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Charge Transfer in 2D Halide Perovskites and 2D/3D Heterostructures 二维卤化物包光体和二维/三维异质结构中的电荷转移
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-17 DOI: 10.1021/acsenergylett.4c01530
Chenjian Lin, Yuanhao Tang, Wenzhan Xu, Prashant Kumar, Letian Dou
Halide perovskites have emerged as a versatile class of materials, with applications spanning photovoltaics, light-emitting diodes, transistors, and photodetectors. The introduction of semiconducting ligands to form two-dimensional (2D) perovskites on the surface of three-dimensional (3D) perovskites in perovskite solar cells has been shown to enhance the performance and stability. To improve the interface properties between the 3D perovskite layer and charge carrier transport layers, understanding the charge transfer (CT) process in 2D perovskites is crucial. In this Perspective, we address common terminological inaccuracies in energy level descriptions, delineate methods for energy alignment characterization, and present practical instances of CT in 2D perovskite-incorporated solar cells. We emphasize the significance of precise terminology, appropriate measurement techniques, and rational design of 2D ligands to harness the full potential of 2D perovskites in optoelectronic applications.
卤化物包晶已成为一类用途广泛的材料,其应用领域涵盖光伏、发光二极管、晶体管和光电探测器。在包晶体太阳能电池的三维(3D)包晶体表面引入半导体配体形成二维(2D)包晶体,已被证明可以提高性能和稳定性。为了改善三维包晶层与电荷载流子传输层之间的界面特性,了解二维包晶的电荷转移(CT)过程至关重要。在本《视角》中,我们讨论了能级描述中常见的术语不准确问题,阐述了能级排列表征方法,并介绍了二维包晶太阳能电池中电荷转移的实际案例。我们强调精确的术语、适当的测量技术和二维配体的合理设计对于充分发挥二维包晶在光电应用中的潜力具有重要意义。
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引用次数: 0
Redox-Mediated Electrodialysis for Desalination, Environmental Remediation, and Resource Recovery 用于海水淡化、环境修复和资源回收的氧化还原电渗析技术
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-17 DOI: 10.1021/acsenergylett.4c00913
Nayeong Kim, Aderiyike Aguda, Choonsoo Kim, Xiao Su
Electrochemically driven separation technologies have become a promising avenue for tackling environmental and energy challenges. By bridging redox-based energy storage and desalination, redox-mediated electrodialysis (redox-ED) platforms can perform continuous desalination from brackish water to seawater with reduced energy consumption. Over the past few years, redox-ED has further expanded its applications to wastewater treatment, selective recovery of metals, and even biomanufacturing. Here, we review the rapidly evolving field of redox-ED technologies in desalination, environmental remediation, and resource recovery. The molecular design of redox species and membranes has played a critical role in enhancing capabilities and improving efficiency. We delve into the fundamental principles behind the technology as well as recent advances in the field, covering system engineering, material design, integration of renewable energy sources, and economic assessment. Lastly, we discuss the upcoming opportunities and challenges facing industrial implementation, such as addressing multicomponent separations, utilizing biphasic systems, and gaining deeper molecular-level mechanistic insights.
