Pub Date : 2024-11-25DOI: 10.1016/j.jpowsour.2024.235888
Hao Tan , Hao Zhong , Liwen Deng , Jinlong Zhou , Ao Xu , Dang Wu , Sheng Chen
With fast development of modern industries and electrical systems, polymer dielectrics are urgently demanded to have high discharged energy density (Ud) in elevated temperature. In this paper, novel core-shell poly [2-((3,6,7,10,11-pentakis (hexyloxy) triphenylene-2-yl) oxy) ethyl methacrylate] (PHT) coated barium titanate nanoparticles (BT) (denoted as PHT@BT) are prepared, and then incorporate into polyetherimide (PEI) matrix via solution blending method. Semi-conductive organic shell layer can not only promote the dispersion and compatibility of BT nanoparticles but also construct deep trap. As a result, 0.3 wt% PHT@BT/PEI composites achieve maximal Ud of 7.62 J cm−3 at 641 MV m−1 and room temperature, which is 1.93 times that of pure PEI film (3.93 J cm−3 at 461 MV m−1). Importantly, the Ud of 4.86 J cm−3 is obtained at 150 °C. This work provides superior interfacial modifier for inorganic nanofiller, which is of great significance for the fabrication of polymer-based nanocomposites with superior Ud.
{"title":"Significantly improved energy storage performance of polyetherimide-based dielectric composites via employing core-shell organic-semiconductor@BaTiO3 nanoparticles","authors":"Hao Tan , Hao Zhong , Liwen Deng , Jinlong Zhou , Ao Xu , Dang Wu , Sheng Chen","doi":"10.1016/j.jpowsour.2024.235888","DOIUrl":"10.1016/j.jpowsour.2024.235888","url":null,"abstract":"<div><div>With fast development of modern industries and electrical systems, polymer dielectrics are urgently demanded to have high discharged energy density (<em>U</em><sub><em>d</em></sub>) in elevated temperature. In this paper, novel core-shell poly [2-((3,6,7,10,11-pentakis (hexyloxy) triphenylene-2-yl) oxy) ethyl methacrylate] (PHT) coated barium titanate nanoparticles (BT) (denoted as PHT@BT) are prepared, and then incorporate into polyetherimide (PEI) matrix via solution blending method. Semi-conductive organic shell layer can not only promote the dispersion and compatibility of BT nanoparticles but also construct deep trap. As a result, 0.3 wt% PHT@BT/PEI composites achieve maximal <em>U</em><sub><em>d</em></sub> of 7.62 J cm<sup>−3</sup> at 641 MV m<sup>−1</sup> and room temperature, which is 1.93 times that of pure PEI film (3.93 J cm<sup>−3</sup> at 461 MV m<sup>−1</sup>). Importantly, the <em>U</em><sub><em>d</em></sub> of 4.86 J cm<sup>−3</sup> is obtained at 150 °C. This work provides superior interfacial modifier for inorganic nanofiller, which is of great significance for the fabrication of polymer-based nanocomposites with superior <em>U</em><sub><em>d</em></sub>.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"628 ","pages":"Article 235888"},"PeriodicalIF":8.1,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723384","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-25DOI: 10.1016/j.jpowsour.2024.235915
Jaemin Kim , Songge Yang , Yu Zhong , Geoffrey Tompsett , Seonghun Jeong , Junyoung Mun , Neelam Sunariwal , Jordi Cabana , Zhenzhen Yang , Yan Wang
High-entropy oxides (HEOs) are emerging as promising cathode materials for Li-ion batteries (LIBs) due to their stable solid-state phase and compositional flexibility. Herein, we investigate the structural and electrochemical properties of a novel non-equimolar high-entropy cathode material, termed high-entropy Li-rich layered oxide (HE-LLO, Li1.15Na0.05Ni0.19Mn0.56Fe0.02Mg0.02Al0.02O1.97F0.03), in comparison to a pristine Li-rich layered oxide (PR-LLO, Li1.2Ni0.2Mn0.6O2). The incorporation of multiple cations (Na+, Al3+, Mg2+, Fe3+) and anion (F−) into HE-LLO introduces compositional diversity, enhancing structural stability through the entropy stabilization effect. Theoretical calculations confirm a significantly higher configurational entropy in HE-LLO compared to PR-LLO, supporting its high-entropy nature. Electrochemical evaluations demonstrate that HE-LLO exhibits considerable capacity retention, preserving 76.8 % of its discharge capacity at 0.5C after 200 cycles, compared to only 36.2 % for PR-LLO. Even under high-temperature conditions, HE-LLO outperformed PR-LLO, maintaining 76.1 % of its discharge capacity after 100 cycles at 5C, while PR-LLO retained only 12.4 %. These enhancements are attributed to the improved phase reversibility and higher Li+ ion diffusion coefficients of HE-LLO, validated by ex-situ characterizations using a synchrotron X-ray technique, along with density functional theory (DFT) calculations. These findings highlight the promise of non-equimolar HEOs as a novel design strategy for high-performance cathode materials.
