ACS Energy Letters 最新文献

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Electrocatalytic Reactive Capture of NO from O2-Containing Simulated Flue Gas Using Highly O2-Resistant Fe2+-(salen-SO3) for NH3 Synthesis 高抗氧化性Fe2+-(salen-SO3)电催化捕获含o2模拟烟气中NO合成NH3
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-05-20 DOI: 10.1021/acsenergylett.5c01278
Heesung Eum, Seok-Hyeon Cheong, Jiyun Kim, Seo-Jung Han, Minji Kang, Sungho Yoon, Hae-Seok Lee, Minserk Cheong, Hyunjoo Lee, Dong Ki Lee
{"title":"Electrocatalytic Reactive Capture of NO from O2-Containing Simulated Flue Gas Using Highly O2-Resistant Fe2+-(salen-SO3) for NH3 Synthesis","authors":"Heesung Eum, Seok-Hyeon Cheong, Jiyun Kim, Seo-Jung Han, Minji Kang, Sungho Yoon, Hae-Seok Lee, Minserk Cheong, Hyunjoo Lee, Dong Ki Lee","doi":"10.1021/acsenergylett.5c01278","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01278","url":null,"abstract":"Efficient removal of nitric oxide (NO) from flue gases remains a significant environmental challenge due to its low concentration, poor water solubility, and the presence of oxygen, which deactivates traditional NO absorbents such as Fe<sup>2+</sup>-EDTA. Herein, we present an electrochemistry-based reactive NO capture system using SO<sub>3</sub>-functionalized Fe<sup>2+</sup>-salen as an NO absorbent with outstanding oxygen resistance. The unique tetracoordinate structure of the salen-SO<sub>3</sub> ligand reduces the electron density at the Fe<sup>2+</sup> center, preventing its oxidation to Fe<sup>3+</sup> under air exposure. Coupled with highly porous NiMo electrocatalysts, the system achieves an NH<sub>3</sub> production rate of 2.0 mmol h<sup>–1</sup> cm<sup>–2</sup><sub>geo</sub> with 97% Faraday efficiency under 100% NO. This continuous NO capture and conversion into NH<sub>3</sub> was maintained under air-exposed conditions at 60% of the performance level under 100% NO, with stability over 160 h. Mechanistic studies reveal that Fe<sup>2+</sup> is the critical active site for NO reduction and elucidate complete reaction pathways for NH<sub>3</sub> synthesis.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"55 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097064","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
Polar-Polymer-Enabled Solvent Anchoring Effect Retunes Anion-Dominated Solvation Sheath in Gel Electrolyte 极性聚合物使溶剂锚定效应回归阴离子主导的凝胶电解质溶剂鞘
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-05-19 DOI: 10.1021/acsenergylett.5c01061
Qiqi Sun, Chengyun Ma, Jiafeng Li, Leyuan Ma, Xuehui Li, Tao Zhang, Zhiwei Zhang, Rutao Wang, Zhao Qian, Guilong Wang, Longwei Yin, Chengxiang Wang
{"title":"Polar-Polymer-Enabled Solvent Anchoring Effect Retunes Anion-Dominated Solvation Sheath in Gel Electrolyte","authors":"Qiqi Sun, Chengyun Ma, Jiafeng Li, Leyuan Ma, Xuehui Li, Tao Zhang, Zhiwei Zhang, Rutao Wang, Zhao Qian, Guilong Wang, Longwei Yin, Chengxiang Wang","doi":"10.1021/acsenergylett.5c01061","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01061","url":null,"abstract":"The application of nonflammable gel polymer electrolytes (GPEs) with triethyl phosphate (TEP) solvents is severely impeded by the incompatibility of free TEP molecules on electrode–electrolyte interfaces. Here, to overcome this obstacle, we synthesize an in situ designed GPE (FGPE) by incorporating fluorinated polar−polymer poly-2,2,2-trifluoroethyl methacrylate (PTFMA) into a lithium difluoro(oxalato)borate (LiDFOB)–TEP-based liquid electrolyte. An innovative TEP solvent anchoring effect via dipole–dipole intermolecular chemistry of PTFMA polymer skeleton to TEP solvents is proposed, which breaks the solvation dominance of TEP solvents and facilitates reconstruction of a DFOB<sup>–</sup>-dominated Li<sup>+</sup> solvation sheath, thereby fostering anion-derived interfacial protective layers. Detailed interfacial resistance evolution revealed accelerated interfacial Li<sup>+</sup> transport kinetics. Therefore, the Li|FGPE|Li cell achieves a remarkably prolonged cycle life of over 5000 h at 0.1 mA cm<sup>–2</sup> and the Li|FGPE|LCO cell demonstrates 90.4% capacity retention after 600 cycles. This work of manipulating the solvent anchoring effect presents different insights into enhancing the interfacial compatibility of GPEs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"134 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088238","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