电化学驱动分离技术已成为应对环境和能源挑战的一条大有可为的途径。氧化还原介导电渗析(Redox-ED)平台将氧化还原储能与海水淡化有机地结合在一起,可以在降低能耗的同时实现从苦咸水到海水的连续海水淡化。在过去几年中,氧化还原电渗析的应用进一步扩展到废水处理、金属的选择性回收,甚至生物制造。在此,我们将回顾在海水淡化、环境修复和资源回收领域快速发展的氧化还原-电子技术。氧化还原物种和膜的分子设计在增强能力和提高效率方面发挥了至关重要的作用。我们将深入探讨该技术背后的基本原理以及该领域的最新进展,包括系统工程、材料设计、可再生能源的整合以及经济评估。最后,我们讨论了工业应用即将面临的机遇和挑战,例如解决多组分分离、利用双相系统以及获得更深入的分子级机理见解。
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引用次数: 0
Fatigue Phase Suppression in Aged High Nickel Layered Cathodes by Aluminum Substitution during Co-precipitation 通过共沉淀过程中的铝置换抑制老化高镍层阴极中的疲劳相
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-17 DOI: 10.1021/acsenergylett.4c01199
Ben Pei, Hui Zhou, Yanxu Zong, Xiaobo Chen, Mateusz J. Zuba, Guangwen Zhou, Hao Liu, M. Stanley Whittingham
LiNi0.8Mn0.1Co0.1O2 (NMC811) is a promising cathode material for lithium-ion batteries (LIBs) in electric vehicle applications but faces severe capacity and voltage decay issues, especially when cycled at high voltages (>4.2 V) which is essential to fully exploit its energy density. A portion of aged NMC811 becomes fatigued above 4.2 V, making further delithiation difficult and limiting the charge window to <74% lithium, which contributes to capacity loss and significant overpotential growth at high voltage. This fatigue structural degradation is universal in pure NMC cathodes with various morphologies and cannot be alleviated by tuning the kinetic limitation via slow charging. However, substituting aluminum uniformly into the NMC811 material effectively suppresses this fatigue phase. Consequently, the mid-point voltage decay was reduced by nearly 84%, enhancing the energy density from 529 to 645 Wh/kg after 150 cycles. This work provides insights into the stabilization mechanism of high-Ni layered oxides and realizes high-energy-density cathodes for LIBs.
LiNi0.8Mn0.1Co0.1O2(NMC811)是一种很有前途的电动汽车锂离子电池(LIB)正极材料,但它面临着严重的容量和电压衰减问题,尤其是在高电压(4.2 V)下循环时,这对充分发挥其能量密度至关重要。部分老化的 NMC811 在 4.2 V 以上会出现疲劳,从而难以进一步脱锂,并将充电窗口限制在 74% 锂的范围内,这导致了容量损失和高压下显著的过电位增长。这种疲劳结构退化在具有各种形态的纯 NMC 正极中普遍存在,无法通过慢速充电调整动力学限制来缓解。然而,在 NMC811 材料中均匀添加铝可以有效抑制这一疲劳阶段。因此,中点电压衰减降低了近 84%,150 个周期后能量密度从 529 Wh/kg 提高到 645 Wh/kg。这项研究深入探讨了高镍层状氧化物的稳定机制,实现了 LIB 的高能量密度阴极。
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引用次数: 0
Elastic Polymer Electrolytes Integrated with In Situ Polymerization-Transferred Electrodes toward Stretchable Batteries 弹性聚合物电解质与原位聚合转移电极集成,实现可伸缩电池
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-17 DOI: 10.1021/acsenergylett.4c01254
Shi Wang, Shijun Xiao, Henan Cai, Wenqing Sun, Tong Wu, Yu Wang, Jixin He, Sheng Yang, Zhen-Dong Huang, Wen-Yong Lai
Stretchable Li-ion batteries (LIBs) are important potential power sources for flexible electronics. Here, we propose an integrated in situ polymerization-transfer strategy to construct intrinsically stretchable LIBs (is-LIBs). Specifically, a polymer electrolyte (PE) with chain-liquid synergistic effect by poly(ethylene glycol methyl ether acrylate)-ionic liquid/lithium salt has been developed, which facilitates rapid Li+ transport (10–4 S cm–1) and promotes mechanical flexibility (stretching over 5000%) due to the unique phase-separated structure of the PE and the ionic–bipolar interactions between the C=O-rich polymer and imidazolium cations. Additionally, Ag nanowires (AgNWs)/electrode materials are transferred to PDMS to construct intrinsically stretchable electrodes. The strong physical interaction between AgNWs/electrode materials and PDMS endows electrodes with a high strain of 100% and low sheet resistance of 0.9 Ω □–1. Finally, an is-LIB is achieved by in situ polymerization-transfer integration, showing good cycle and rate performance. The results suggest a new avenue for the development of stretchable energy storage devices.