{"title":"High-entropy Li-rich layered oxide cathode for Li-ion batteries","authors":"Jaemin Kim , Songge Yang , Yu Zhong , Geoffrey Tompsett , Seonghun Jeong , Junyoung Mun , Neelam Sunariwal , Jordi Cabana , Zhenzhen Yang , Yan Wang","doi":"10.1016/j.jpowsour.2024.235915","DOIUrl":"10.1016/j.jpowsour.2024.235915","url":null,"abstract":"<div><div>High-entropy oxides (HEOs) are emerging as promising cathode materials for Li-ion batteries (LIBs) due to their stable solid-state phase and compositional flexibility. Herein, we investigate the structural and electrochemical properties of a novel non-equimolar high-entropy cathode material, termed high-entropy Li-rich layered oxide (HE-LLO, Li<sub>1.15</sub>Na<sub>0.05</sub>Ni<sub>0.19</sub>Mn<sub>0.56</sub>Fe<sub>0.02</sub>Mg<sub>0.02</sub>Al<sub>0.02</sub>O<sub>1.97</sub>F<sub>0.03</sub>), in comparison to a pristine Li-rich layered oxide (PR-LLO, Li<sub>1.2</sub>Ni<sub>0.2</sub>Mn<sub>0.6</sub>O<sub>2</sub>). The incorporation of multiple cations (Na<sup>+</sup>, Al<sup>3+</sup>, Mg<sup>2+</sup>, Fe<sup>3+</sup>) and anion (F<sup>−</sup>) into HE-LLO introduces compositional diversity, enhancing structural stability through the entropy stabilization effect. Theoretical calculations confirm a significantly higher configurational entropy in HE-LLO compared to PR-LLO, supporting its high-entropy nature. Electrochemical evaluations demonstrate that HE-LLO exhibits considerable capacity retention, preserving 76.8 % of its discharge capacity at 0.5C after 200 cycles, compared to only 36.2 % for PR-LLO. Even under high-temperature conditions, HE-LLO outperformed PR-LLO, maintaining 76.1 % of its discharge capacity after 100 cycles at 5C, while PR-LLO retained only 12.4 %. These enhancements are attributed to the improved phase reversibility and higher Li<sup>+</sup> ion diffusion coefficients of HE-LLO, validated by ex-situ characterizations using a synchrotron X-ray technique, along with density functional theory (DFT) calculations. These findings highlight the promise of non-equimolar HEOs as a novel design strategy for high-performance cathode materials.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"628 ","pages":"Article 235915"},"PeriodicalIF":8.1,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723634","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-25DOI: 10.1016/j.jpowsour.2024.235902
Jian Wen , Li Wang , Xiangming He
The intricate interplay of multi-scale and multi-physics phenomena within battery systems poses a substantial challenge in harmonizing microscopic electrochemical processes. This complexity impedes the advancement of innovative designs for large-scale transportation and energy storage applications, frequently culminating in prohibitively high costs. Anticipating the real-world impact of laboratory-developed batteries on industrial devices remains largely an elusive endeavor. Nonetheless, physics-based numerical inquiries have emerged as a promising approach to illuminating the interactions across various battery domains and scales, ranging from the individual cell to the system level. Physical models, grounded in a set of assumptions, may result in critical inaccuracies when based on ill-informed predictions, a particular risk within the nuanced sphere of battery design, which is fraught with complex physical and chemical interactions. This paper endeavors to clarify the subtleties of numerical models utilized in battery research and design. It seeks to demystify the development of battery models by drawing on physical expressions from scholarly works to map the interconnections among diverse models. This paper provides an insight into the subject, delineating the essential electrochemical governing equations, equivalent circuit models, degradation mechanisms, and methodologies for multi-physics integration, thereby establishing a robust framework for the exploration and creation of cutting-edge battery technologies.
