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学者姓名：尉海军
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Abstract ：
The practical applications of high-energy Li-rich layered oxides (LLOs) have been hindered by the severe performance degradation including voltage decay and capacity fading. The gradient construction toward high-activity interior and high-stability exterior, typically realized by gradually changed transition metal (TM) gradient in LLOs, can alleviate the performance degradation to certain degrees. In this study, a gradient design of Al/Mg dopants is demonstrated for the TM-gradient LLOs to further harmonize the high-activity interior and high-stability exterior, thereby forming the dual (TM and doping) gradient. As a result, superior capacity retention of 86% and a minor voltage decay of 0.54 mV cycle(-1) are achieved at 1 C after 300 cycles. The improved electrochemical stability of the dual-gradient LLO is attributed to the enhanced surface stability and suppressed bulk structure degeneration of LLOs upon electrochemical cycling. The dual-gradient design serves as an important approach to fabricate high-performance bulk LLOs toward applications.
Keyword ：
gradient Al/Mg co-doping gradient Al/Mg co-doping voltage decay voltage decay dual-gradient construction dual-gradient construction Li-ion batteries Li-ion batteries Li-rich layered oxides Li-rich layered oxides
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| GB/T 7714 | Wu, Tianhao , Zhang, Xu , Liu, Shiqi et al. Dual-Gradient Construction on Li-Rich Cathodes for High Stability Lithium Battery [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
| MLA | Wu, Tianhao et al. "Dual-Gradient Construction on Li-Rich Cathodes for High Stability Lithium Battery" . | ADVANCED FUNCTIONAL MATERIALS (2025) . |
| APA | Wu, Tianhao , Zhang, Xu , Liu, Shiqi , Zhuo, Zengqing , Yang, Wanli , Wu, Lingqiao et al. Dual-Gradient Construction on Li-Rich Cathodes for High Stability Lithium Battery . | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
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Abstract ：
With the rising demand of lithium batteries from application fields including electric vehicles (EVs) and various electric aircrafts, it is imperative to greatly enhance the energy density of lithium batteries by rational design. However, there is still a lack of design roadmap for high-energy-density lithium batteries, largely owing to the uncertain selections of electrochemically active materials and the complicated relationships of diverse factors. In this article, based on the discussion of effects of key components and prototype design of lithium batteries with different energy density classes, we aim to tentatively present an overall and systematic design principle and roadmap, covering the key factors and reflecting crucial relationships. This article starts from the fundamental principles of battery design, and the effects of cathode, anode, electrolyte, and other components to realize highenergy-density lithium batteries have been discussed. Based on the prototype design of high-energy-density lithium batteries, it is shown that energy densities of different classes up to 1000 Wh/kg can be realized, where lithium-rich layered oxides (LLOs) and solid-state electrolytes play central roles to gain high energy densities above 500 Wh/kg. Lithium batteries are thus categorized according to different energy density classes, with available component options, to meet their most suitable application scenes.
Keyword ：
High-energy-density High-energy-density Lithium batteries Lithium batteries Solid-state batteries Solid-state batteries Design principle Design principle Lithium-rich layered oxides Lithium-rich layered oxides
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| GB/T 7714 | Du, Haozhe , Zhang, Xu , Yu, Haijun . Design of high-energy-density lithium batteries: Liquid to all solid state [J]. | ETRANSPORTATION , 2025 , 23 . |
| MLA | Du, Haozhe et al. "Design of high-energy-density lithium batteries: Liquid to all solid state" . | ETRANSPORTATION 23 (2025) . |
| APA | Du, Haozhe , Zhang, Xu , Yu, Haijun . Design of high-energy-density lithium batteries: Liquid to all solid state . | ETRANSPORTATION , 2025 , 23 . |
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Abstract ：
Manganese-based (Mn-based) layered oxides have emerged as competitive cathode materials for sodium-ion batteries (SIBs), primarily due to their high energy density, cost-effectiveness, and potential for mass production. However, these materials often suffer from irreversible oxygen redox reactions, significant phase transitions, and microcrack formation, which lead to considerable internal stress and degradation of electrochemical performance. This study introduces a high-entropy engineering strategy for P2-type Mn-based layered oxide cathodes (HE-NMCO), wherein a multi-ingredient cocktail effect strengthens the lattice framework by modulating the local environmental chemistry. This innovative approach fosters sustainable reversible oxygen activity, mitigates stress concentrations at grain boundaries, and accelerates Na+ transport kinetics. The resulting robust lattice framework with optimized elemental interactions significantly improves structural integrity and reduces the formation of intragranular fractures. Consequently, HE-NMCO demonstrates remarkable cycling stability, retaining 93.5 % capacity after 100 deep (de)sodiation cycles, alongside an enhanced rate capability of 134.1 mAh g-1 at 5 C. Notably, comparative studies through multimodal characterization techniques highlight HE-NMCO ' s superior reversibility in oxygen anion redox (OAR) reactions over extensive cycling, contrasting sharply with conventional NMCO cathode. This work elucidates the potential for advancing high energy and power density Mn-based cathodes for SIBs through local species diversity.
