为高性能氢/铁电池的正极
Pub Date : 2024-05-07 DOI: 10.1016/j.nxener.2024.100132
Xiong Dan , Wei Li , Fandi Ning , Qinglin Wen , Can He , Zhi Chai , Xiaochun Zhou

The electrode is a core component that affects the overall performance of the hydrogen/iron redox flow battery. To address the drawbacks associated with the limited electrochemical activity and fewer active sites of the carbon-based electrode, this study employs a straightforward and effective flame method to synthesize carbon nanotubes (CNTs) on carbon paper and NiO/CNT composite on graphite felt. The CNT on the modified carbon-based electrode contains many hydrophilic and oxygen-containing functional groups, greatly improving the hydrophilicity of the electrode, thereby increasing the electrochemical surface area. The modified carbon-based electrode exhibits better electrochemical activity due to the CNT or NiO/CNT providing more active sites. At 50 mA cm−2, the energy efficiency of pristine carbon paper and graphite felt is 60.8% and 52.4%, respectively, while the energy efficiency of the modified carbon paper and graphite felt reached 75.3% and 80.5%, respectively. The modified carbon-based electrode achieves a 100% coulombic efficiency, with no significant degradation in energy efficiency after running for 300 cycles, demonstrating excellent stability. This study not only investigates the performance of graphite felt electrodes in hydrogen/iron batteries but also proposes a flame method for preparing CNT-modified carbon-based electrodes for high-performance hydrogen/iron batteries.

电极是影响氢/铁氧化还原液流电池整体性能的核心部件。针对碳基电极电化学活性有限、活性位点较少的缺点,本研究采用直接有效的火焰法在碳纸上合成碳纳米管(CNT),在石墨毡上合成 NiO/CNT 复合材料。改性碳基电极上的 CNT 含有许多亲水和含氧官能团,大大提高了电极的亲水性,从而增加了电化学表面积。由于 CNT 或 NiO/CNT 提供了更多的活性位点,改性碳基电极表现出更高的电化学活性。在 50 mA cm-2 的条件下,原始碳纸和石墨毡的能量效率分别为 60.8% 和 52.4%,而改性碳纸和石墨毡的能量效率分别达到 75.3% 和 80.5%。改性碳基电极的库仑效率达到了 100%,在运行 300 个循环后,能量效率没有明显降低,表现出极佳的稳定性。该研究不仅探讨了石墨毡电极在氢/铁电池中的性能,还提出了一种火焰法制备碳纳米管改性碳基电极,用于高性能氢/铁电池。
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引用次数: 0
Small modular nuclear reactors: A pathway to cost savings and environmental progress in SAGD operations 小型模块化核反应堆:在 SAGD 运行中实现成本节约和环境进步的途径
Pub Date : 2024-05-07 DOI: 10.1016/j.nxener.2024.100128
Samaneh Ashoori, Ian D. Gates

Small Modular Nuclear Reactors (SMRs) offer a promising option for environmentally friendly bitumen recovery operations. The extraction of oil sands in Western Canada is vital for the economy, but traditional methods like Steam-Assisted Gravity Drainage (SAGD) contribute significantly to greenhouse gas (GHG) emissions. In SAGD, steam generation, primarily fueled by natural gas combustion, is the main source of emissions. Given the imperative to reduce carbon intensity, less emissive recovery methods are needed to sustain production and economic viability in Canadian oil sands. Currently, there are limited non-carbon alternatives for steam generation in oil sands applications. The utilization of SMRs for steam generation presents a clean alternative. In this study, we examine the feasibility of employing SMRs in in-situ oil sands recovery operations. Through standardized economic metrics and sensitivity analysis, we demonstrate that integrating SMRs into SAGD operations eliminates GHG emissions significantly and can potentially outperform conventional natural gas-based steam generation in terms of net present value, under certain operational scenarios. Hence, our findings indicate that SMRs hold promise for decarbonizing oil sands recovery processes.