{"title":"Navigating the intricacies: A critical review of numerical modeling in battery research and design","authors":"Jian Wen , Li Wang , Xiangming He","doi":"10.1016/j.jpowsour.2024.235902","DOIUrl":"10.1016/j.jpowsour.2024.235902","url":null,"abstract":"<div><div>The intricate interplay of multi-scale and multi-physics phenomena within battery systems poses a substantial challenge in harmonizing microscopic electrochemical processes. This complexity impedes the advancement of innovative designs for large-scale transportation and energy storage applications, frequently culminating in prohibitively high costs. Anticipating the real-world impact of laboratory-developed batteries on industrial devices remains largely an elusive endeavor. Nonetheless, physics-based numerical inquiries have emerged as a promising approach to illuminating the interactions across various battery domains and scales, ranging from the individual cell to the system level. Physical models, grounded in a set of assumptions, may result in critical inaccuracies when based on ill-informed predictions, a particular risk within the nuanced sphere of battery design, which is fraught with complex physical and chemical interactions. This paper endeavors to clarify the subtleties of numerical models utilized in battery research and design. It seeks to demystify the development of battery models by drawing on physical expressions from scholarly works to map the interconnections among diverse models. This paper provides an insight into the subject, delineating the essential electrochemical governing equations, equivalent circuit models, degradation mechanisms, and methodologies for multi-physics integration, thereby establishing a robust framework for the exploration and creation of cutting-edge battery technologies.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"628 ","pages":"Article 235902"},"PeriodicalIF":8.1,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723321","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-25DOI: 10.1016/j.jpowsour.2024.235867
Peilin Ran , Xiaoqing Li , Kang Wu , Na Li , Kesheng Gao , Chenzhang Gu , Jinkui Zhao , Enyue Zhao , Zhimin Wu , Fangwei Wang
Cobalt-free Lithium-rich layered oxides (LRLOs) are promising cathodes for low-cost and high-energy-density Li-ion batteries. However, their remarkable capacity comes with challenges including structural degradation, irreversible oxygen release and sluggish kinetics. Herein, we conduct a one-step dual-modified strategy by yttrium doping and Li3PO4 surface modification. Combining density-functional theory calculations with in-situ X-ray diffraction and in-situ differential electrochemical mass spectrometry, the Y3+ doping and Li3PO4 nano coating modified LRLOs is demonstrated has an excellent structural stability with enhanced Li⁺ diffusion kinetics and stabilized oxygen lattice. Excellent rate performance and thermal stability are achieved: high discharge specific capacity of 221 mAh·g−1 at room temperature (96.5 % at 1 C after 100 cycles) and incredible discharge specific capacity of 210 mAh·g−1 at 55 °C (91.8 % at 2 C after 100 cycles). This work resolves the safety and stability issues and provides a feasible strategy for Co-free LRLOs.
{"title":"Enabling stable cobalt-free Li-rich cathodes through a one-step dual-modified strategy","authors":"Peilin Ran , Xiaoqing Li , Kang Wu , Na Li , Kesheng Gao , Chenzhang Gu , Jinkui Zhao , Enyue Zhao , Zhimin Wu , Fangwei Wang","doi":"10.1016/j.jpowsour.2024.235867","DOIUrl":"10.1016/j.jpowsour.2024.235867","url":null,"abstract":"<div><div>Cobalt-free Lithium-rich layered oxides (LRLOs) are promising cathodes for low-cost and high-energy-density Li-ion batteries. However, their remarkable capacity comes with challenges including structural degradation, irreversible oxygen release and sluggish kinetics. Herein, we conduct a one-step dual-modified strategy by yttrium doping and Li<sub>3</sub>PO<sub>4</sub> surface modification. Combining density-functional theory calculations with <em>in-situ</em> X-ray diffraction and <em>in-situ</em> differential electrochemical mass spectrometry, the Y<sup>3+</sup> doping and Li<sub>3</sub>PO<sub>4</sub> nano coating modified LRLOs is demonstrated has an excellent structural stability with enhanced Li⁺ diffusion kinetics and stabilized oxygen lattice. Excellent rate performance and thermal stability are achieved: high discharge specific capacity of 221 mAh·g<sup>−1</sup> at room temperature (96.5 % at 1 C after 100 cycles) and incredible discharge specific capacity of 210 mAh·g<sup>−1</sup> at 55 °C (91.8 % at 2 C after 100 cycles). This work resolves the safety and stability issues and provides a feasible strategy for Co-free LRLOs.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"628 ","pages":"Article 235867"},"PeriodicalIF":8.1,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723637","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-24DOI: 10.1016/j.jpowsour.2024.235905
Rita Salloum , François Rabuel , Sara Abada , Mathieu Morcrette
The occurrence of an Internal Short-Circuit (ISC) in 18650 lithium-ion cells under thermal abuse conditions remains elusive. Equipped with Current Interrupt Devices (CID), the cell's voltage drop may introduce ambiguity, and potentially obscure the precise determination of an ISC. Therefore, comprehensive investigations were undertaken to rigorously explore the ISC and thermal runaway (TR) relationship.