可拉伸锂离子电池(LIB)是柔性电子产品的重要潜在电源。在此,我们提出了一种原位聚合-转移综合策略,用于构建本征可拉伸锂离子电池(is-LIBs)。具体来说,通过聚(乙二醇甲基醚丙烯酸酯)-离子液体/锂盐开发出了一种具有链-液协同效应的聚合物电解质(PE),由于 PE 独特的相分离结构以及富含 C=O 的聚合物和咪唑阳离子之间的离子-双极相互作用,该电解质可促进 Li+ 的快速传输(10-4 S cm-1)并提高机械柔性(拉伸超过 5000%)。此外,Ag 纳米线(AgNWs)/电极材料被转移到 PDMS 上,从而构建了本征可拉伸电极。AgNWs/电极材料与 PDMS 之间强烈的物理相互作用使电极具有 100% 的高应变和 0.9 Ω □-1 的低薄层电阻。最后,通过原位聚合-转移集成实现了等效 LIB,显示出良好的循环和速率性能。这些结果为开发可拉伸储能器件提供了一条新途径。
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引用次数: 0
A Coordinated-Anion-Enriched Electrolyte for Lean-Electrolyte Li–S Batteries 用于贫电解质锂-S 电池的协调阴离子富集电解质
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-15 DOI: 10.1021/acsenergylett.4c00859
Kaiqiang Qin, Shi Li, Dean Yen, Weiran Zhang, Zhenzhen Yang, Ethan Phillip Kamphaus, Eric Youngsam Kim, Jinghao Huang, John J. Shea, Enyuan Hu, Lei Cheng, Chunsheng Wang, Chao Luo
The solid electrolyte interphase (SEI) on Li and cathode electrolyte interphase (CEI) at sulfurized polyacrylonitrile (SPAN) formed in the commonly used liquid electrolytes cannot accommodate the large volume change of both Li anode and SPAN cathode, resulting in severe electrolyte and Li consumption and fast capacity decay under high mass loading and lean electrolyte conditions. Herein, a LiF-rich SEI and a LiF–LixNyOz coenriched CEI are simultaneously formed by adding ionic liquid (Py13TFSI) in the localized high-concentration electrolyte (LHCE), which forms a coordinated-anion-enriched solvation structure. The LiF-rich interphase results in less stress/strain during large volume changes of Li and SPAN, therefore achieving obviously improved stability even at a high areal capacity. Consequently, Li (50 μm)||SPAN (6 mg cm–2) pouch cells under the lean electrolyte conditions (E/S ratio of 5 mL gSPAN–1) deliver a stable cycle life of 120 cycles with 79.2% capacity retention, demonstrating great promise for high-energy-density lithium–sulfur batteries.
在常用液态电解质中形成的锂固态电解质相(SEI)和硫化聚丙烯腈(SPAN)阴极电解质相(CEI)无法适应锂阳极和 SPAN 阴极的巨大体积变化,导致在高负载质量和贫电解质条件下电解质和锂消耗严重,容量衰减快。在此,通过在局部高浓度电解质(LHCE)中加入离子液体(Py13TFSI),形成配位离子富集的溶解结构,同时形成富含 LiF 的 SEI 和 LiF-LixNyOz 共富集的 CEI。富含 LiF 的中间相在锂和 SPAN 发生较大体积变化时产生的应力/应变较小,因此即使在高电容下也能明显提高稳定性。因此,在贫电解质条件下(E/S 比为 5 mL gSPAN-1),锂(50 μm)||SPAN(6 mg cm-2)袋装电池的循环寿命稳定在 120 次,容量保持率为 79.2%,为高能量密度的锂硫电池带来了巨大前景。
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引用次数: 0
Complete Single-Pass Conversion of Dilute Nitrate to Ammonia Using Cu/Co(OH)2 Tandem Electrocatalyst 使用 Cu/Co(OH)2 串联电催化剂将稀硝酸盐完全单程转化为氨气
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-15 DOI: 10.1021/acsenergylett.4c01247
Zhuanghe Ren, Kaige Shi, Zhen Meng, Maia D. Willis, Xiaofeng Feng
Electrochemical nitrate reduction reaction (NO3RR) provides a promising route for the denitrification of wastewater and sustainable NH3 production but requires active and selective electrocatalysts. Here, we demonstrate a rigorous design of a tandem electrocatalyst for efficient conversion of NO3 to NH3. Based on the screening of tandem components, a catalyst coupling Cu and Co(OH)2 with an optimal ratio and tandem architecture was developed to promote and balance the activities of sequential NO3RR steps on different active sites. Compared to counterpart catalysts including Cu, Co(OH)2, and Cu–Co alloy, the Cu/Co(OH)2 catalyst with separated phases showed much higher activity and selectivity for the NO3RR to NH3, suggesting a tandem mechanism that involves NO3 reduction to NO2 on Cu and solution transfer and further reduction of NO2 to NH3 on Co-based sites. When operated in a flow cell, the Cu/Co(OH)2 catalyst achieved 100% single-pass conversion of dilute NO3 solution to NH3 at low overpotentials.
