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Elevating operation voltage of LiTFSI-electrolyte via a universal passivation strategy for high-voltage lithium-metal batteries 采用通用钝化策略提高高压锂金属电池的工作电压
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-02 DOI: 10.1016/j.ensm.2025.104588
Rongrong Guo , Xiaoyun Xu , Songmei Li , Yangyang Cheng , Junwei An , Mei Yu , Jinyan Zhong , Juan Du , Shubin Yang , Bin Li
{"title":"Elevating operation voltage of LiTFSI-electrolyte via a universal passivation strategy for high-voltage lithium-metal batteries","authors":"Rongrong Guo ,&nbsp;Xiaoyun Xu ,&nbsp;Songmei Li ,&nbsp;Yangyang Cheng ,&nbsp;Junwei An ,&nbsp;Mei Yu ,&nbsp;Jinyan Zhong ,&nbsp;Juan Du ,&nbsp;Shubin Yang ,&nbsp;Bin Li","doi":"10.1016/j.ensm.2025.104588","DOIUrl":"10.1016/j.ensm.2025.104588","url":null,"abstract":"<div><div>Lithium bis((trifluoromethyl)sulfonyl)azanide (LiTFSI) based electrolytes have become the preferred electrolytes for lithium metal batteries (LMBs) due to their exceptional anode stability and ionic conductivity. However, challenges including unstable cathode electrolyte interface (CEI) formation and aluminum current collector (AlCC) corrosion have hindered the application of LiTFSI-based electrolyte in high-voltage LMBs. In this work, a universal passivation strategy is proposed and achieved with additive 8-hydroxyquinoline (8-HQ) in LiTFSI based electrolyte (ED-HQ). The 8-HQ additive preferentially decomposes on the cathode surface to generate Li<sub>3</sub>N, inducing the formation of inorganic-rich CEI with a uniform thickness of only 10 nm. The dense and homogeneous inorganic-rich CEI enables the cycling stability of the cathode. Meanwhile, the 8-HQ additive shows strong adsorption on the AlCC surface, which promotes the formation of a composite passivation layer consisting of an Aluminum-8-hydroxyquinoline (Alq<sub>3</sub>) chelate layer and an AlF<sub>3</sub>/LiF inorganic layer, increasing the stable operating voltage of AlCC to 4.9 V and reducing the corrosion current density to one tenth. As a result, the joint effects enable Li||LiFePO<sub>4</sub> cells with ED-HQ electrolyte to achieve 89.8% capacity retention after 500 cycles at an elevated cutoff voltage of 4.5 V, demonstrating a viable pathway toward stable high-voltage LMB operation.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104588"},"PeriodicalIF":20.2,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144931203","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
Embedded sensing: The neural frontier and early-warning revolution in battery safety monitoring 嵌入式传感:电池安全监测中的神经前沿和预警革命
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-01 DOI: 10.1016/j.ensm.2025.104582
Sheng Guo , Hao Luo , Zhe Gao , Yizheng Ding , Shiwen Wang , Pengcheng Wang , Feihong Wang , Jizhong Cao , Yajie Song , Ning Ren , Mi Lu
{"title":"Embedded sensing: The neural frontier and early-warning revolution in battery safety monitoring","authors":"Sheng Guo ,&nbsp;Hao Luo ,&nbsp;Zhe Gao ,&nbsp;Yizheng Ding ,&nbsp;Shiwen Wang ,&nbsp;Pengcheng Wang ,&nbsp;Feihong Wang ,&nbsp;Jizhong Cao ,&nbsp;Yajie Song ,&nbsp;Ning Ren ,&nbsp;Mi Lu","doi":"10.1016/j.ensm.2025.104582","DOIUrl":"10.1016/j.ensm.2025.104582","url":null,"abstract":"<div><div>The rapid proliferation of battery systems has positioned thermal runaway prevention as a crucial technological imperative. In-situ sensor-based monitoring frameworks enable real-time tracking of internal parameters, thereby providing early warnings and interventions for thermal management. However, conventional sensors, limited by their unidimensional architectures, struggle to accurately capture the intricate interplay among thermal, mechanical, and chemical fields. This limitation results in significant blind spots when predicting battery degradation under multiphysics conditions over the entire lifecycle. Consequently, advancing multi-parameter sensing technologies and developing multidimensional sensing architectures become essential for achieving comprehensive battery safety monitoring. From an embedded sensing perspective, this review systematically examines critical challenges related to chemical compatibility, measurement accuracy, and multi-parameter monitoring encountered during sensor integration. It provides a detailed elaboration on the operating principles and practical applications of thermocouples, optical fiber sensors, and thin-film sensors in batteries. To address technological bottlenecks, such as risks to structural integrity, electrolyte-induced performance degradation, and limitations in single-parameter monitoring, we propose strategies that include sensor miniaturization, the selection of chemically robust materials, integrated multidimensional in-situ platforms, and the incorporation of artificial intelligence (AI) technologies. This review advances comprehensive understanding of battery multidimensional sensing systems, significantly enhancing active safety engineering and multiphysics diagnostic frameworks.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104582"},"PeriodicalIF":20.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144924302","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
