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学者姓名：闫鹏飞
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Abstract ：
Developing rational regeneration protocol to upgrade spent cathode material for their usage in next generation lithium-ion batteries (LIBs) can alleviate resource stress and benefit environment and carbon neutrality. This work demonstrates that direct regeneration of spent LiCoO2(LCO) encounters the negative effects of Al impurity, which is a common impurity in the spent LIB materials introduced during battery cycling and disassembly process. Our microanalysis show that Al impurity tends to segregate on the LCO surface during the direct regeneration process, which not only causes poor surface regeneration but also degenerates the surface modification effect for upgrading purpose. We therefore propose a one-pot protocol by using a bifunctional solution to realize Al impurity removal and Ti surface coating simultaneously, which successfully upgrade the spent LCO for high voltage and high-power usage. The upgraded LCO cathode can achieve 90 % and 97 % capacity retentions at 0.2C and 2C rates after 2.8-4.5 V 100 cycles, and their initial specific capacity is 180 mAh/g and 149 mAh/g, respectively. The microstructure characterizations in this work provide in-depth understanding of the direct regeneration process, which is essential for understanding and optimizing the recycling process. Further economic analysis show that the established regeneration protocol holds promise for realizing large-scale industrial recycling process of spent LCO.
Keyword ：
Spent LiCoO2 Spent LiCoO2 Upgrading process Upgrading process Surface modification Surface modification Direct regeneration Direct regeneration Al impurity Al impurity
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| GB/T 7714 | Mu, Xulin , Dong, Enhua , Huang, Kai et al. Surface engineering to upgrade spent LiCoO2 by removing Al impurity [J]. | JOURNAL OF POWER SOURCES , 2025 , 638 . |
| MLA | Mu, Xulin et al. "Surface engineering to upgrade spent LiCoO2 by removing Al impurity" . | JOURNAL OF POWER SOURCES 638 (2025) . |
| APA | Mu, Xulin , Dong, Enhua , Huang, Kai , Li, Chao , Liu, Jingzi , Sui, Manling et al. Surface engineering to upgrade spent LiCoO2 by removing Al impurity . | JOURNAL OF POWER SOURCES , 2025 , 638 . |
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Abstract ：
High nickel content worsens the thermal stability of layered cathodes for lithium-ion batteries, raising safety concerns for their applications. Thoroughly understanding the thermal failure process can offer valuable guidance for material optimization on thermal stability and new opportunities in monitoring battery thermal runaway (TR). Herein, this work comprehensively investigates the thermal failure process of a single-crystal nickel-rich layered cathode and finds that the latent thermal failure starts at similar to 120 degrees C far below the TR temperature (225 degrees C). During this stage of heat accumulation, sequential structure transition is revealed by atomic resolution electron microscopy, which follows the layered -> cation mixing layered -> LiMn2O4-type spinel -> disordered spinel -> rock salt. This progression occurs as a result of the continuous migration and densification of transition metal cations. Phase transition generates gaseous oxygen, initially confined within the isolated closed pores, thereby not showing any thermal failure phenomena at the macro-level. Increasing temperature leads to pore growth and coalescence, and eventually to the formation of open pores, causing oxygen gas release and weight loss, which are the typical TR features. We highlight that latent thermal instability occurs before the macro-level TR, suggesting that suppressing phase transitions caused by early thermal instability is a crucial direction for material optimization. Our findings can also be used for early warning of battery thermal runaway.