In this paper, and for the first time, a three-electrode 18650 lab-scale cell is tested in an Accelerated Rate Calorimeter (ARC) to analyze the potentials' variation under adiabatic conditions. Results have shown that the cell's voltage drop coincides with the positive potential drop (Ewe). Furthermore, tests on cells without CID have indicated that the accelerated TR is triggered following the massive ISC.
Moreover, for a long time, the ISC has been associated with the melting of the separator. Hence, this study includes tests on identical lab-scale cells utilizing three types of separators: polyethylene, trilayer, and coated polypropylene. TR tests, conducted under adiabatic and ambient conditions, didn't reveal a significant impact of the separators. Given that the novel preliminary test developed in this study has demonstrated that the loss of their mechanical integrity happens at around the same temperature, the outcomes of the TR tests were comparable.
{"title":"Investigating the internal short-circuit in 18650 cells under thermal abuse conditions","authors":"Rita Salloum , François Rabuel , Sara Abada , Mathieu Morcrette","doi":"10.1016/j.jpowsour.2024.235905","DOIUrl":"10.1016/j.jpowsour.2024.235905","url":null,"abstract":"<div><div>The occurrence of an Internal Short-Circuit (ISC) in 18650 lithium-ion cells under thermal abuse conditions remains elusive. Equipped with Current Interrupt Devices (CID), the cell's voltage drop may introduce ambiguity, and potentially obscure the precise determination of an ISC. Therefore, comprehensive investigations were undertaken to rigorously explore the ISC and thermal runaway (TR) relationship.</div><div>In this paper, and for the first time, a three-electrode 18650 lab-scale cell is tested in an Accelerated Rate Calorimeter (ARC) to analyze the potentials' variation under adiabatic conditions. Results have shown that the cell's voltage drop coincides with the positive potential drop (E<sub>we</sub>). Furthermore, tests on cells without CID have indicated that the accelerated TR is triggered following the massive ISC.</div><div>Moreover, for a long time, the ISC has been associated with the melting of the separator. Hence, this study includes tests on identical lab-scale cells utilizing three types of separators: polyethylene, trilayer, and coated polypropylene. TR tests, conducted under adiabatic and ambient conditions, didn't reveal a significant impact of the separators. Given that the novel preliminary test developed in this study has demonstrated that the loss of their mechanical integrity happens at around the same temperature, the outcomes of the TR tests were comparable.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"628 ","pages":"Article 235905"},"PeriodicalIF":8.1,"publicationDate":"2024-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723319","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-24DOI: 10.1016/j.jpowsour.2024.235912
Shoujing Mao, Ying Wu, Shurong Xu, Tianyi Xiao, Yangyang Li, Zhongkai Li, Xiaofang Pan, Bo Yuan, Yafen Xu, Hao Wen, Qingxuan Sui, Yuan Quan, Jun Liu
Aqueous zinc-ion batteries (AZIBs), distinguished by their high safety and cost-effectiveness, hold significant promise for grid-level energy storage systems. However, the strong interactions between zinc ions and the host lattice of materials lead to suboptimal cycling stability and rate performance. To address this, we present a novel superlattice structure incorporating conductive polymer (PANI) and metal cation (Ni2+) double interlayers, which can be utilized as cathodes for AZIBs. The incorporation of the conductive host polymer polyaniline (PANI) reduces the valence state of vanadium, enhances the electrical conductivity, and effectively expands the channels for zinc ion insertion. Additionally, metal cations (Ni2+) can effectively induce the synergistic interactions with zinc ions, thereby mitigating the electrostatic interactions with the V2O5 host. Consequently, the assembled Zn//PANI-NixV2O5 (PNV) battery exhibits a specific capacity of up to 470 mAh g−1 at 0.1 A g−1, and retains 89.5 % of its capacity after 1000 cycles at 5 A g−1.