Keyword ：
Mn-based cathode Mn-based cathode high-entropy configuration high-entropy configuration lattice stress lattice stress Na-ion battery Na-ion battery oxygen redox oxygen redox
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| GB/T 7714 | Liu, Shiqi , Liu, Fangzheng , Zhao, Shu et al. A High-Entropy Engineering on Sustainable Anionic Redox Mn-Based Cathode with Retardant Stress for High-Rate Sodium-Ion Batteries [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (10) . |
| MLA | Liu, Shiqi et al. "A High-Entropy Engineering on Sustainable Anionic Redox Mn-Based Cathode with Retardant Stress for High-Rate Sodium-Ion Batteries" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 10 (2025) . |
| APA | Liu, Shiqi , Liu, Fangzheng , Zhao, Shu , Zhuo, Zengqing , Xiao, Dongdong , Cui, Zhongyi et al. A High-Entropy Engineering on Sustainable Anionic Redox Mn-Based Cathode with Retardant Stress for High-Rate Sodium-Ion Batteries . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (10) . |
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Abstract ：
The cobalt-free Mn-based Li-rich layered oxide material has the advantages of low cost, high energy density, and good performance at low temperatures, and is the promising choice for energy storage batteries. However, the long-cycling stability of batteries needs to be improved. Herein, the Mn-based Li-rich cathode materials with small amounts of Li2MnO3 crystal domains and gradient doping of Al and Ti elements from the surface to the bulk have been developed to improve the structure and interface stability. Then the batteries with a high energy density of 600 Wh kg(-1), excellent capacity retention of 99.7 % with low voltage decay of 0.03 mV cycle(-1) after 800 cycles, and good rates performances can be achieved. Therefore, the structure and cycling stability of low voltage Mn-based Li-rich cathode materials can be significantly improved by the bulk structure design and interface regulation, and this work has paved the way for developing low-cost and high-energy Mn-based energy storage batteries with long lifetime. (c) 2024 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.
Keyword ：
Lithium-ion batteries Lithium-ion batteries Elemental gradient Elemental gradient Li2MnO3 crystal domain Li2MnO3 crystal domain Mn-based Li-rich layered oxide cathode Mn-based Li-rich layered oxide cathode Energy storage Energy storage
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| GB/T 7714 | Wang, Yinzhong , Liu, Shiqi , Guo, Xianwei et al. Elements gradient doping in Mn-based Li-rich layered oxides for long-life lithium-ion batteries [J]. | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY , 2025 , 207 : 266-273 . |
| MLA | Wang, Yinzhong et al. "Elements gradient doping in Mn-based Li-rich layered oxides for long-life lithium-ion batteries" . | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY 207 (2025) : 266-273 . |
| APA | Wang, Yinzhong , Liu, Shiqi , Guo, Xianwei , Wang, Boya , Zhang, Qinghua , Li, Yuqiang et al. Elements gradient doping in Mn-based Li-rich layered oxides for long-life lithium-ion batteries . | JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY , 2025 , 207 , 266-273 . |
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Abstract ：
Fluorinated polymer matrix emerges as a promising candidate owing to their enhanced anti-oxidation ability, but their application is plagued by the relatively low ion conduction ability and the ambiguous ionic conduction mechanism in the fluorinated polymer electrolytes (PEs). Herein, a series of acrylate-based electrolytes with different fluorinated functional units (fluorinated-FUs) of poly(ethyl methacrylate) electrolyte (0F PE), poly (trifluoroethyl methacrylate) electrolyte (3F PE) and poly(hexafluorobutyl methacrylate) electrolyte (6F PE) were investigated. Beneficial from the long fluorinated-FUs in the side chain, the 6F PE exhibits improved both ionic conductivity of 4.0x10(-4) S cm(-1) and Li+ transference number of 0.65 at 25 degrees C, which are superior to those of the 0F PE and the 3F PE. The enhanced ion conduction mechanism was clarified via combining the theoretical calculations and experimental data, where the integration of local fluorinated-FUs provides additional coordinating sites for the continuous Li+ migration and regulates the ion transporting pathways. This work demonstrates that the regulation of local fluorinated-FUs can provide a promising strategy for achieving high performance PEs applied in solid-state batteries.