电化学硝酸盐还原反应(NO3RR)为废水脱氮和可持续生产 NH3 提供了一条前景广阔的途径,但需要活性和选择性电催化剂。在此,我们展示了一种严格的串联电催化剂设计,用于将 NO3- 高效转化为 NH3。在对串联组分进行筛选的基础上,我们开发了一种具有最佳比例和串联结构的 Cu 和 Co(OH)2 偶联催化剂,以促进和平衡不同活性位点上的 NO3RR 顺序步骤的活性。与包括 Cu、Co(OH)2 和 Cu-Co 合金在内的对应催化剂相比,具有分离相的 Cu/Co(OH)2 催化剂在 NO3RR 到 NH3 的过程中表现出更高的活性和选择性,这表明串联机制包括在 Cu 上将 NO3 还原为 NO2-,以及在 Co 基位点上将 NO2-溶液转移并进一步还原为 NH3。在流动池中运行时,Cu/Co(OH)2 催化剂在低过电位下实现了稀 NO3- 溶液到 NH3 的 100% 单程转化。
{"title":"Complete Single-Pass Conversion of Dilute Nitrate to Ammonia Using Cu/Co(OH)2 Tandem Electrocatalyst","authors":"Zhuanghe Ren, Kaige Shi, Zhen Meng, Maia D. Willis, Xiaofeng Feng","doi":"10.1021/acsenergylett.4c01247","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01247","url":null,"abstract":"Electrochemical nitrate reduction reaction (NO<sub>3</sub>RR) provides a promising route for the denitrification of wastewater and sustainable NH<sub>3</sub> production but requires active and selective electrocatalysts. Here, we demonstrate a rigorous design of a tandem electrocatalyst for efficient conversion of NO<sub>3</sub><sup>–</sup> to NH<sub>3</sub>. Based on the screening of tandem components, a catalyst coupling Cu and Co(OH)<sub>2</sub> with an optimal ratio and tandem architecture was developed to promote and balance the activities of sequential NO<sub>3</sub>RR steps on different active sites. Compared to counterpart catalysts including Cu, Co(OH)<sub>2</sub>, and Cu–Co alloy, the Cu/Co(OH)<sub>2</sub> catalyst with separated phases showed much higher activity and selectivity for the NO<sub>3</sub>RR to NH<sub>3</sub>, suggesting a tandem mechanism that involves NO<sub>3</sub><sup>–</sup> reduction to NO<sub>2</sub><sup>–</sup> on Cu and solution transfer and further reduction of NO<sub>2</sub><sup>–</sup> to NH<sub>3</sub> on Co-based sites. When operated in a flow cell, the Cu/Co(OH)<sub>2</sub> catalyst achieved 100% single-pass conversion of dilute NO<sub>3</sub><sup>–</sup> solution to NH<sub>3</sub> at low overpotentials.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141618422","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
“Faraday Cage” Induced Anion-Confined Interface Enables Industrially Compatible Microsized Silicon Anodes "法拉第笼 "诱导阴离子约束界面实现了工业兼容的微型硅阳极
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-15 DOI: 10.1021/acsenergylett.4c01517
Ziyun Zhao, Jingshuo Zhang, Jiawei Shi, Fanqi Chen, Yong Guo, Siyuan Pan, Yingxin Liu, Xiangze Xin, Yun Tian, Zhen Zhou, Shichao Wu, Zhe Weng, Quan-Hong Yang
The anion-derived inorganic-rich solid electrolyte interphase (SEI) provides highly desirable protection for anodes; however, it is hardly formed in commercial electrolytes due to the electromigration of free anions away from anodes under the charging electric field. High-concentration electrolytes are capable of curing this issue, but they are economically impractical. Here, we pioneer an industrially compatible approach to shield the electric field by engineering a surface “Faraday cage” from a polymer matrix electrostatically integrated with a weakly dissociated salt. An anion-confined interphase (ACI) is produced on the representative silicon microparticles (SiMPs). The ACI enables a sustainable anion-enriched microenvironment, which promotes the participation of anions in the Li+ solvation sheath and guarantees more anion reduction to the inorganic-rich SEI upon long cycling stability at a high areal capacity (∼4 mAh cm–2). This approach offers a straightforward yet practical solution to SEI innovation in commercial batteries.