小型模块化核反应堆(SMRs)为环保型沥青开采作业提供了一种前景广阔的选择。加拿大西部的油砂开采对经济至关重要,但蒸汽辅助重力泄油(SAGD)等传统方法却大大增加了温室气体(GHG)的排放量。在 SAGD 中,主要以天然气燃烧为燃料的蒸汽发电是主要的排放源。鉴于降低碳强度势在必行,需要采用排放较少的开采方法来维持加拿大油砂的生产和经济可行性。目前,油砂应用中用于蒸汽生产的非碳替代方法十分有限。利用 SMR 生产蒸汽是一种清洁的替代方法。在本研究中,我们探讨了在油砂原地采油作业中使用 SMR 的可行性。通过标准化的经济指标和敏感性分析,我们证明将 SMRs 集成到 SAGD 作业中可显著减少温室气体排放,并且在某些作业情况下,就净现值而言,SMRs 有可能优于传统的天然气蒸汽发电。因此,我们的研究结果表明,SMRs 有望实现油砂开采过程的去碳化。
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引用次数: 0
Editorial: Aqueous rechargeable batteries: Current status and what’s next 社论:水性可充电电池:现状与未来
Pub Date : 2024-05-07 DOI: 10.1016/j.nxener.2024.100129
Hong Jin Fan , Chunyi Zhi , Jiang Zhou , Dongliang Chao
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引用次数: 0
Synergistic coupling of optical field and built-in electric field for lithium-sulfur batteries with high cyclabilities and energy densities 高循环能力和高能量密度锂硫电池的光场和内置电场协同耦合效应
Pub Date : 2024-05-06 DOI: 10.1016/j.nxener.2024.100134
Yu-Hao Liu , Cheng-Ye Yang , Chun-Yu Yu , Jia-Cheng Yu , Mei-Chen Han , Jia-Hao Zhang , Yu Yu , Zhong-Zhen Yu , Jin Qu

Photo-assisted lithium sulfur batteries (PA-LSBs) provide vital and sustainable protocols for promoting sulfur redox reactions via powerful photoinduced effects. However, precise control of the stepwise adsorption, diffusion and photocatalytic conversion of polysulfides at the surface of photocatalysts is required to accelerate the photo-assisted process. Herein, optical field and built-in electric field synergistically-assisted LSBs are developed with a p-n junction of Co3O4-TiO2 on the carbon cloth, possessing a spontaneously generated built-in electric field and a well-matched energy band structure with sulfur redox reactions. Under light irradiation, the directional migration of soluble polysulfides and the space separation of photogenerated carriers are achieved with the synergistical coupling of the optical field and built-in electric field to precisely regulate the selective deposition of Li2S and inhibit the shuttle effect via an effective photocatalytic-promoted process, leading to a maximum capacity of 1087 mAh g−1 at 2 C and a low capacity attenuation of 0.068% per cycle at 5 C. A high areal capacity of 9.6 mAh cm−2 and a great potential photo-charge process can be realized with light irradiation. Furthermore, the stability of lithium metal anodes is improved accordingly. This work demonstrates a new insight to develop high-performance LSBs with a multifield synergistical coupling protocol.

光辅助锂硫电池(PA-LSBs)通过强大的光诱导效应,为促进硫氧化还原反应提供了重要的可持续方案。然而,要加速光助过程,就必须精确控制光催化剂表面多硫化物的逐步吸附、扩散和光催化转化。本文利用碳布上的 Co3O4-TiO2 p-n 结开发了光场和内置电场协同辅助的 LSB,它具有自发产生的内置电场和与硫氧化还原反应相匹配的能带结构。在光照射下,通过光场和内置电场的协同耦合,实现了可溶性多硫化物的定向迁移和光生载流子的空间分离,从而精确地调节了 Li2S 的选择性沉积,并通过有效的光催化促进过程抑制了穿梭效应,在 2 C 时实现了 1087 mAh g-1 的最大容量,在 5 C 时实现了每周期 0.068% 的低容量衰减。在光照射下,可实现 9.6 mAh cm-2 的高单位容量和潜力巨大的光充电过程。此外,锂金属阳极的稳定性也得到了相应提高。这项研究为利用多场协同耦合协议开发高性能 LSB 提供了新的思路。
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引用次数: 0
Scalable Slurry-Casting Fabrication of Ultrathin, Flexible, and High-Voltage Halide-based Composite Solid-State Electrolytes for Lithium Metal Batteries 为金属锂电池制造超薄、柔性和高电压卤化物基复合固态电解质的可扩展浆状铸造技术
Pub Date : 2024-05-02 DOI: 10.1016/j.nxener.2024.100120
Junjie Chen , Yu Wang , Yanke Lin , Jianbo Xu , Yiju Li , Tianshou Zhao