Keyword ：
Transmission electron microscopy Transmission electron microscopy Nickel-rich layered cathode Nickel-rich layered cathode Lithium -ion battery Lithium -ion battery Phase transition Phase transition Thermal runaway Thermal runaway
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| GB/T 7714 | Han, Xiao , Xu, Ruoyu , Li, Yan et al. Early-stage latent thermal failure of single-crystal Ni-rich layered cathode [J]. | JOURNAL OF ENERGY CHEMISTRY , 2024 , 96 : 578-587 . |
| MLA | Han, Xiao et al. "Early-stage latent thermal failure of single-crystal Ni-rich layered cathode" . | JOURNAL OF ENERGY CHEMISTRY 96 (2024) : 578-587 . |
| APA | Han, Xiao , Xu, Ruoyu , Li, Yan , Ding, Yang , Zhang, Manchen , Wang, Bo et al. Early-stage latent thermal failure of single-crystal Ni-rich layered cathode . | JOURNAL OF ENERGY CHEMISTRY , 2024 , 96 , 578-587 . |
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Abstract ：
The high energy density and low-cost O3-layered NaNi1/3Fe1/3Mn1/3O2 (NFM) is a representative layered cathode for sodium-ion batteries (SIBs). However, its long-term cycling stability needs further improvement and its high voltage usage is highly desired, which is quite challenging. The lack of full understanding of the cycling-induced failures hinders material optimization. Herein, we utilize advanced microanalysis techniques to comprehensively investigate the failure mechanisms of the O3-NFM layered cathode upon low-voltage (2.0-4.0 V) and high-voltage (2.0-4.3 V) cycling. We found that surface degradations play a dominant role during low-voltage cycling, and bulk failures become prominent upon high-voltage cycling. Surface cracking, corrosion, and structure transition together lead to slow charge transfer kinetics, resulting in chronic capacity decay. Bulk degradations such as intragranular cracking, void formation, and interlayer cation mixing severely deteriorate Na storage performance and Na diffusion kinetics, causing rapid capacity decay and voltage fading issues, which are the main challenges of the NFM layered cathode for high voltage usage. High charging cutoff voltage activates the cation migration and condensation, causing a highly disordered layered structure but no phase transition occurs in the bulk. Synergistically stabilizing the surface and bulk structure of the high-voltage O3-layered cathode is essential for achieving superior electrochemical performance. Interfacial degradations dominate the performance decay of O3-layered cathode during low-voltage cycling; high voltage cycling induced bulk failures cause rapid performance decay due to transition metal cation migration.
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| GB/T 7714 | Zhao, Xuejiao , Zhang, Lihan , Wang, Xiaoqi et al. Deciphering cycling voltage-dependent failures of O3-layered cathode for sodium ion battery [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (19) : 11681-11690 . |
| MLA | Zhao, Xuejiao et al. "Deciphering cycling voltage-dependent failures of O3-layered cathode for sodium ion battery" . | JOURNAL OF MATERIALS CHEMISTRY A 12 . 19 (2024) : 11681-11690 . |
| APA | Zhao, Xuejiao , Zhang, Lihan , Wang, Xiaoqi , Li, Jinhui , Zhang, Lin , Liu, Di et al. Deciphering cycling voltage-dependent failures of O3-layered cathode for sodium ion battery . | JOURNAL OF MATERIALS CHEMISTRY A , 2024 , 12 (19) , 11681-11690 . |
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Abstract ：
本发明涉及一种钠离子电池层状正极材料的制备方法，属于钠离子电池技术领域。本发明将Na2CO3、NiO、Mn2O3、掺杂金属氧化物混合均匀得到混合粉A，混合粉A加入到易挥发溶剂中搅拌混合得到浆料A，浆料A烘干去除易挥发溶剂后压片，再置于温度500～1200℃烧结5～30h，随炉冷却至温度为不高于150℃得到正极材料粉末；将正极材料粉末、PVDF、乙炔黑混合均匀得到混合粉B，混合粉B中加入N‑甲基吡咯烷酮进行调浆得到浆料B，然后将浆料B涂覆在铝箔上，真空干燥得到极片；以极片为正极，金属钠或软碳为负极，NaClO4电解液为电池电解液，组装成钠离子电池并循环1～50圈，拆出电极得到循环后的极片，循环后的极片经热处理得到钠离子电池层状正极。该电极具有优异的循环稳定性。