阴离子衍生的富含无机物的固体电解质间相(SEI)为阳极提供了非常理想的保护;然而,由于游离阴离子在充电电场作用下会电迁移离开阳极,因此在商用电解质中几乎不会形成SEI。高浓度电解质能够解决这一问题,但在经济上并不可行。在这里,我们开创了一种与工业兼容的屏蔽电场的方法,即利用聚合物基质与弱离解盐的静电结合,在其表面制造一个 "法拉第笼"。在具有代表性的硅微颗粒(SiMPs)上产生了阴离子封闭相(ACI)。ACI 实现了可持续的阴离子富集微环境,促进了阴离子参与 Li+ 溶胶鞘,并保证了在高电容(∼4 mAh cm-2)下长期稳定循环时,更多的阴离子还原到富含无机物的 SEI 中。这种方法为商业电池中 SEI 的创新提供了一种直接而实用的解决方案。
{"title":"“Faraday Cage” Induced Anion-Confined Interface Enables Industrially Compatible Microsized Silicon Anodes","authors":"Ziyun Zhao, Jingshuo Zhang, Jiawei Shi, Fanqi Chen, Yong Guo, Siyuan Pan, Yingxin Liu, Xiangze Xin, Yun Tian, Zhen Zhou, Shichao Wu, Zhe Weng, Quan-Hong Yang","doi":"10.1021/acsenergylett.4c01517","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01517","url":null,"abstract":"The anion-derived inorganic-rich solid electrolyte interphase (SEI) provides highly desirable protection for anodes; however, it is hardly formed in commercial electrolytes due to the electromigration of free anions away from anodes under the charging electric field. High-concentration electrolytes are capable of curing this issue, but they are economically impractical. Here, we pioneer an industrially compatible approach to shield the electric field by engineering a surface “Faraday cage” from a polymer matrix electrostatically integrated with a weakly dissociated salt. An anion-confined interphase (ACI) is produced on the representative silicon microparticles (SiMPs). The ACI enables a sustainable anion-enriched microenvironment, which promotes the participation of anions in the Li<sup>+</sup> solvation sheath and guarantees more anion reduction to the inorganic-rich SEI upon long cycling stability at a high areal capacity (∼4 mAh cm<sup>–2</sup>). This approach offers a straightforward yet practical solution to SEI innovation in commercial batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141618423","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sulfonated-Ligand Engineering Enables a Stable Alkaline All-Iron Ion Redox Flow Battery 磺化配体工程实现了稳定的碱性全铁离子氧化还原液流电池
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-15 DOI: 10.1021/acsenergylett.4c01550
Wendong Yang, Hua Jiang, Linfeng Wang, Pei Liu, Jintao Meng, Shuangyan Gui, Xue Long, Xuan Cai, Yilin Zeng, Yifan Zhang, Jinhua Guo, Jun Wang, Jun Zhou, Jiangjiang Duan
Alkaline all-iron ion redox flow batteries (RFBs) are considered promising devices for large-scale energy storage due to their remarkable resistance to dendrite formation and the hydrogen evolution reaction. However, the decomposition of negative complexes and ligand crossover issues have limited their stable operation. Herein, we have developed a tetra-sulfonated ethylenediamine derivative ligand (EDTS) to chelate with iron ions to serve as the negative active species (Fe(EDTS)). Benefiting from its stable hexa-coordinated structure, the Fe(EDTS) chelate exhibits unprecedented stability during long-term cycling. Additionally, the EDTS ligand with high charge density and large volume effectively mitigates crossover through size exclusion and Donnan effects. Paired with the Fe(CN)6 electrolyte, the Fe(CN)6/Fe(EDTS) RFB demonstrates a formal cell voltage of 1.25 V, a high energy density of 25.04 Ah L–1, and an unprecedented durability among reported capacity-symmetric all-iron RFBs, achieving a Coulombic efficiency of 99.93% and capacity retention of 96.08% after 3000 cycles.