Deciphering the capacitive behavior of heteroatom–doped carbon materials with small mesopores 小介孔杂原子掺杂碳材料的电容性分析
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-01 DOI: 10.1016/j.ensm.2025.104584
Xiang Cai , Kuixuan Zhang , Wangxu Chen, Xinqi Hu
{"title":"Deciphering the capacitive behavior of heteroatom–doped carbon materials with small mesopores","authors":"Xiang Cai ,&nbsp;Kuixuan Zhang ,&nbsp;Wangxu Chen,&nbsp;Xinqi Hu","doi":"10.1016/j.ensm.2025.104584","DOIUrl":"10.1016/j.ensm.2025.104584","url":null,"abstract":"<div><div>The charge storage processes of heteroatom–doped carbon materials with small mesopores (2 ∼ 4 nm) occur by both double–layer capacitance and pseudocapacitance. Yet, owing to the ambiguous understanding on how electrolyte ions affect their capacitive behavior, it is hard to form a unified design principle to guide the selection of electrolytes, with the purpose of boosting supercapacitors. Herein, an all–in–one carbon electrode with abundant oxygen–containing groups and an average pore size of 2.5 nm was used as a model electrode to investigate the capacitive behavior of this class of carbon materials. It is found that in ammonium acetate aqueous electrolyte the model electrode shows a significantly increased specific capacitance, and an ion exchange mechanism dominates charge storage. Acetate anions with a larger ion radius can better match small mesopores in size and thus increase double–layer capacitance due to the suppression of the “over–screening” effect in the first adsorbed layer on carbon surfaces. Besides, ammonium cations forms hydrogen bonds with oxygen–containing groups maximizing the Gibbs free energy change related to faradic reactions, which enhances pseudocapacitance. Our work elaborated the effect of electrolyte ions on the capacitance of heteroatom–doped carbon materials with small mesopores and provided new understanding on designing high–performance aqueous supercapacitors.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104584"},"PeriodicalIF":20.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144924339","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
Ultrathin lithium metal anodes for high-efficiency lithium batteries: synergizing surface LiF and Lithiophilic alloying 高效锂电池用超薄锂金属阳极:表面LiF和亲锂合金化的协同作用
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-01 DOI: 10.1016/j.ensm.2025.104579
Bo Yu , Luo Fei , Mengfei Li , Zhiyuan Ma , Bingshu Guo , Junchen Chen , Xingyang Wang , Zhiyu Xue , Liujiang Zhou , John Wang
{"title":"Ultrathin lithium metal anodes for high-efficiency lithium batteries: synergizing surface LiF and Lithiophilic alloying","authors":"Bo Yu ,&nbsp;Luo Fei ,&nbsp;Mengfei Li ,&nbsp;Zhiyuan Ma ,&nbsp;Bingshu Guo ,&nbsp;Junchen Chen ,&nbsp;Xingyang Wang ,&nbsp;Zhiyu Xue ,&nbsp;Liujiang Zhou ,&nbsp;John Wang","doi":"10.1016/j.ensm.2025.104579","DOIUrl":"10.1016/j.ensm.2025.104579","url":null,"abstract":"<div><div>Lithium metal batteries are considered one of the most promising candidates for next-generation energy storage systems. However, challenges such as dendrite formation, unstable cycling, and low lithium utilization have severely hindered their practical implementation. Herein, we propose a universal and scalable strategy for fabricating ultrathin lithium anodes by integrating lithiophilic alloys and metal fluoride coatings onto current collectors through a simple SnF<sub>2</sub>-based gas-phase reaction. A roll-to-roll system enables scalable production on various metal substrates, as demonstrated by Ni mesh coated with Ni<sub>3</sub>Sn<sub>2</sub> and NiF<sub>2</sub>. Electrochemical lithium deposition and molten infusion induce in situ Li-Sn alloy formation and LiF surface migration, which synergistically enable uniform plating, interface stabilization, and high lithium utilization. The resulting anodes deliver tunable areal capacities of 3–10 mAh cm<sup>−2</sup>, effectively overcoming the fabrication limitations of lithium foils thinner than 50 μm and significantly reducing lithium consumption. Specifically, ultrathin lithium anodes with a capacity of 3.4 mAh cm<sup>−2</sup> exhibit stable cycling over 2200 h in symmetric cells. Full cells with LiFePO<sub>4</sub> cathodes deliver an average Coulombic efficiency of 99.8 % over 200 cycles at 0.5 C.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104579"},"PeriodicalIF":20.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144928508","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