The Importance of Fabricating Hard Carbon-Based Full Cells to Overcome Sodium Metal Anode Limitations in Evaluating High-Mass-Loading Cathodes 在评估高质量负载阴极时,制造硬质碳基全电池克服金属钠阳极限制的重要性
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-05-19 DOI: 10.1021/acsenergylett.5c00479
Huiya Yang, Yuejing Zeng, Wei Li, Yang Yang, Jinbao Zhao
{"title":"The Importance of Fabricating Hard Carbon-Based Full Cells to Overcome Sodium Metal Anode Limitations in Evaluating High-Mass-Loading Cathodes","authors":"Huiya Yang, Yuejing Zeng, Wei Li, Yang Yang, Jinbao Zhao","doi":"10.1021/acsenergylett.5c00479","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00479","url":null,"abstract":"Developing advanced cathode materials is pivotal for successful commercialization of sodium-ion batteries (SIBs), but it requires reliable evaluation of electrochemical performance. However, the widely used sodium metal anode in academic research is not a “qualified counter electrode”, particularly under high-mass-loading and limited-Na conditions. Herein, the limitations of Na metal anode are discussed, and reliable high-mass-loading hard carbon (HC)-based full cells are proposed with a detailed guideline provided for qualified slurry preparation, electrode fabrication, and cell design. Three-electrode tests reveal Na metal’s severe potential fluctuations, which influences the evaluation of electrochemical performance for high-mass-loading NaNi<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> cathodes. Encouragingly, HC-based pouch cells demonstrate good electrochemical performance, including lower polarization (∼0.07 Ω ohmic resistance), enhanced cycling stability (85% retention after 250 cycles), and rate performance (80% capacity maintained at 4 C), highlighting the exceptional reliability and suitability. This study offers a robust methodology for evaluating lab-developed cathode materials, bridging the gap between academia and industrial applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"31 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088236","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
Multifunctional Tunnel Structural Interfacial Modulation Promises Fast-Charge and Long-Life Na-Layered Oxides 多功能隧道结构界面调制有望实现快速充电和长寿命的钠层氧化物
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-05-19 DOI: 10.1021/acsenergylett.5c01161
Xin-Yu Zhang, Ling-Yi Kong, Junjie Ding, Yan-Fang Zhu, Jia-Yang Li, Zhuang-Chun Jian, Hanshen Xin, Meng-Ying Li, Peng Tan, Wei Kong Pang, Shi-Xue Dou, Yao Xiao
{"title":"Multifunctional Tunnel Structural Interfacial Modulation Promises Fast-Charge and Long-Life Na-Layered Oxides","authors":"Xin-Yu Zhang, Ling-Yi Kong, Junjie Ding, Yan-Fang Zhu, Jia-Yang Li, Zhuang-Chun Jian, Hanshen Xin, Meng-Ying Li, Peng Tan, Wei Kong Pang, Shi-Xue Dou, Yao Xiao","doi":"10.1021/acsenergylett.5c01161","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01161","url":null,"abstract":"Na-layered oxides are famous for their environmental friendliness and facile synthesis, however, developing cathodes with fast Na<sup>+</sup> transport kinetics, robust structure, and air/water stability to realize fast-charge and long-life layered oxide cathodes for sodium-ion batteries (SIBs) remains a great challenge. Herein, we propose the concept of multifunctional tunnel interfacial modulation to stabilize the phase structure of P2-Na<sub>2/3</sub>Ni<sub>1/3</sub>Mn<sub>1/3</sub>Ti<sub>1/3</sub>O<sub>2</sub>. Relying on the unique structure of the Na<sub>0.44</sub>MnO<sub>2</sub> with S-channel, the modified electrode prepared with an aqueous binder achieves capacity retention of 80.87% after 4000 cycles at 2C. The calculation results of stress simulation reveal that the tunnel structure could dissipate the mechanical stress of the P2 phase upon cycling. Overall, such multifunctional tunnel interfacial modulation provides a new research direction for the development of fast-charge and long-life SIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"55 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144088241","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