Flexible composite polymer electrolytes with high ionic conductivity, high voltage, and small thickness are critical for achieving scalable fabrication of high-energy-density solid-state lithium metal batteries (SSLMBs). Owing to the intrinsically lower density (2.5–3.0 g cm−3) than that of oxides (>4.0 g cm−3), high ionic conductivity (∼10−3 S cm−1), high modulus, and high voltage, halides can be used as effective functional Li-ion-conductive fillers to construct thin, lightweight, and high-performance composite polymer electrolytes while achieving high-energy-density of SSLMBs. Nevertheless, the chemical vulnerability of halide solid electrolyte materials to common polar solvents restricts the scalable slurry-casting fabrication of halide-based composite polymer electrolytes for practical SSLMBs. To this end, a bi-functional low-polarity solvent, dimethyl carbonate, is screened to render halides, which are usually slurry-incompatible, amenable to scalable slurry fabrication. As a result, an ultrathin (10 µm) and flexible halide-incorporated composite electrolyte with a high electrochemical window up to 4.8 V vs. Li+/Li, high thermal stability, and desirable self-extinguishing ability is developed. Benefiting from the multiple Li-ion transport mechanisms enabled by the interaction between fillers, salts, and polymers, the obtained composite polymer electrolyte can achieve a high ionic conductivity of 0.325 mS cm–1 at 25 °C. The assembled solid-state Li|LiFePO4 cell based on the halide-based composite electrolyte achieves a high capacity of 153 mAh g−1 at 0.2 C with a capacity retention of 98% after 175 cycles, and the Li|LiNi0.6Co0.2Mn0.2O2 cell can stably cycle at a cut-off voltage of 4.3 V and achieve a high capacity of 160 mAh g−1 at 0.2 C with a capacity retention of 89% after 170 cycles. This work provides an effective strategy for large-scale manufacturing of ultrathin and flexible halide-based composite electrolytes for high-performance SSLMBs.

具有高离子电导率、高电压和小厚度的柔性复合聚合物电解质对于实现高能量密度固态锂金属电池(SSLMB)的规模化制造至关重要。由于卤化物的密度(2.5-3.0 g cm-3)比氧化物的密度(4.0 g cm-3)低、离子电导率高(10-3 S cm-1)、模量高、电压高,因此卤化物可作为有效的功能性锂离子导电填料,用于构建薄型、轻质、高性能的复合聚合物电解质,同时实现 SSLMB 的高能量密度。然而,由于卤化物固体电解质材料易受普通极性溶剂的化学影响,因此限制了用于实用 SSLMB 的卤化物基复合聚合物电解质的规模化浆料浇铸制造。为此,我们筛选出一种双功能低极性溶剂--碳酸二甲酯,使通常与浆料不相容的卤化物也能用于可扩展的浆料制造。结果,一种超薄(10 微米)、柔韧的卤化物掺杂复合电解质被开发出来,这种电解质具有高达 4.8 V 的电化学窗口(相对于 Li+/Li)、高热稳定性和理想的自熄灭能力。得益于填料、盐和聚合物之间相互作用所产生的多种锂离子传输机制,所获得的复合聚合物电解质在 25 °C 时的离子电导率高达 0.325 mS cm-1。基于卤化物基复合电解质组装的固态锂|锂铁PO4电池在0.2 C条件下实现了153 mAh g-1的高容量,循环175次后容量保持率达98%;锂|镍0.6钴0.2锰0.2O2电池可在4.3 V截止电压下稳定循环,在0.2 C条件下实现了160 mAh g-1的高容量,循环170次后容量保持率达89%。这项工作为大规模制造用于高性能 SSLMB 的超薄、柔性卤化物基复合电解质提供了有效策略。
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