锌离子水电池（AZIBs）具有安全性高、成本效益高的特点，在电网级储能系统中大有可为。然而，锌离子与材料主晶格之间的强相互作用导致循环稳定性和速率性能不理想。为解决这一问题，我们提出了一种新型超晶格结构，其中包含导电聚合物（PANI）和金属阳离子（Ni2+）双层夹层，可用作 AZIB 的阴极。导电主聚合物聚苯胺（PANI）的加入降低了钒的价态，增强了导电性，并有效扩大了锌离子的插入通道。此外，金属阳离子（Ni2+）能有效地诱导锌离子的协同作用，从而减轻与 V2O5 主基的静电作用。因此，组装好的 Zn//PANI-NixV2O5 (PNV) 电池在 0.1 A g-1 的条件下显示出高达 470 mAh g-1 的比容量，并且在 5 A g-1 条件下循环 1000 次后仍能保持 89.5% 的容量。
{"title":"Design of large-spacing, high-stability PANI-NixV2O5 nanobelts as cathode for aqueous zinc-ion batteries using an organic-inorganic co-embedding strategy","authors":"Shoujing Mao, Ying Wu, Shurong Xu, Tianyi Xiao, Yangyang Li, Zhongkai Li, Xiaofang Pan, Bo Yuan, Yafen Xu, Hao Wen, Qingxuan Sui, Yuan Quan, Jun Liu","doi":"10.1016/j.jpowsour.2024.235912","DOIUrl":"10.1016/j.jpowsour.2024.235912","url":null,"abstract":"<div><div>Aqueous zinc-ion batteries (AZIBs), distinguished by their high safety and cost-effectiveness, hold significant promise for grid-level energy storage systems. However, the strong interactions between zinc ions and the host lattice of materials lead to suboptimal cycling stability and rate performance. To address this, we present a novel superlattice structure incorporating conductive polymer (PANI) and metal cation (Ni<sup>2+</sup>) double interlayers, which can be utilized as cathodes for AZIBs. The incorporation of the conductive host polymer polyaniline (PANI) reduces the valence state of vanadium, enhances the electrical conductivity, and effectively expands the channels for zinc ion insertion. Additionally, metal cations (Ni<sup>2+</sup>) can effectively induce the synergistic interactions with zinc ions, thereby mitigating the electrostatic interactions with the V<sub>2</sub>O<sub>5</sub> host. Consequently, the assembled Zn//PANI-Ni<sub>x</sub>V<sub>2</sub>O<sub>5</sub> (PNV) battery exhibits a specific capacity of up to 470 mAh g<sup>−1</sup> at 0.1 A g<sup>−1</sup>, and retains 89.5 % of its capacity after 1000 cycles at 5 A g<sup>−1</sup>.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"628 ","pages":"Article 235912"},"PeriodicalIF":8.1,"publicationDate":"2024-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723222","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-24DOI: 10.1016/j.jpowsour.2024.235907
Jie Zhang, Rong Zou, Shengtao Niu, Guang Liu, Yuanyou Peng, Xiaoya Kang, Maocheng Liu, Fen Ran
Traditional liquid lithium-sulfur batteries possess the merits of high energy density and low cost, and have a wide application prospect in the field of energy storage; however, the growth of lithium dendrites, the side reaction of the liquid electrolyte, and the harmful “shuttle effect” of lithium polysulfides have hindered their practical application. Herein, a solid-state composite polymeric electrolyte with a macroscopic built-in polarization electric field is designed to improve lithium-ion transport and depress shuttle effect. The introduction of barium titanate as a functional filler effectively reduces the crystallinity of the polymer and promotes the dissociation of the lithium salt. At the same time, the built-in polarization electric field generated by its crystal structure provides a strong driving force for lithium-ion transport, thus accelerating lithium-ion migration. The experimental results show that the built-in electric field can enhance the lithium-ion transport and accelerate redox kinetics. Furthermore, the macroscopic charges can establish strong chemical interactions between polysulfides, which leads to the suppression of the shuttle effect and effectively improves the cycling stability of all-solid-state lithium-sulfur batteries. Benefiting from these properties, Li||Li symmetric batteries exhibit stable cycling for more than 900 h, and all-solid-state lithium-sulfur batteries have a high cycling stability of more than 200 cycles at a rate of 0.1 C. This work provides a simple and effective method for designing high-performance all-solid-state lithium-sulfur batteries.