Keyword ：
Local fluorinated functional units Local fluorinated functional units Polymer electrolytes Polymer electrolytes Mechanism of ion transport Mechanism of ion transport Ion-dipole interaction Ion-dipole interaction Solid-state lithium metal battery Solid-state lithium metal battery
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| GB/T 7714 | Ding, Peipei , Zhao, Shu , Lin, Zhiyuan et al. Local fluorinated functional units enhance Li+ transport in acrylate-based polymer electrolytes for lithium metal batteries [J]. | NANO ENERGY , 2024 , 129 . |
| MLA | Ding, Peipei et al. "Local fluorinated functional units enhance Li+ transport in acrylate-based polymer electrolytes for lithium metal batteries" . | NANO ENERGY 129 (2024) . |
| APA | Ding, Peipei , Zhao, Shu , Lin, Zhiyuan , Wu, Lingqiao , Xu, Ligang , Liu, Shiqi et al. Local fluorinated functional units enhance Li+ transport in acrylate-based polymer electrolytes for lithium metal batteries . | NANO ENERGY , 2024 , 129 . |
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Abstract ：
With the increasing demand for high energy density (>400 Wh kg-1) of lithium-ion batteries (LIBs), the higher demand for electrolytes is put forward to meet the performance of high voltage, fast charge, wide temperature, and low flammability. However, ethylene carbonate (EC) with low melting point and flammability in the commercial electrolyte will suffer a series of side reactions such as nucleophilic, dehydrogenation, and ring-opening at the cathode interphase at a voltage of >4.3 V, forming an organic-rich unstable interphase at the electrodes, which cannot match the current high energy density battery. To address this bottleneck, researchers have developed a series of EC-free electrolyte systems. The oxidation resistance of the electrolyte itself, the solvation structure, and the stable, in situ formed electrode/electrolyte interphase play a crucial role in the performance of high energy density lithium batteries, such as fast charge, wide temperature, high safety, and long cycle life. In this review, the development history, latest progress, scientific challenges, design strategies, and action mechanisms of EC-free electrolytes are comprehensively and systematically summarized. Finally, the most promising EC-free electrolyte design scheme is proposed to stimulate the wide application of next-generation lithium-ion batteries with high energy density.
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| GB/T 7714 | Xu, Congyu , Liang, Yuan , Zhang, Ruochen et al. Ethylene Carbonate-Free Electrolytes for High Voltage Lithium-Ion Batteries: Progress and Perspectives [J]. | ENERGY & FUELS , 2024 , 38 (19) : 18208-18226 . |
| MLA | Xu, Congyu et al. "Ethylene Carbonate-Free Electrolytes for High Voltage Lithium-Ion Batteries: Progress and Perspectives" . | ENERGY & FUELS 38 . 19 (2024) : 18208-18226 . |
| APA | Xu, Congyu , Liang, Yuan , Zhang, Ruochen , Cheng, Jianghan , Yu, Haijun . Ethylene Carbonate-Free Electrolytes for High Voltage Lithium-Ion Batteries: Progress and Perspectives . | ENERGY & FUELS , 2024 , 38 (19) , 18208-18226 . |
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Abstract ：
The state-of-the-art layered oxide as the cathode material for lithium-ion batteries has attracted wide attention; however, harsh operations of high-energy and high-safety energy-storage technology at high temperature is challenging owing to the aggravated structural instability and parasitic reactions at the cathodes. Herein, the layered/olivine composite structure architecture is designed at the grain surface to govern constant electrochemistry in a harsh environment, and a gradient LiF interlayer is developed onto the cathodes to suppress the interfacial degradation. By a combination of interfacial-sensitive characterizations and theoretical analysis at the cathode/interface, the formation mechanism of this special interphase induced by the composite structure cathode is revealed. The composite structure cathode could deliver an excellent high-temperature cycling stability with 90.8% retention for 300 cycles in the half cell and 95.6% retention for 1000 cycles in the pouch cell and simultaneously enhances similar to 51% of the thermal stability, which broadens the approaches for developing high-stable cathodes that work in extreme environments.