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| GB/T 7714 | 程苏兰 , 李金辉 , 隋曼龄 et al. 一种钠离子电池层状正极材料的制备方法 : CN202310443754.3[P]. | 2023-04-24 . |
| MLA | 程苏兰 et al. "一种钠离子电池层状正极材料的制备方法" : CN202310443754.3. | 2023-04-24 . |
| APA | 程苏兰 , 李金辉 , 隋曼龄 , 闫鹏飞 . 一种钠离子电池层状正极材料的制备方法 : CN202310443754.3. | 2023-04-24 . |
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Abstract ：
Single-crystal LiNixCoyMnzO2 (SC-NCM, x+y+z=1) cathodes are renowned for their high structural stability and reduced accumulation of adverse side products during long-term cycling. While advances have been made using SC-NCM cathode materials, careful studies of cathode degradation mechanisms are scarce. Herein, we employed quasi single-crystalline LiNi0.65Co0.15Mn0.20O2 (SC-NCM65) to test the relationship between cycling performance and material degradation for different charge cutoff potentials. The Li/SC-NCM65 cells showed >77 % capacity retention below 4.6 V vs. Li+/Li after 400 cycles and revealed a significant decay to 56 % for 4.7 V cutoff. We demonstrate that the SC-NCM65 degradation is due to accumulation of rock-salt (NiO) species at the particle surface rather than intragranular cracking or side reactions with the electrolyte. The NiO-type layer formation is also responsible for the strongly increased impedance and transition-metal dissolution. Notably, the capacity loss is found to have a linear relationship with the thickness of the rock-salt surface layer. Density functional theory and COMSOL Multiphysics modeling analysis further indicate that the charge-transfer kinetics is decisive, as the lower lithium diffusivity of the NiO phase hinders charge transport from the surface to the bulk.
Keyword ：
Multiphysics Analysis Multiphysics Analysis Structural Stability Structural Stability Single-Crystal Cathodes Single-Crystal Cathodes Transfer Kinetics Transfer Kinetics Rock-Salt Formation Rock-Salt Formation
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| GB/T 7714 | Zhao, Wengao , Wang, Kuan , Fan, Xinming et al. Quantifying Degradation Parameters of Single-Crystalline Ni-Rich Cathodes in Lithium-Ion Batteries [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (32) . |
| MLA | Zhao, Wengao et al. "Quantifying Degradation Parameters of Single-Crystalline Ni-Rich Cathodes in Lithium-Ion Batteries" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62 . 32 (2023) . |
| APA | Zhao, Wengao , Wang, Kuan , Fan, Xinming , Ren, Fucheng , Xu, Xieyu , Liu, Yangyang et al. Quantifying Degradation Parameters of Single-Crystalline Ni-Rich Cathodes in Lithium-Ion Batteries . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (32) . |
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Abstract ：
Layered transition-metal oxides are promising cathode candidates for sodium-ion batteries. However, the inferior interphase formation and particulate fracture during sodiation/desodiation result in structure degradation and poor stability. Herein, the interface chemistry of P2-Na0.640Ni0.343Mn0.657O2 in an electrolyte of 1.0 mol/L NaPF6 in diglyme is unveiled to enable highly reversible Na extraction and intercalation. The uniform and robust cathode-electrolyte interphase layer is in situ formed with decomposition of diglyme molecules and anions in initial cycles. The NaF- and CO-rich CEI film exhibits high mechanical strength and ionic conductivity, which suppresses the reconstruction of its electrode interphase from P2 phase to spinel-like structure and reinforces its structure integrity without cracks. This favours facile Na+ transport and stable bulk redox reactions. It is demonstrated to show long cycling stability with capacity retention of 94.4% for 180 cycles and superior rate capability. This investigation highlights the cathode interphase chemistry in sodium-ion batteries.