传统的液态锂硫电池具有能量密度高、成本低的优点，在储能领域具有广泛的应用前景，但锂枝晶的生长、液态电解质的副反应以及多硫化锂的有害 "穿梭效应 "阻碍了其实际应用。在此，我们设计了一种具有宏观内置极化电场的固态复合聚合物电解质，以改善锂离子传输并抑制穿梭效应。钛酸钡作为功能填料的引入有效降低了聚合物的结晶度，促进了锂盐的解离。同时，其晶体结构产生的内置极化电场为锂离子迁移提供了强大的驱动力，从而加速了锂离子迁移。实验结果表明，内置电场能增强锂离子迁移并加速氧化还原动力学。此外，宏观电荷可在多硫化物之间建立强烈的化学作用，从而抑制穿梭效应，有效提高全固态锂硫电池的循环稳定性。得益于这些特性，锂||锂对称电池的稳定循环时间超过 900 小时，全固态锂硫电池在 0.1 C 的速率下具有超过 200 次循环的高循环稳定性。
{"title":"Macroscopic built-in polarization electric field powers high lithium-ion transport for all-solid-state lithium-sulfur batteries","authors":"Jie Zhang, Rong Zou, Shengtao Niu, Guang Liu, Yuanyou Peng, Xiaoya Kang, Maocheng Liu, Fen Ran","doi":"10.1016/j.jpowsour.2024.235907","DOIUrl":"10.1016/j.jpowsour.2024.235907","url":null,"abstract":"<div><div>Traditional liquid lithium-sulfur batteries possess the merits of high energy density and low cost, and have a wide application prospect in the field of energy storage; however, the growth of lithium dendrites, the side reaction of the liquid electrolyte, and the harmful “shuttle effect” of lithium polysulfides have hindered their practical application. Herein, a solid-state composite polymeric electrolyte with a macroscopic built-in polarization electric field is designed to improve lithium-ion transport and depress shuttle effect. The introduction of barium titanate as a functional filler effectively reduces the crystallinity of the polymer and promotes the dissociation of the lithium salt. At the same time, the built-in polarization electric field generated by its crystal structure provides a strong driving force for lithium-ion transport, thus accelerating lithium-ion migration. The experimental results show that the built-in electric field can enhance the lithium-ion transport and accelerate redox kinetics. Furthermore, the macroscopic charges can establish strong chemical interactions between polysulfides, which leads to the suppression of the shuttle effect and effectively improves the cycling stability of all-solid-state lithium-sulfur batteries. Benefiting from these properties, Li||Li symmetric batteries exhibit stable cycling for more than 900 h, and all-solid-state lithium-sulfur batteries have a high cycling stability of more than 200 cycles at a rate of 0.1 C. This work provides a simple and effective method for designing high-performance all-solid-state lithium-sulfur batteries.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"628 ","pages":"Article 235907"},"PeriodicalIF":8.1,"publicationDate":"2024-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723636","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-24DOI: 10.1016/j.jpowsour.2024.235853
Huanyan Liu , Bobo Lu , Shichao Zhang , Wenbo Liu
Traditional CuxO (x = 1, 2) electrodes exhibit excellent specific capacity, but the poor stress-buffering performance and inferior conductivity hinder its further application. To solve these issues, herein, we develop a built-in bifunctional ultrafine Cu nanocrystalline networks hybridized 3D hollow nanoporous CuxO (BUCN@3D-HN CuxO) integrated anode by a facile gas-phase Kirkendall effect. The 3D hollow nanoporous (3D-HN) structure can bidirectionally retard the change of stress, while the built-in ultrafine Cu nanocrystalline networks (BUCN) own the effect of providing rapid internal electron transport across the active/inert Cu/CuxO system. Benefiting from the synergistic effect of the excellent stress-buffering ability and improved electronic conductivity, the designed BUCN@3D-HN CuxO electrode delivers a high initial reversible capacity of 1.67 mAh cm−2 under the current density of 1 mA cm−2. Besides, a high capacity retention of 0.96 mAh cm−2 with a high capacity retention ratio of 85.7 % is achieved even after 800 cycles at a high rate of 4 mA cm−2. This work provides a facile yet effective method to prepare hollow nanoporous electrodes and emphasizes the significance of active/inert system, which may shed light on the design of other high-performance electrodes beyond Lithium-ion batteries.