碱性全铁离子氧化还原液流电池(RFBs)具有显著的抗枝晶形成和抗氢气进化反应能力,因此被认为是具有大规模储能前景的设备。然而,负极配合物的分解和配体交叉问题限制了其稳定运行。在此,我们开发了一种四磺化乙二胺衍生物配体(EDTS),可与铁离子螯合,作为负活性物种(Fe(EDTS))。得益于其稳定的六配位结构,Fe(EDTS)螯合物在长期循环过程中表现出前所未有的稳定性。此外,EDTS 配体电荷密度高、体积大,可通过尺寸排阻和唐南效应有效缓解交叉。与 Fe(CN)6 电解质配对后,Fe(CN)6/Fe(EDTS) RFB 的正式电池电压为 1.25 V,能量密度高达 25.04 Ah L-1,在已报道的容量对称全铁 RFB 中具有前所未有的耐用性,3000 次循环后库仑效率达到 99.93%,容量保持率达到 96.08%。
{"title":"Sulfonated-Ligand Engineering Enables a Stable Alkaline All-Iron Ion Redox Flow Battery","authors":"Wendong Yang, Hua Jiang, Linfeng Wang, Pei Liu, Jintao Meng, Shuangyan Gui, Xue Long, Xuan Cai, Yilin Zeng, Yifan Zhang, Jinhua Guo, Jun Wang, Jun Zhou, Jiangjiang Duan","doi":"10.1021/acsenergylett.4c01550","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01550","url":null,"abstract":"Alkaline all-iron ion redox flow batteries (RFBs) are considered promising devices for large-scale energy storage due to their remarkable resistance to dendrite formation and the hydrogen evolution reaction. However, the decomposition of negative complexes and ligand crossover issues have limited their stable operation. Herein, we have developed a tetra-sulfonated ethylenediamine derivative ligand (EDTS) to chelate with iron ions to serve as the negative active species (Fe(EDTS)). Benefiting from its stable hexa-coordinated structure, the Fe(EDTS) chelate exhibits unprecedented stability during long-term cycling. Additionally, the EDTS ligand with high charge density and large volume effectively mitigates crossover through size exclusion and Donnan effects. Paired with the Fe(CN)<sub>6</sub> electrolyte, the Fe(CN)<sub>6</sub>/Fe(EDTS) RFB demonstrates a formal cell voltage of 1.25 V, a high energy density of 25.04 Ah L<sup>–1</sup>, and an unprecedented durability among reported capacity-symmetric all-iron RFBs, achieving a Coulombic efficiency of 99.93% and capacity retention of 96.08% after 3000 cycles.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141618424","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Operando Focused Ion Beam–Scanning Electron Microscope (FIB-SEM) Revealing Microstructural and Morphological Evolution in a Solid-State Battery 揭示固态电池微结构和形态演变的操作型聚焦离子束扫描电子显微镜 (FIB-SEM)
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acsenergylett.4c01750
Patrice Perrenot, Pascale Bayle-Guillemaud, Pierre-Henri Jouneau, Adrien Boulineau, Claire Villevieille
Thiophosphates have emerged as a promising solid electrolyte for the forthcoming solid-state battery technology only if transport properties, both electronic and ionic, can be controlled within the composite electrode. Unfortunately, during cycling, several chemo-mechanical degradations are occurring hindering the transport properties inside the batteries. Solutions could be provided if one could track the dynamics of such degradation processes. The development of a specific operando focused ion beam–scanning electron microscope (FIB-SEM) approach helps us to perform imaging during cycling and thus address the dynamic morphological investigation of a composite electrode LiNi0.6Mn0.2Co0.2O2 (NMC622 coupled to amorphous Li3PS4). This advanced methodology makes it possible to highlight the mechanical stress endured by the electroactive materials and by the electrolyte during cycling. In this study, polycrystalline NMC622 microstructural evolution was monitored during charge and discharge, showing that the polycrystalline morphology is poorly adapted to solid-state batteries and that the interface adhesion should be better controlled to enhance the electrochemical performance.