Keyword ：
Sodium-ion batteries Sodium-ion batteries Ether electrolyte Ether electrolyte Reversibility Reversibility Surface Chemistry Surface Chemistry Cathodes Cathodes Layered oxides Layered oxides
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| GB/T 7714 | Wang, Chenchen , Wang, Kuan , Ren, Meng et al. Interfacial Chemistry Enables Highly Reversible Na Extraction/Intercalation in Layered-Oxide Cathode Materials [J]. | CHINESE JOURNAL OF CHEMISTRY , 2023 . |
| MLA | Wang, Chenchen et al. "Interfacial Chemistry Enables Highly Reversible Na Extraction/Intercalation in Layered-Oxide Cathode Materials" . | CHINESE JOURNAL OF CHEMISTRY (2023) . |
| APA | Wang, Chenchen , Wang, Kuan , Ren, Meng , Huang, Yaohui , Zhang, Kai , Liao, Changzhong et al. Interfacial Chemistry Enables Highly Reversible Na Extraction/Intercalation in Layered-Oxide Cathode Materials . | CHINESE JOURNAL OF CHEMISTRY , 2023 . |
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Abstract ：
Twin boundaries (TBs) as a common defect in layered cathodes play multiple roles in affecting materials' performance, which requires a deep understanding and an effective regulation method to realize rational design of superior layered cathodes. Herein, by virtue of advanced electron microscopy, we demonstrate that TBs can be quantitatively estimated and characterized, and we further validate that TBs can initiate massive cracks upon electrochemical cycling, which aggravates the performance decay of LiNiO2. Adjusting the synthesis conditions cannot avoid TB formation for the solid-state method, but fortunately, we find that a coprecipitation method can effectively eliminate TBs; thus, the improved cycling stability of LiNiO2 is achieved. We further validate that TB-free LiCoO2 can also be synthesized by the coprecipitation method, which demonstrates improved cycling stability.
Keyword ：
lithium-ion battery lithium-ion battery cracking cracking LiNiO2 LiNiO2 twin boundary twin boundary layered cathode layered cathode
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| GB/T 7714 | Mu, Xulin , Hui, Xiaojuan , Wang, Mingming et al. Mitigating Twin Boundary-Induced Cracking for Enhanced Cycling Stability of Layered Cathodes [J]. | ACS APPLIED ENERGY MATERIALS , 2023 , 6 (9) . |
| MLA | Mu, Xulin et al. "Mitigating Twin Boundary-Induced Cracking for Enhanced Cycling Stability of Layered Cathodes" . | ACS APPLIED ENERGY MATERIALS 6 . 9 (2023) . |
| APA | Mu, Xulin , Hui, Xiaojuan , Wang, Mingming , Wang, Kuan , Li, Yan , Zhang, Yuefei et al. Mitigating Twin Boundary-Induced Cracking for Enhanced Cycling Stability of Layered Cathodes . | ACS APPLIED ENERGY MATERIALS , 2023 , 6 (9) . |
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Abstract ：
There remain significant challenges in developing fast-charging materials for lithium-ion batteries (LIBs) due to sluggish ion diffusion kinetics and unfavorable electrolyte mass transportation in battery electrodes. In this work, a mesoporous single-crystalline lithium titanate (MSC-LTO) microrod that can realize exceptional fast charge/discharge performance and excellent long-term stability in LIBs is reported. The MSC-LTO microrods are featured with a single-crystalline structure and interconnected pores inside the entire single-crystalline body. These features not only shorten the lithium-ion diffusion distance but also allow for the penetration of electrolytes into the single-crystalline interior during battery cycling. Hence, the MSC-LTO microrods exhibit unprecedentedly high rate capability, achieving a specific discharge capacity of approximate to 174 mAh g(-1) at 10 C, which is very close to its theoretical capacity, and approximate to 169 mAh g(-1) at 50 C. More importantly, the porous single-crystalline microrods greatly mitigate the structure degradation during a long-term cycling test, offering approximate to 92% of the initial capacity after 10 000 cycles at 20 C. This work presents a novel strategy to engineer porous single-crystalline materials and paves a new venue for developing fast-charging materials for LIBs.