Engineering the future of silicon-based all-solid-state lithium-ion batteries: Current barriers and innovative solutions 设计硅基全固态锂离子电池的未来:当前的障碍和创新的解决方案
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-01 DOI: 10.1016/j.ensm.2025.104583
Haizhou Zhao , Sizhe Wang , Sihang Xia , Fei Liang , Yancheng Yang , Ji Qian , Haojie Song , Chao Yang , Renjie Chen
{"title":"Engineering the future of silicon-based all-solid-state lithium-ion batteries: Current barriers and innovative solutions","authors":"Haizhou Zhao ,&nbsp;Sizhe Wang ,&nbsp;Sihang Xia ,&nbsp;Fei Liang ,&nbsp;Yancheng Yang ,&nbsp;Ji Qian ,&nbsp;Haojie Song ,&nbsp;Chao Yang ,&nbsp;Renjie Chen","doi":"10.1016/j.ensm.2025.104583","DOIUrl":"10.1016/j.ensm.2025.104583","url":null,"abstract":"<div><div>As a leading contender for advanced energy storage systems, silicon-based all-solid-state lithium-ion batteries (Si-ASSLIBs) have garnered critical research frontier due to their demonstrated capacity to offer enhanced energy density and superior thermal stability and safety compared to conventional lithium-ion batteries. However, Si-ASSLIBs still faces challenges in practical applications, such as cell failure due to the significant volume expansion of silicon. Innovatively, we highlight that pressure plays two critical roles in Si-ASSLIBs. Herein, we systematically review the recent advances and challenges in Si-ASSLIBs, with a particular emphasis on their industrialization pathways. The research progress of Si-ASSLIBs is comprehensively summarized, and different silicon anodes and their electrochemical performance optimization strategies are presented. Next, we systematically summarize the mechanical properties, simulation, and morphological/structural characterization approaches pertaining to volume expansion in Si-ASSLIBs. Crucially, we propose that fabrication pressure pre-stabilizes electrode interfaces, while operational pressure dynamically regulates stress evolution. In order to promote the scaled-up industrial production of Si-ASSLIBs, we summarize the current state of research on the pre-lithiation process and present our views for industrialization. As a core enabler, pre-lithiation technology is rigorously evaluated via scalable production pathways, establishing design standards and an industrial roadmap. Finally, the challenges and opportunities for achieving high energy density Si-ASSLIBs and future developments are outlined. This review outlooks the challenges, opportunities, and future directions for advanced Si-ASSLIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104583"},"PeriodicalIF":20.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144924340","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
Precise Ni/Co separation from spent Li-Ion batteries: Revealing the pivotal role of H2O in deep eutectic solvents 从废锂离子电池中精确分离Ni/Co:揭示H2O在深共晶溶剂中的关键作用
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-01 DOI: 10.1016/j.ensm.2025.104585
Xingyu Hu , Hui Shi , Yilei Zheng , Penghui Shao , Liming Yang , Xubiao Luo
{"title":"Precise Ni/Co separation from spent Li-Ion batteries: Revealing the pivotal role of H2O in deep eutectic solvents","authors":"Xingyu Hu ,&nbsp;Hui Shi ,&nbsp;Yilei Zheng ,&nbsp;Penghui Shao ,&nbsp;Liming Yang ,&nbsp;Xubiao Luo","doi":"10.1016/j.ensm.2025.104585","DOIUrl":"10.1016/j.ensm.2025.104585","url":null,"abstract":"<div><div>The sustainable recovery of valuable metals from end-of-life lithium-ion batteries (LIBs) has become essential for relieving the supply-demand contradiction of key resources. However, the high similarity in physicochemical properties of transition metals poses a fundamental challenge for the selective recycling. Here we proposed a facile strategy for defining the demarcation line of precipitation/dissolution behavior for precise Ni/Co separation. A malonic acid-based deep eutectic solvent (DES) is developed, emphasizing the H<sub>2</sub>O-mediated competitive coordination and differentiated solubility. We discovered the distinctive formation of [Ni(H<sub>2</sub>O)<sub>6</sub>]<sup>2+</sup> and [CoCl<sub>4</sub>]<sup>2-</sup> in the DES-20 % H<sub>2</sub>O system. Furthermore, the <em>K</em><sub>sp</sub> differences of the Ni-complex and Co-complex in the C<sub>3</sub>H<sub>2</sub>O<sub>4</sub><sup>2-</sup>-rich environment was effectively magnified. These significant differences synergistically enable the generation of C<sub>3</sub>H<sub>2</sub>NiO<sub>4</sub>·2H<sub>2</sub>O precipitation (∼ 99.9 % purity), achieving a remarkable Ni/Co separation factor of 125, which guarantees sequential separation of all metals. This universal methodology along with in-depth mechanism understanding provides a guideline toward value-added recovery of LIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104585"},"PeriodicalIF":20.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144928631","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
