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学者姓名：闫鹏飞
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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 ：
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 ：
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 ：
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 ：
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 ：
Solid-state polymer electrolytes (SPEs) have attracted increasing attention due to good interfacial con-tact, light weight, and easy manufacturing. However, the practical application of SPEs such as the most widely studied poly(ethylene oxide) (PEO) in high-energy solid polymer batteries is still challenging, and the reasons are yet elusive. Here, it is found that the mismatch between PEO and 4.2 V-class cathodes is beyond the limited electrochemical window of PEO in the solid LiNi1/3Mn1/3Co1/3O2 (NMC)-PEO batter-ies. The initial oxidation of PEO initiates remarkable surface reconstruction of NMC grains in solid batter-ies that are different from the situation in liquid electrolytes. Well-aligned nanovoids are observed in NMC grains during the diffusion of surface reconstruction layers towards the bulk in solid batteries. The substantial interphasial degradation, therefore, blocks smooth Li' transport across the NMC-PEO interface and causes performance degradation. A thin yet effective LiF-containing protection layer on NMC can effectively stabilize the NMC-PEO interface with a greatly improved lifespan of NMC|PEO|Li bat-teries. This work deepens the understanding of degradations in high-voltage solid-state polymer batteries.(c) 2022 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
Keyword ：
Poly(ethylene oxide) Poly(ethylene oxide) Interphasial degradation Interphasial degradation High-energy solid polymer batteries High-energy solid polymer batteries Surface reconstruction Surface reconstruction
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| GB/T 7714 | Huang, Renzhi , Ding, Yang , Zhang, Fenglin et al. The interphasial degradation of 4.2 V-class poly(ethylene oxide)-based solid batteries beyond electrochemical voltage limit [J]. | JOURNAL OF ENERGY CHEMISTRY , 2022 , 75 : 504-511 . |
| MLA | Huang, Renzhi et al. "The interphasial degradation of 4.2 V-class poly(ethylene oxide)-based solid batteries beyond electrochemical voltage limit" . | JOURNAL OF ENERGY CHEMISTRY 75 (2022) : 504-511 . |
| APA | Huang, Renzhi , Ding, Yang , Zhang, Fenglin , Jiang, Wei , Zhang, Canfu , Yan, Pengfei et al. The interphasial degradation of 4.2 V-class poly(ethylene oxide)-based solid batteries beyond electrochemical voltage limit . | JOURNAL OF ENERGY CHEMISTRY , 2022 , 75 , 504-511 . |
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Abstract ：
Nitriles as efficient electrolyte additives are widely used in high-voltage lithium-ion batteries. However, their working mechanisms are still mysterious, especially in practical high-voltage LiCoO2 pouch lithium-ion batteries. Herein, we adopt a tridentate ligand-containing 1,3,6-hexanetricarbonitrile (HTCN) as an effective electrolyte additive to shed light on the mechanism of stabilizing high-voltage LiCoO2 cathode (4.5 V) through nitrites. The LiCoO2 lgraphite pouch cells with the HTCN additive electrolyte possess superior cycling performance, 90% retention of the initial capacity after 800 cycles at 25 degrees C, and 72% retention after 500 cycles at 45 degrees C, which is feasible for practical application. Such an excellent cycling performance can be attributed to the stable interface: The HTCN molecules with strong electron-donating ability participate in the construction of cathode-electrolyte interphase (CEI) through coordinating with Co ions, which suppresses the decomposition of electrolyte and improves the structural stability of LiCoO2 during cycling. In summary, the work recognizes a coordinating-based interphase-forming mechanism as an effective strategy to optimize the performance of high voltage LiCoO2 cathode with appropriate electrolyte additives for practical pouch batteries.