Keyword ：
layered/olivine structure layered/olivine structure lithium-ion battery lithium-ion battery interfacialstability interfacialstability gradient interface gradient interface composite structure composite structure
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| GB/T 7714 | Tian, Shaoze , Liu, Shiqi , Du, Haozhe et al. Layered/Olivine Composite Structure-Induced Stable Gradient Interfacial Chemistry toward High-Temperature Lithium-Ion Batteries [J]. | ACS NANO , 2024 , 18 (46) : 32065-32076 . |
| MLA | Tian, Shaoze et al. "Layered/Olivine Composite Structure-Induced Stable Gradient Interfacial Chemistry toward High-Temperature Lithium-Ion Batteries" . | ACS NANO 18 . 46 (2024) : 32065-32076 . |
| APA | Tian, Shaoze , Liu, Shiqi , Du, Haozhe , Zhang, Runke , Wang, Yulong , Ding, Peipei et al. Layered/Olivine Composite Structure-Induced Stable Gradient Interfacial Chemistry toward High-Temperature Lithium-Ion Batteries . | ACS NANO , 2024 , 18 (46) , 32065-32076 . |
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Abstract ：
Stable electrolytes are urgently required for lithium-ion batteries based on lithium-rich layered oxides (LLOs), which generally suffer from fast capacity and voltage decay at high voltages up to 4.8 V. Herein, we report a salt-concentrated electrolyte consisting of 4 M lithium hexafluorophosphate (LiPF6) salt in ester solvents of fluoroethylene carbonate (FEC) and dimethyl carbonate (DMC) to alleviate the above challenges. The solvent structure in the 4 M electrolyte shows more volatile DMC integrated with Li+ and more free antioxidative FEC compared with a 1 M electrolyte, broadening the operation voltage. Simultaneously, this electrolyte endows a thin yet high elasticity modulus LiF-rich interphase on the LLOs surface, which can effectively prevent diverse side reactions and transition metal migration, consequently improving the electrochemical performance with a voltage decay of only 0.46 mV/cycle and capacity retention of 80.3% after 500 cycles. This simple and effective approach boosts the development of high-energy-density batteries using LLOs.
Keyword ：
Lithium-ion battery Lithium-ion battery High elastic modulus High elastic modulus Li-rich layered oxides Li-rich layered oxides Cathode-electrolyte interphase Cathode-electrolyte interphase Salt-concentration electrolyte Salt-concentration electrolyte
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| GB/T 7714 | Han, Zhijie , Liang, Yuan , Zhao, Shu et al. Salt-Concentrated Electrolyte Constructing High Elasticity Modulus Interphase for Li-Rich Layered Oxide Cathode [J]. | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (47) : 64646-64655 . |
| MLA | Han, Zhijie et al. "Salt-Concentrated Electrolyte Constructing High Elasticity Modulus Interphase for Li-Rich Layered Oxide Cathode" . | ACS APPLIED MATERIALS & INTERFACES 16 . 47 (2024) : 64646-64655 . |
| APA | Han, Zhijie , Liang, Yuan , Zhao, Shu , Zhu, Qianwen , Zhao, Jingteng , Wang, Errui et al. Salt-Concentrated Electrolyte Constructing High Elasticity Modulus Interphase for Li-Rich Layered Oxide Cathode . | ACS APPLIED MATERIALS & INTERFACES , 2024 , 16 (47) , 64646-64655 . |
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Abstract ：
Elemental doping is widely used to improve the performance of cathode materials in lithium-ion batteries. However, macroscopic/statistical investigation on how doping sites are distributed in the material lattice, despite being a key prerequisite for understanding and manipulating the doping effect, has not been effectively established. Herein, to solve this predicament, a universal strategy is proposed to quantitatively identify the locations of Al and Mg dopants in lithium-rich layered oxides (LLOs). Solid evidence confirms that Al prefers to occupy the transition metal (TM) layer, while Mg evenly occupies both TM and Li layers. As a result, Mg significantly reduces the thickness of LiO2 slabs at room temperature, which will increase the energy barrier of oxygen activation and enhance the structure stability of LLOs. The suppressed oxygen activity in Mg-doped LLO can be kinetically unlocked at 55 degrees C. The different characteristics of Al and Mg enlighten an Al/Mg co-doping strategy to optimize LLOs, which significantly improves the cycle performance while lifting the capacity. These insights from the quantitative identification of doping sites shed light on the manipulation of doping effects toward better cathodes.