Hydrogen bond engineering in aqueous electrolytes: Strategies for cryogenic battery applications 水溶液氢键工程:低温电池应用策略
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-08-31 DOI: 10.1016/j.ensm.2025.104576
Shuhua Yang , Shang Wang , Yiqun Du , Jinfeng Sun , Degang Zhao , Bingqiang Cao
{"title":"Hydrogen bond engineering in aqueous electrolytes: Strategies for cryogenic battery applications","authors":"Shuhua Yang ,&nbsp;Shang Wang ,&nbsp;Yiqun Du ,&nbsp;Jinfeng Sun ,&nbsp;Degang Zhao ,&nbsp;Bingqiang Cao","doi":"10.1016/j.ensm.2025.104576","DOIUrl":"10.1016/j.ensm.2025.104576","url":null,"abstract":"<div><div>Zinc-based and lithium-based battery systems have been extensively utilized in modern electronic devices and automotive applications owing to their exceptional energy density-to-volume ratios. Nevertheless, these energy storage systems employing aqueous electrolytes face critical operational limitations under subzero conditions, where electrolyte crystallization induces severe ionic conductivity degradation and eventual functional failure. Current research efforts exhibit a notable gap in comprehensive mechanistic analyses addressing cryogenic performance deterioration from the perspective of hydrogen bond network disruption. This work presents a systematic review of the fundamental correlation between hydrogen bonding dynamics and phase transition behavior in aqueous media, and the consequent impacts on ion transport mechanisms. The established structure-property relationships offer valuable insights for developing advanced low-temperature aqueous electrolytes through targeted molecular engineering of hydrogen-bond interactions.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104576"},"PeriodicalIF":20.2,"publicationDate":"2025-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144920909","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
Molecular reconfiguration of pitch-derived hard carbon anodes with balanced thermodynamic stability and rapid sodium storage kinetics for high-performance sodium-ion batteries 具有平衡热力学稳定性和高性能钠离子电池快速储钠动力学的沥青衍生硬碳阳极的分子重构
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-08-31 DOI: 10.1016/j.ensm.2025.104580
Chuangchuang Li , Qinghang Chen , Yinghao Zhang , Pandeng Zhao , Xiangxi He , Qinfen Gu , Jiazhao Wang , Shu-Lei Chou , Xingqiao Wu
{"title":"Molecular reconfiguration of pitch-derived hard carbon anodes with balanced thermodynamic stability and rapid sodium storage kinetics for high-performance sodium-ion batteries","authors":"Chuangchuang Li ,&nbsp;Qinghang Chen ,&nbsp;Yinghao Zhang ,&nbsp;Pandeng Zhao ,&nbsp;Xiangxi He ,&nbsp;Qinfen Gu ,&nbsp;Jiazhao Wang ,&nbsp;Shu-Lei Chou ,&nbsp;Xingqiao Wu","doi":"10.1016/j.ensm.2025.104580","DOIUrl":"10.1016/j.ensm.2025.104580","url":null,"abstract":"<div><div>Pre-oxidation, a key modification method to enhance the sodium storage properties of pitch-based amorphous carbon through molecular reconfiguration, results in suboptimal sodium storage kinetics within the extended plateau region. Therefore, it is of great significance to clarify the effects of pre-oxidation and carbonization on the pitch-derived carbon microstructure and electrochemical behavior. In this work, the pitch precursors with different pre-oxidation degrees were carbonized to unveil the crucial effects of molecular reconfiguration and carbonization temperature on the microstructural evolution by various characterization methods. In situ Raman and electrochemical analyses reveal that defects govern Na<sup>+</sup> diffusion kinetics, while interlayer spacing/pore structures dictate storage thermodynamics. Consequently, PHC-A-1100 synthesized via 300 ℃ pre-oxidation followed by 1100 ℃ carbonization achieves synergistic regulation of Na<sup>+</sup>-storage kinetics and thermodynamics through controlled molecular reconfiguration-carbonization coupling, enabling Ah-level capacity in 18650 cylindrical cells with 80.04 % capacity retention after 200 cycles at 1 C. Moreover, this study provides a comprehensive insight into optimizing sodium storage behavior for constructing high-performance carbon anodes of sodium-ion batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104580"},"PeriodicalIF":20.2,"publicationDate":"2025-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144924341","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