Keyword ：
high voltage high voltage LiCoO2 LiCoO2 pouch cell pouch cell nitrile additive nitrile additive electrolyte modificationi electrolyte modificationi interface adsorption interface adsorption
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| GB/T 7714 | Tang, Chao , Chen, Yawei , Zhang, Zhengfeng et al. Stable cycling of practical high-voltage LiCoO2 pouch cell via electrolyte modification [J]. | NANO RESEARCH , 2022 , 16 (3) : 3864-3871 . |
| MLA | Tang, Chao et al. "Stable cycling of practical high-voltage LiCoO2 pouch cell via electrolyte modification" . | NANO RESEARCH 16 . 3 (2022) : 3864-3871 . |
| APA | Tang, Chao , Chen, Yawei , Zhang, Zhengfeng , Li, Wenqiang , Jian, Junhua , Jie, Yulin et al. Stable cycling of practical high-voltage LiCoO2 pouch cell via electrolyte modification . | NANO RESEARCH , 2022 , 16 (3) , 3864-3871 . |
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Abstract ：
Dramatic growth of lithium (Li) dendrite andstructural deterioration of LiCoO2(LCO) lead to rapid failureof a high-voltage Li parallel to LCO battery. The nitrile group (-Cxe0c9;N) isbeneficial to maintain the integrity of the LCO lattice due to itsstrong affiliation to Co ions, whereas the-Cxe0c9;N bond isincompatible with the Li metal anode, leading to form adeleterious solid electrolyte interphase (SEI)film. Herein, adual-functional electrolyte additive potassium selenocyanate(KSeCN) is introduced to construct stable and dense SEI/cathode electrolyte interphase (CEI)films by synergistic effectswith-Se and-Cxe0c9;N groups, resulting in uniform Lideposition and a stabilized LCO lattice during cycling. With atrace amount of KSeCN (0.1 wt %) in conventional carbonatedelectrolyte, the Li parallel to LCO battery exhibits promoted cycling performance at high charge cutoff4.6 V. This work provides astrategic guidance for rational design of electrolyte to construct stable SEI and CEIfilms, to achieve a high-energy-densityLi parallel to LCO battery with great performance.
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| GB/T 7714 | Fu, Ang , Lin, Jiande , Zhang, Zhengfeng et al. Synergistical Stabilization of Li Metal Anodesand LiCoO2 Cathodes in High-VoltageLi parallel to LiCoO(2 )Batteries by Potassium Selenocyanate (KSeCN) Additive [J]. | ACS ENERGY LETTERS , 2022 , 7 (4) : 1364-1373 . |
| MLA | Fu, Ang et al. "Synergistical Stabilization of Li Metal Anodesand LiCoO2 Cathodes in High-VoltageLi parallel to LiCoO(2 )Batteries by Potassium Selenocyanate (KSeCN) Additive" . | ACS ENERGY LETTERS 7 . 4 (2022) : 1364-1373 . |
| APA | Fu, Ang , Lin, Jiande , Zhang, Zhengfeng , Xu, Chuanjing , Zou, Yue , Liu, Chengyong et al. Synergistical Stabilization of Li Metal Anodesand LiCoO2 Cathodes in High-VoltageLi parallel to LiCoO(2 )Batteries by Potassium Selenocyanate (KSeCN) Additive . | ACS ENERGY LETTERS , 2022 , 7 (4) , 1364-1373 . |
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Abstract ：
本发明公开了一种均匀包覆金属氧化物到锂电池正极材料表面的方法，其原理是：在高温退火过程中，掺杂元素从正极材料颗粒表面析出富集，形成均匀的包覆层。以TiO2包覆LiCoO2表面为例，其步骤如下：步骤一：将LiOH·H2O、Co3O4、纳米TiO2按照Li、Co、Ti摩尔比1.03‑1.07∶1‑x∶x(其中x取0.001‑0.1)混合后煅烧；步骤二：将步骤一中煅烧完成的物料破碎，得到Ti掺杂的LiCoO2粉末；步骤三：将步骤二中制得的Ti掺杂的LiCoO2粉末在500‑1200℃下煅烧0.1‑100h，之后随炉冷却至室温，获得TiO2均匀包覆的LiCoO2粉末。本发明提出的包覆方法工序简单、成本低廉、易于工业化生产并且所制得的包覆层厚度均一，经该方法所制备的金属氧化物表面包覆的锂电正极材料具有优异的倍率性及循环稳定性。
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| GB/T 7714 | 闫鹏飞 , 李金辉 , 秦昌东 et al. 一种均匀包覆金属氧化物到锂电池正极材料表面的制备方法 : CN202110488162.4[P]. | 2021-05-06 . |
| MLA | 闫鹏飞 et al. "一种均匀包覆金属氧化物到锂电池正极材料表面的制备方法" : CN202110488162.4. | 2021-05-06 . |
| APA | 闫鹏飞 , 李金辉 , 秦昌东 , 张正锋 , 隋曼龄 . 一种均匀包覆金属氧化物到锂电池正极材料表面的制备方法 : CN202110488162.4. | 2021-05-06 . |
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