Diketopyrrolopyrroles Act as Redox Mediators in Lithium–Sulfur Batteries 二酮吡咯在锂硫电池中的氧化还原介质作用
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-05-17 DOI: 10.1021/acsenergylett.5c01262
Joanne S. Searle, Ferdinando Malagreca, Benjamin M. G. Denison, Alexander J. Kibler, Darren A. Walsh, Lee R. Johnson, David B. Amabilino, Graham N. Newton
{"title":"Diketopyrrolopyrroles Act as Redox Mediators in Lithium–Sulfur Batteries","authors":"Joanne S. Searle, Ferdinando Malagreca, Benjamin M. G. Denison, Alexander J. Kibler, Darren A. Walsh, Lee R. Johnson, David B. Amabilino, Graham N. Newton","doi":"10.1021/acsenergylett.5c01262","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01262","url":null,"abstract":"Lithium–sulfur (Li–S) batteries are among the most promising next-generation energy storage technologies, offering gravimetric energy densities greater than those of state-of-the-art lithium-ion batteries. However, widespread commercialization of the technology is hindered by challenges related to the multistep redox chemistry of sulfur. The addition of diketopyrollopyrroles (DPPs) to Li–S battery electrolytes can improve cell performance; however, their mechanism of action remains unclear. Here, we use a range of electrochemical methods to elucidate the mechanism through which DPPs affect the performance of the Li–S batteries. Electrochemical analysis demonstrates the importance of DPP redox potentials in enhancing the redox kinetics of polysulfide reduction, with analytical measurements confirming this is via a redox mediation process in which electrons are shuttled between polysulfide intermediates and the underlying current collector via the DPP molecule. We show that DPP derivatives that are not redox active at the potentials associated with the multi-step interconversion of sulfur and lithium sulfide in Li–S batteries do not show the same effect. Galvanostatic analysis confirms that the enhancement of the kinetics of polysulfide conversion translates to the operation of Li–S batteries, which show an improvement in the discharge capacity after the addition of the additives.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"64 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066968","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
Probing Capacity Decay in Vanadium Oxide Cathodes of Aqueous Zinc-Ion Batteries Using Operando EQCM-D 用EQCM-D探测水锌离子电池氧化钒阴极容量衰减
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-05-16 DOI: 10.1021/acsenergylett.5c00901
Zijian Li, Yuexin Liu, Shu Yang, Zhenghui Pan, Congcong Liu, Xiaoli Zhao, Xiaowei Yang
{"title":"Probing Capacity Decay in Vanadium Oxide Cathodes of Aqueous Zinc-Ion Batteries Using Operando EQCM-D","authors":"Zijian Li, Yuexin Liu, Shu Yang, Zhenghui Pan, Congcong Liu, Xiaoli Zhao, Xiaowei Yang","doi":"10.1021/acsenergylett.5c00901","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00901","url":null,"abstract":"Zn-ion batteries are promising for their safety and cost-effectiveness. Vanadium-based compounds are notable due to their layered structure and polyvalent nature, enabling high-rate capability and large capacity. The type and properties of charge carriers critically influence the structural and performance stability of vanadium-based electrodes, which, however, remain obscure. Herein, we elucidate the H<sup>+</sup>-dominated intercalation mechanism of vanadium oxide and its correlation with capacity degradation via an electrochemical quartz crystal microbalance investigation. By tracking real-time mass changes and ion diffusion during the electrochemical process, we demonstrate that H<sup>+</sup> is the predominant shuttling cation. H<sup>+</sup> intercalation generates OH<sup>–</sup> at the electrode–electrolyte interface, causing alkaline dissolution of vanadium oxide and the capacity decay. With nanosized modification, the dissolution can be mitigated. The electrode exhibits a capacity retention of 98.2% after 2000 cycles at 5 A g<sup>–1</sup>. This study deepens the understanding of vanadium oxide’s charge storage, guiding the design of high-performance aqueous batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"36 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066575","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