硫代磷酸盐是一种前景广阔的固态电解质,只有在复合电极内部的电子和离子传输特性得到控制的情况下,这种电解质才有可能被应用于未来的固态电池技术中。遗憾的是,在循环过程中,一些化学机械降解现象会阻碍电池内部的传输特性。如果能跟踪这些降解过程的动态,就能找到解决方案。开发一种特殊的操作式聚焦离子束扫描电子显微镜(FIB-SEM)方法有助于我们在循环过程中进行成像,从而解决复合电极 LiNi0.6Mn0.2Co0.2O2(NMC622 与无定形 Li3PS4 相耦合)的动态形态研究问题。这种先进的方法可以突出显示电活性材料和电解液在循环过程中承受的机械应力。本研究监测了多晶 NMC622 在充放电过程中的微观结构演变,结果表明多晶形态对固态电池的适应性较差,应更好地控制界面粘附以提高电化学性能。
{"title":"Operando Focused Ion Beam–Scanning Electron Microscope (FIB-SEM) Revealing Microstructural and Morphological Evolution in a Solid-State Battery","authors":"Patrice Perrenot, Pascale Bayle-Guillemaud, Pierre-Henri Jouneau, Adrien Boulineau, Claire Villevieille","doi":"10.1021/acsenergylett.4c01750","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01750","url":null,"abstract":"Thiophosphates have emerged as a promising solid electrolyte for the forthcoming solid-state battery technology only if transport properties, both electronic and ionic, can be controlled within the composite electrode. Unfortunately, during cycling, several chemo-mechanical degradations are occurring hindering the transport properties inside the batteries. Solutions could be provided if one could track the dynamics of such degradation processes. The development of a specific <i>operando</i> focused ion beam–scanning electron microscope (FIB-SEM) approach helps us to perform imaging during cycling and thus address the dynamic morphological investigation of a composite electrode LiNi<sub>0.6</sub>Mn<sub>0.2</sub>Co<sub>0.2</sub>O<sub>2</sub> (NMC622 coupled to amorphous Li<sub>3</sub>PS<sub>4</sub>). This advanced methodology makes it possible to highlight the mechanical stress endured by the electroactive materials and by the electrolyte during cycling. In this study, polycrystalline NMC622 microstructural evolution was monitored during charge and discharge, showing that the polycrystalline morphology is poorly adapted to solid-state batteries and that the interface adhesion should be better controlled to enhance the electrochemical performance.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602870","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Formal Oxidation States and Coordination Environments in the Catalytic Reduction of CO to Methanol 催化 CO 还原成甲醇过程中的形式氧化态和配位环境
IF 22 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-12 DOI: 10.1021/acsenergylett.4c01269
Irene Barba-Nieto, Andressa V. Müller, Charles J. Titus, Dominik Wierzbicki, Cherno Jaye, Mehmed Z. Ertem, Gerald J. Meyer, Javier J. Concepcion, José A. Rodriguez
Fundamental insight into multielectron, multiproton redox reactions with organometallic catalysts is greatly facilitated by knowledge of the formal oxidation state of the metal center in each of the elementary reaction steps that comprise the catalytic cycle. X-ray absorption near edge structure (XANES) is utilized herein to quantify the oxidation states and coordination environment of the organometallic resting state and intermediates in a newly proposed catalytic reduction of carbon monoxide to methanol.
了解构成催化循环的每个基本反应步骤中金属中心的形式氧化态,有助于从根本上了解有机金属催化剂的多电子、多质子氧化还原反应。本文利用 X 射线吸收近边缘结构 (XANES) 来量化一氧化碳催化还原为甲醇过程中有机金属静止态和中间产物的氧化态和配位环境。
{"title":"Formal Oxidation States and Coordination Environments in the Catalytic Reduction of CO to Methanol","authors":"Irene Barba-Nieto, Andressa V. Müller, Charles J. Titus, Dominik Wierzbicki, Cherno Jaye, Mehmed Z. Ertem, Gerald J. Meyer, Javier J. Concepcion, José A. Rodriguez","doi":"10.1021/acsenergylett.4c01269","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01269","url":null,"abstract":"Fundamental insight into multielectron, multiproton redox reactions with organometallic catalysts is greatly facilitated by knowledge of the formal oxidation state of the metal center in each of the elementary reaction steps that comprise the catalytic cycle. X-ray absorption near edge structure (XANES) is utilized herein to quantify the oxidation states and coordination environment of the organometallic resting state and intermediates in a newly proposed catalytic reduction of carbon monoxide to methanol.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141602847","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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