传统的 CuxO（x = 1，2）电极具有出色的比容量，但应力缓冲性能差、导电性低，阻碍了其进一步应用。为了解决这些问题，我们在本文中通过简便的气相柯肯达尔效应开发了一种内置双功能超细铜纳米晶网络杂化三维中空纳米多孔 CuxO（BUCN@3D-HN CuxO）集成阳极。三维中空纳米多孔（3D-HN）结构可以双向延缓应力变化，而内置的超细铜纳米晶网络（BUCN）则具有在活性/惰性铜/CuxO体系中提供快速内部电子传输的作用。得益于优异的应力缓冲能力和更高的电子传导性的协同效应，所设计的 BUCN@3D-HN CuxO 电极在 1 mA cm-2 的电流密度下可提供 1.67 mAh cm-2 的高初始可逆容量。此外，即使在 4 mA cm-2 的高速率下循环 800 次，也能实现 0.96 mAh cm-2 的高容量保持，容量保持率高达 85.7%。这项研究为制备中空纳米多孔电极提供了一种简便而有效的方法，并强调了活性/惰性体系的重要性，这可能会为设计锂离子电池以外的其他高性能电极带来启示。
{"title":"Gas-phase Kirkendall effect inducing built-in bifunctional ultrafine Cu nanocrystalline integrated 3D hollow nanoporous CuxO anode towards excellent lithium storage performance","authors":"Huanyan Liu , Bobo Lu , Shichao Zhang , Wenbo Liu","doi":"10.1016/j.jpowsour.2024.235853","DOIUrl":"10.1016/j.jpowsour.2024.235853","url":null,"abstract":"<div><div>Traditional Cu<sub>x</sub>O (x = 1, 2) electrodes exhibit excellent specific capacity, but the poor stress-buffering performance and inferior conductivity hinder its further application. To solve these issues, herein, we develop a built-in bifunctional ultrafine Cu nanocrystalline networks hybridized 3D hollow nanoporous Cu<sub>x</sub>O (BUCN@3D-HN Cu<sub>x</sub>O) integrated anode by a facile gas-phase Kirkendall effect. The 3D hollow nanoporous (3D-HN) structure can bidirectionally retard the change of stress, while the built-in ultrafine Cu nanocrystalline networks (BUCN) own the effect of providing rapid internal electron transport across the active/inert Cu/Cu<sub>x</sub>O system. Benefiting from the synergistic effect of the excellent stress-buffering ability and improved electronic conductivity, the designed BUCN@3D-HN Cu<sub>x</sub>O electrode delivers a high initial reversible capacity of 1.67 mAh cm<sup>−2</sup> under the current density of 1 mA cm<sup>−2</sup>. Besides, a high capacity retention of 0.96 mAh cm<sup>−2</sup> with a high capacity retention ratio of 85.7 % is achieved even after 800 cycles at a high rate of 4 mA cm<sup>−2</sup>. This work provides a facile yet effective method to prepare hollow nanoporous electrodes and emphasizes the significance of active/inert system, which may shed light on the design of other high-performance electrodes beyond Lithium-ion batteries.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"628 ","pages":"Article 235853"},"PeriodicalIF":8.1,"publicationDate":"2024-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723318","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-23DOI: 10.1016/j.jpowsour.2024.235891
Meiyuan Jiao , Pan Huang , Zheyuan Pang , Sijing Wang , Honglai Liu , Yiting Lin , Cheng Lian
Direct current internal resistance (DCIR), as a fundamental characteristic of lithium-ion batteries, serves as a critical indicator for the accurate estimation and prediction of battery health. The DCIR of a battery is affected by the electrode structure. Despite its significance, the relationship between the electrode structure and the DCIR during charging and discharging remains unclear. Based on a pore network model of a lithium manganate cell, this work focuses on the cathode and quantifies the effects of cathode thickness (), porosity (), connectivity (), average particle size () and specific surface area () on DCIR. Combined with machine learning, this work identify that cathode thickness, porosity and average particle size the primary determinants of the DCIR, and the formulas for calculating charging and discharging DCIR are derived, and . This work proposes a research framework for predicting DCIR from the electrode structure, which is applicable to most porous electrode batteries, providing a theoretical basis for calculating the DCIR and is of great significance for electrode design.