Electronic structure regulated by precursor gradient design assists inhibition of nanopores for stable Ni-rich cathodes 由前驱体梯度设计调节的电子结构有助于抑制稳定富镍阴极的纳米孔
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-08-31 DOI: 10.1016/j.ensm.2025.104578
Yuting Deng , Lang Qiu , Yi Wang , Jun Zhang , Mengke Zhang , Shuli Zheng , Qiyu Zhang , Benhe Zhong , Yao Xiao , Xiaodong Guo
{"title":"Electronic structure regulated by precursor gradient design assists inhibition of nanopores for stable Ni-rich cathodes","authors":"Yuting Deng ,&nbsp;Lang Qiu ,&nbsp;Yi Wang ,&nbsp;Jun Zhang ,&nbsp;Mengke Zhang ,&nbsp;Shuli Zheng ,&nbsp;Qiyu Zhang ,&nbsp;Benhe Zhong ,&nbsp;Yao Xiao ,&nbsp;Xiaodong Guo","doi":"10.1016/j.ensm.2025.104578","DOIUrl":"10.1016/j.ensm.2025.104578","url":null,"abstract":"<div><div>The mechanical integrity of particles plays a key role in the electrochemical performance of Ni-rich cathodes. However, nanopore defects, caused by the non-synchronized thermodynamics and kinetics during the sintering process, destroy the structural integrity. Herein, we report an approach to regulating the electronic structure of the precursor to promote the synchronization of lithiation and decomposition processes during sintering. The findings based on structural characterizations and density functional theory calculations demonstrate that constructing more Ni-O-Mn configurations on the precursor surface <em>via</em> element gradient design can accelerate charge transfer kinetics and reduce Li⁺ insertion energy barrier, ultimately enhancing lithiation kinetics and suppressing nanopore formation. This work presents a new strategy for preserving the mechanical integrity of particles during the high-temperature lithiation of Ni-rich precursors.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104578"},"PeriodicalIF":20.2,"publicationDate":"2025-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144920910","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
Decoding electrochemo-mechanical degradation in solid-state batteries: A phase-field study toward robust cathode design 解码固态电池的电化学-机械退化:稳健阴极设计的相场研究
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-08-30 DOI: 10.1016/j.ensm.2025.104577
Chunhao Yuan , Jing Wu , Wenjing Zhang , Jun Xu
{"title":"Decoding electrochemo-mechanical degradation in solid-state batteries: A phase-field study toward robust cathode design","authors":"Chunhao Yuan ,&nbsp;Jing Wu ,&nbsp;Wenjing Zhang ,&nbsp;Jun Xu","doi":"10.1016/j.ensm.2025.104577","DOIUrl":"10.1016/j.ensm.2025.104577","url":null,"abstract":"<div><div>The commercialization of all-solid-state batteries (ASSBs) is hindered by complex electro-chemo-mechanical degradation processes in composite cathodes, particularly particle fracture and solid electrolyte (SE)–particle interfacial debonding. To uncover the underlying mechanisms, we develop a fully coupled three-dimensional electro-chemo-mechanical phase-field model incorporating electrochemical reaction kinetics, mechanical deformation, interfacial decohesion, particle fracture, and realistic polycrystalline microstructures. Simulations reveal that interfacial debonding stems from mismatched contraction between particles and the SE during delithiation, while anisotropic volume changes within primary crystallites induce localized GPa-level stresses, initiating cracks at particle junctions and impacting over 18 % of the secondary particle volume. Although softer SEs delay damage onset, they cannot prevent fracture or debonding. Strengthening the particle–SE interface reduces interfacial separation but accelerates internal fracture. In contrast, enhancing active material fracture toughness effectively suppresses crack initiation. Based on these insights, we propose a cathode design strategy combining microstructural homogenization, strong interfacial bonding, compliant SEs (e.g., sulfides), and improved fracture toughness. This work provides a critical mechanistic understanding of degradation pathways in ASSB cathodes and offers actionable guidelines for the design of durable, high-performance solid-state batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104577"},"PeriodicalIF":20.2,"publicationDate":"2025-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144920911","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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