Solvent–Binder Engineering for a Practically Viable Solution Process for Fabricating Sulfide-Based All-Solid-State Batteries 一种实际可行的制造硫化物基全固态电池的溶液工艺的溶剂粘合剂工程
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-05-16 DOI: 10.1021/acsenergylett.5c00762
Jihoon Oh, Seung Ho Choi, Heejin Kim, Woo Jun Chung, Minkwan Kim, Inwoo Kim, Taeyong Lee, Jieun Lee, Dong Ok Kim, Sunung Moon, Donghoon Kim, Jang Wook Choi
{"title":"Solvent–Binder Engineering for a Practically Viable Solution Process for Fabricating Sulfide-Based All-Solid-State Batteries","authors":"Jihoon Oh, Seung Ho Choi, Heejin Kim, Woo Jun Chung, Minkwan Kim, Inwoo Kim, Taeyong Lee, Jieun Lee, Dong Ok Kim, Sunung Moon, Donghoon Kim, Jang Wook Choi","doi":"10.1021/acsenergylett.5c00762","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00762","url":null,"abstract":"The commercial viability of sulfide all-solid-state batteries (ASSBs) has been hindered by limited solvent compatibility in solution processing as sulfide solid electrolytes (SEs) degrade in polar solvents. This constraint significantly restricts binder selection, which is critical for both performance─particularly at low pressures─and processability. This study addresses this critical issue by investigating thermoplastic polyurethane (TPU) as a binder dissolved in 1,6-dichlorohexane (DCH), a solvent specifically tailored for sulfide ASSBs. TPU demonstrates outstanding adhesion properties in composite anode, cathode, and SE layers, which not only enhance the long-term cycling performance but also enable double-cast solution processing with minimal binder content for electrode-SE layer manufacturing. A silicon-graphite (Si-Gr)-based pouch-cell fabricated through this solution process maintained 80% capacity retention over 100 cycles under practical conditions (40 μm SE layer, 25 °C, and 2 MPa), validating its practical feasibility. The successful implementation of this optimized solvent–binding system for solution processing represents a significant advancement toward practical ASSB technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"74 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144067087","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
Charge Transfer from Perovskite Quantum Dots to Multifunctional Ligands with Tethered Molecular Species 钙钛矿量子点与系链分子的多功能配体之间的电荷转移
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-05-15 DOI: 10.1021/acsenergylett.5c00881
Mariam Kurashvili, Lena S. Stickel, Jordi Llusar, Christian Wilhelm, Fabian Felixberger, Ivana Ivanović-Burmazović, Ivan Infante, Jochen Feldmann, Quinten A. Akkerman
{"title":"Charge Transfer from Perovskite Quantum Dots to Multifunctional Ligands with Tethered Molecular Species","authors":"Mariam Kurashvili, Lena S. Stickel, Jordi Llusar, Christian Wilhelm, Fabian Felixberger, Ivana Ivanović-Burmazović, Ivan Infante, Jochen Feldmann, Quinten A. Akkerman","doi":"10.1021/acsenergylett.5c00881","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00881","url":null,"abstract":"Perovskite quantum dots (pQDs) are promising materials for optoelectronic and photocatalytic applications due to their unique optical properties. To enhance charge carrier extraction or injection, donor/acceptor molecules can be tethered to the pQD. These molecules must strongly bind to the ionic surfaces of pQDs without compromising colloidal stability. This is achieved by using multifunctional ligands containing a quaternary ammonium binding group for strong pQD surface attachment, a long tail group for colloidal stability, and a functional group near the pQD surface. Such pQDs with ferrocene-functionalized ligands show fast photoexcited hole transfer with near-unity efficiency. Density functional theory calculations reveal how ferrocene’s molecular structure reorganizes following hole transfer, affecting its charge separation efficiency. This approach can also be extended to photoexcited electron and energy transfer processes with pQDs. Therefore, this strategy offers a blueprint for creating efficient pQD–molecular hybrids for applications like photocatalysis.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"25 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066443","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