{"title":"Uncovering the battery direct current internal resistance puzzle: A machine learning-driven pore network approach","authors":"Meiyuan Jiao , Pan Huang , Zheyuan Pang , Sijing Wang , Honglai Liu , Yiting Lin , Cheng Lian","doi":"10.1016/j.jpowsour.2024.235891","DOIUrl":"10.1016/j.jpowsour.2024.235891","url":null,"abstract":"<div><div>Direct current internal resistance (DCIR), as a fundamental characteristic of lithium-ion batteries, serves as a critical indicator for the accurate estimation and prediction of battery health. The DCIR of a battery is affected by the electrode structure. Despite its significance, the relationship between the electrode structure and the DCIR during charging and discharging remains unclear. Based on a pore network model of a lithium manganate cell, this work focuses on the cathode and quantifies the effects of cathode thickness (<span><math><mrow><mi>L</mi></mrow></math></span>), porosity (<span><math><mrow><mi>ε</mi></mrow></math></span>), connectivity (<span><math><mrow><mi>G</mi></mrow></math></span>), average particle size (<span><math><mrow><mi>d</mi></mrow></math></span>) and specific surface area (<span><math><mrow><mi>S</mi><mo>/</mo><mi>V</mi></mrow></math></span>) on DCIR. Combined with machine learning, this work identify that cathode thickness, porosity and average particle size the primary determinants of the DCIR, and the formulas for calculating charging and discharging DCIR are derived, <span><math><mrow><msub><mtext>DCIR</mtext><mtext>Charge</mtext></msub><mo>=</mo><mn>0.168</mn><msup><mrow><mi>L</mi><mi>d</mi></mrow><mn>4</mn></msup><mo>/</mo><msup><mi>ε</mi><mn>2.5</mn></msup></mrow></math></span> and <span><math><mrow><msub><mtext>DCIR</mtext><mtext>Discharge</mtext></msub><mo>=</mo><mn>0.072</mn><msup><mrow><mi>L</mi><mi>d</mi></mrow><mn>3</mn></msup><mo>/</mo><msup><mi>ε</mi><mn>2</mn></msup></mrow></math></span>. This work proposes a research framework for predicting DCIR from the electrode structure, which is applicable to most porous electrode batteries, providing a theoretical basis for calculating the DCIR and is of great significance for electrode design.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"628 ","pages":"Article 235891"},"PeriodicalIF":8.1,"publicationDate":"2024-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723224","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-23DOI: 10.1016/j.jpowsour.2024.235883
Jianglin Tu , Jinwang Li , Zhefei Pan , Xun Zhu , Dingding Ye , Yang Yang , Hong Wang , Liang An , Rong Chen , Qiang Liao
Photoelectrochemical water splitting represents a promising route for converting solar energy into hydrogen, but sluggish reaction kinetics associated with inefficient charge separation and migration, and poor stability limit solar-to-hydrogen conversion. In this work, we develop a N-doped-CdS/TiO2-nanorods heterojunction photoanode for photoelectrochemical water splitting by anchoring CdS on TiO2 nanorods followed by nitrogen doping. The light harvesting is significantly enhanced and the charge separation and migration are promoted due to the formed heterojunction and nitrogen doping, which greatly enhances the water oxidation reaction. As a result, the photoelectrochemical cell with the optimized N-doped-CdS/TiO2-nanorods heterojunction photoanode yields a hydrogen production rate of 42.6 μmol cm−2 h−1, which is 2.51 times higher than that of the TiO2-nanorods photoanode. In particular, doping nitrogen atoms into CdS greatly alleviates the photocorrosion problem. Therefore, the newly-developed photoanode exhibits excellent stability under a continuous 10-h running.
{"title":"Nitrogen-doped CdS/TiO2 nanorods heterojunction photoanode for efficient and stable photoelectrochemical water splitting","authors":"Jianglin Tu , Jinwang Li , Zhefei Pan , Xun Zhu , Dingding Ye , Yang Yang , Hong Wang , Liang An , Rong Chen , Qiang Liao","doi":"10.1016/j.jpowsour.2024.235883","DOIUrl":"10.1016/j.jpowsour.2024.235883","url":null,"abstract":"<div><div>Photoelectrochemical water splitting represents a promising route for converting solar energy into hydrogen, but sluggish reaction kinetics associated with inefficient charge separation and migration, and poor stability limit solar-to-hydrogen conversion. In this work, we develop a N-doped-CdS/TiO<sub>2</sub>-nanorods heterojunction photoanode for photoelectrochemical water splitting by anchoring CdS on TiO<sub>2</sub> nanorods followed by nitrogen doping. The light harvesting is significantly enhanced and the charge separation and migration are promoted due to the formed heterojunction and nitrogen doping, which greatly enhances the water oxidation reaction. As a result, the photoelectrochemical cell with the optimized N-doped-CdS/TiO<sub>2</sub>-nanorods heterojunction photoanode yields a hydrogen production rate of 42.6 μmol cm<sup>−2</sup> h<sup>−1</sup>, which is 2.51 times higher than that of the TiO<sub>2</sub>-nanorods photoanode. In particular, doping nitrogen atoms into CdS greatly alleviates the photocorrosion problem. Therefore, the newly-developed photoanode exhibits excellent stability under a continuous 10-h running.</div></div>","PeriodicalId":377,"journal":{"name":"Journal of Power Sources","volume":"628 ","pages":"Article 235883"},"PeriodicalIF":8.1,"publicationDate":"2024-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723382","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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