Keyword ：
cycle performance cycle performance lithium-rich layered oxides lithium-rich layered oxides oxygen activity oxygen activity doping sites doping sites lithium-ion battery lithium-ion battery
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| GB/T 7714 | Wu, Tianhao , Zhang, Xu , Li, Yuqiang et al. Quantitative Identification of Dopant Occupation in Li-Rich Cathodes [J]. | ADVANCED MATERIALS , 2024 . |
| MLA | Wu, Tianhao et al. "Quantitative Identification of Dopant Occupation in Li-Rich Cathodes" . | ADVANCED MATERIALS (2024) . |
| APA | Wu, Tianhao , Zhang, Xu , Li, Yuqiang , Du, Haozhe , Liu, Tongchao , Yang, Yubo et al. Quantitative Identification of Dopant Occupation in Li-Rich Cathodes . | ADVANCED MATERIALS , 2024 . |
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Abstract ：
Solid-state Li metal batteries (SSLMBs) are widely investigated since they possess promising energy density and high safety. However, the poor interfacial compatibility between the electrolyte and electrodes limits their promising development. Herein, a robust composite electrolyte (poly(vinyl ethylene carbonate) electrolyte with 3 wt % of BaTiO3, PVEC-3BTO) with excellent interfacial performance is rationally designed by incorporating ferroelectric BaTiO3 (BTO) nanoparticles into the poly(vinyl ethylene carbonate) (PVEC) electrolyte matrix. Benefiting from the high dielectric constant and ferroelectric properties of BTO, the interfacial compatibility between electrolytes and electrodes was significantly improved. The enhanced Li+ transference number (0.64) of solid electrolyte and in situ generated BaF2 inorganic interphase contribute to the enhanced cycling stability of PVEC-3BTO based Li//Li symmetrical batteries. Furthermore, the antioxidation ability of PVEC-3BTO has also been enhanced by modulating the local electric field for good pairing with high-voltage LiCoO2 material. Therefore, in this work, the mechanism of BTO for improving interfacial compatibility is revealed, and also useful methods for addressing the interface issues of SSLMBs have been provided.
Keyword ：
local electric field local electric field interfacial compatibility interfacial compatibility Li metal battery Li metal battery composite solid-state electrolyte composite solid-state electrolyte ferroelectric BaTiO3 ferroelectric BaTiO3
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| GB/T 7714 | Wu, Lingqiao , Lv, Haoran , Zhang, Rui et al. Ferroelectric BaTiO3 Regulating the Local Electric Field for Interfacial Stability in Solid-State Lithium Metal Batteries [J]. | ACS NANO , 2024 , 18 (7) : 5498-5509 . |
| MLA | Wu, Lingqiao et al. "Ferroelectric BaTiO3 Regulating the Local Electric Field for Interfacial Stability in Solid-State Lithium Metal Batteries" . | ACS NANO 18 . 7 (2024) : 5498-5509 . |
| APA | Wu, Lingqiao , Lv, Haoran , Zhang, Rui , Ding, Peipei , Tang, Mingxue , Liu, Shiqi et al. Ferroelectric BaTiO3 Regulating the Local Electric Field for Interfacial Stability in Solid-State Lithium Metal Batteries . | ACS NANO , 2024 , 18 (7) , 5498-5509 . |
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