Keyword ：
ion transportation pathway ion transportation pathway fast-charging electrode fast-charging electrode mesoporous single-crystalline structure mesoporous single-crystalline structure lithium titanate lithium titanate lithium-ion batteries lithium-ion batteries
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| GB/T 7714 | Jin, Xu , Han, Yehu , Zhang, Zhengfeng et al. Mesoporous Single-Crystal Lithium Titanate Enabling Fast-Charging Li-Ion Batteries [J]. | ADVANCED MATERIALS , 2022 , 34 (18) . |
| MLA | Jin, Xu et al. "Mesoporous Single-Crystal Lithium Titanate Enabling Fast-Charging Li-Ion Batteries" . | ADVANCED MATERIALS 34 . 18 (2022) . |
| APA | Jin, Xu , Han, Yehu , Zhang, Zhengfeng , Chen, Yawei , Li, Jianming , Yang, Tingting et al. Mesoporous Single-Crystal Lithium Titanate Enabling Fast-Charging Li-Ion Batteries . | ADVANCED MATERIALS , 2022 , 34 (18) . |
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Abstract ：
本发明涉及一种废旧锂电池正极材料剥离并直接再生的方法，属于锂电池正极技术领域。本发明机械拆解废旧锂电池正极得到含Al集流体的正极极片，在含Al集流体的正极极片表面喷涂锂盐溶液形成锂盐薄膜，烘干得到补锂正极极片；在空气氛围下，补锂正极极片进行低温焙烧，敲打物理分离得到废旧LiCoO2正极材料，废旧LiCoO2正极材料研磨过筛得到粉末A；将粉末A加入到NaOH溶液中碱浸除铝得到粉末B；将过量锂盐加入到粉末B中混合均匀，在空气氛围中高温烧结得到再生锂电池正极材料。相比较传统正极材料剥离的方式，低温补锂法高效的将正极材料与铝箔分离，所再生的LiCoO2正极材料满足工业化应用。
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| GB/T 7714 | 闫鹏飞 , 隋曼龄 , 牟许霖 et al. 一种废旧锂电池正极材料剥离并直接再生的方法 : CN202211601633.9[P]. | 2022-12-13 . |
| MLA | 闫鹏飞 et al. "一种废旧锂电池正极材料剥离并直接再生的方法" : CN202211601633.9. | 2022-12-13 . |
| APA | 闫鹏飞 , 隋曼龄 , 牟许霖 , 董恩华 , 黄开 . 一种废旧锂电池正极材料剥离并直接再生的方法 : CN202211601633.9. | 2022-12-13 . |
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Abstract ：
本发明公开了一种Al掺杂的富镍正极单晶材料的制备方法，该方法通过控制多次不同球磨处理方式，解决了直接球磨方式中因为原料带结晶水而混合不均一的问题，通过控制连续多次煅烧方式，调控锂含量参数和煅烧时间，最终可以制备出层状结构良好，结晶度高且具有优异电化学性能的Al掺杂的富镍正极单晶材料。通过Al掺杂，不仅可以显著减少富镍正极单晶颗粒的开裂，有效抑制富镍材料在电化学循环过程中的结构退化，而且也能明显减少表面相变程度，在表界面方面同样起着积极的作用。该方法操作简单，成本低廉，适合大规模工业化生产性能优异的Al掺杂正极材料。
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| GB/T 7714 | 闫鹏飞 , 惠小娟 , 夏月明 et al. 一种Al掺杂的富镍正极单晶材料的制备方法 : CN202210511210.1[P]. | 2022-05-11 . |
| MLA | 闫鹏飞 et al. "一种Al掺杂的富镍正极单晶材料的制备方法" : CN202210511210.1. | 2022-05-11 . |
| APA | 闫鹏飞 , 惠小娟 , 夏月明 , 牟许霖 . 一种Al掺杂的富镍正极单晶材料的制备方法 : CN202210511210.1. | 2022-05-11 . |
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