Rational Design of Phosphate Cathodes with Improved Na-storage Performance 提高na存储性能的磷酸盐阴极的合理设计
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-05-15 DOI: 10.1021/acsenergylett.5c00653
Xusheng Zhang, Huican Mao, Zhao Chen, Lin Zhou, Lilu Liu, Mingxuan Wu, Zilong Lv, Zhihao Zhang, Yukun Zhong, Yong-Sheng Hu, Junmei Zhao
{"title":"Rational Design of Phosphate Cathodes with Improved Na-storage Performance","authors":"Xusheng Zhang, Huican Mao, Zhao Chen, Lin Zhou, Lilu Liu, Mingxuan Wu, Zilong Lv, Zhihao Zhang, Yukun Zhong, Yong-Sheng Hu, Junmei Zhao","doi":"10.1021/acsenergylett.5c00653","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00653","url":null,"abstract":"As a typical Na-superionic conductor (NASICON), the Na<sub>3+<i>x</i></sub>V<sub>2–<i>x</i></sub>Mn<sub><i>x</i></sub>(PO<sub>4</sub>)<sub>3</sub> cathodes have a high capacity of over 120 mA g<sup>–1</sup> owing to the multielectron reaction. However, these cathodes always show structural degradation and sluggish Na-ion diffusion kinetics derived from the Jahn-Teller distortion of Mn. Here, Al<sup>3+</sup> was first used to replace Mn<sup>2+</sup> in Na<sub>3.5</sub>V<sub>1.5</sub>Mn<sub>0.5</sub>(PO<sub>4</sub>)<sub>3</sub>, which could significantly reduce the Jahn-Teller distortion through regulating the MnO<sub>6</sub> local crystal structure and enhancing Mn–O bond strength. Additionally, Al<sup>3+</sup> could also increase the electronic conductivity and the Na-ion migration ability. As a result, the as-prepared Na<sub>3.3</sub>V<sub>1.5</sub>Mn<sub>0.3</sub>Al<sub>0.2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode achieved a high-rate capacity of 96.8 mAh g<sup>–1</sup> at 20 C and a high-capacity retention of 88.8% after 3000 cycles at 10 C. The application prospects of Na<sub>3.3</sub>V<sub>1.5</sub>Mn<sub>0.3</sub>Al<sub>0.2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode were further confirmed by a scale-up synthesis, and a 21700-type cylindrical cell showed an excellent cycling performance of over 80% capacity retention after 4000 cycles at 1 C.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"120 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066442","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
Regulating Bond Structure in Polyanion Cathode for Long-Cycle-Life Sodium-Ion Batteries 长循环寿命钠离子电池聚阴离子阴极键结构调控研究
IF 22 1区 材料科学
ACS Energy Letters Pub Date : 2025-05-15 DOI: 10.1021/acsenergylett.5c00769
Shuoshuo Cheng, Yibing Zhang, Peng Lv, Shiyu Li, Ying Bai
{"title":"Regulating Bond Structure in Polyanion Cathode for Long-Cycle-Life Sodium-Ion Batteries","authors":"Shuoshuo Cheng, Yibing Zhang, Peng Lv, Shiyu Li, Ying Bai","doi":"10.1021/acsenergylett.5c00769","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00769","url":null,"abstract":"The NASICON-type Na<sub>4</sub>MnV(PO<sub>4</sub>)<sub>3</sub> (NMVP) cathode is a potential candidate for sodium-ion batteries (SIBs) due to its intrinsic safety and cost advantages. However, its performance is limited by intrinsic low electronic conductivity and Jahn–Teller distortion of Mn. In this study, Co is substituted at the Mn site to take advantage of the stronger polarization effect of Co<sup>2+</sup> and the ionic radius difference, which shortens the Mn–O bond length and strengthens its bonding, stabilizing the MnO<sub>6</sub> octahedral structure. Furthermore, Co doping lowers the Na<sup>+</sup> migration energy barrier and facilitates more efficient Na<sup>+</sup> transport. Therefore, the prepared NMCVP-0.05 sample exhibits a stable cycling performance (retaining 88.9% after 3800 cycles at 10 C) and rate performance (71.7 mAh g<sup>–1</sup> at 50 C). This work reveals the mechanism by which regulating the bond structure in NMVP affects sodium storage performance and proposes a stability-enhancing strategy for Mn-based polyanionic cathodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"129 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143979872","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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