Compositional Gradient Design of Ni-Rich Co-Poor Cathodes Enhanced Cyclability and Safety in High-Voltage Li-Ion Batteries DOI

Wenshuai Guo,

Haifeng Yu, Min Wang

и другие.

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Фев. 20, 2025

Developing cost-effective high-voltage Ni-rich cathodes has reached a consensus to replace conventional ultrahigh Ni counterparts for high-energy Li-ion batteries, but more rigorous requirements are put forward their mechanical and chemical stability. Herein, we report the design synthesis of full concentration gradient LiNi0.75Mn0.20Co0.05O2 cathode with Mn-rich Ni-poor surface, which been realized by in situ forming PO43- distribution retard transition-metal ions' interdiffusion during high-temperature lithiation process. This mitigates stress at source high morphological integrity refrains lattice oxygen loss under 4.5 V operation. After Li0.1B0.967PO4 is coated, surface parasitic reactions further ameliorated stable interface chemistry. The resultant deliver reversible capacity as 212.6 mAh g-1 2.7-4.5 an energy density >800 Wh kg-1cathode, almost equivalent state-of-the-art Ni-content 90% 2.7-4.3 V. In commercial-grade cells, superior cycle life 80.5% retention achieved 1C within after 1700 cycles, exhibiting promising opportunities compositional cathodes.

Язык: Английский

Thermal Stability and Outgassing Behaviors of High‐nickel Cathodes in Lithium‐ion Batteries DOI Creative Commons
Zehao Cui, Arumugam Manthiram

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(43)

Опубликована: Июнь 9, 2023

Abstract LiNiO 2 ‐based high‐nickel layered oxide cathodes are regarded as promising cathode materials for high‐energy‐density automotive lithium batteries. Most of the attention thus far has been paid towards addressing their surface and structural instability issues brought by increase Ni content (>90 %) with an aim to enhance cycle stability. However, poor safety performance remains intractable problem commercialization in market, yet it not received appropriate attention. In this review, we focus on gas generation thermal degradation behaviors high‐Ni cathodes, which critical factors determining overall performance. A comprehensive overview mechanisms outgassing runaway reactions is presented analyzed from a chemistry perspective. Finally, discuss challenges insights into developing robust, safe cathodes.

Язык: Английский

Процитировано

93

Electrolytes with Solvating Inner Sheath Engineering for Practical Na–S Batteries DOI Creative Commons
Dong Guo, Jiaao Wang, Tianxing Lai

и другие.

Advanced Materials, Год журнала: 2023, Номер 35(24)

Опубликована: Март 16, 2023

Sodium-sulfur (Na-S) batteries with durable Na-metal stability, shuttle-free cyclability, and long lifespan are promising to large-scale energy storages. However, meeting these stringent requirements poses huge challenges the existing electrolytes. Herein, a localized saturated electrolyte (LSE) is proposed 2-methyltetrahydrofuran (MeTHF) as an inner sheath solvent, which represents new category of for Na-S system. Unlike traditional high concentration electrolytes, LSE realized low salt-to-solvent ratio diluent-to-solvent ratio, pushes limit (LHCE). The appropriate molecular structure solvation ability MeTHF regulate sheath, features reinforced coordination Na+ anions, enlarged -solvent distance, weakened anion-diluent interaction. Such configuration found be key build sustainable interphase quasi-solid-solid sulfur redox process, making dendrite-inhibited battery possible. With this electrolyte, pouch cells decent cycling performance under rather demanding conditions demonstrated.

Язык: Английский

Процитировано

62

Insights into the precursor specific surface area for engineering Co-free Ni-rich cathodes with tailorable properties DOI
Kang‐Yu Zou,

Shangchen Xie,

Mingzhu Jiang

и другие.

Chemical Engineering Journal, Год журнала: 2024, Номер 483, С. 149189 - 149189

Опубликована: Фев. 2, 2024

Язык: Английский

Процитировано

37

Factors Influencing Gas Evolution from High‐Nickel Layered Oxide Cathodes in Lithium‐Based Batteries DOI

Richard Sim,

Arumugam Manthiram

Advanced Energy Materials, Год журнала: 2024, Номер 14(8)

Опубликована: Янв. 26, 2024

Abstract Gas evolution from high‐nickel layered oxide cathodes (>90% Ni) remains a major issue for their practical application. Gaseous species, such as CO 2 , O and CO, that are evolved at high states of charge (SOC) worsen the overall safety batteries, pressure build‐up within cell may lead to rupture. Since these gasses produced during cathode degradation, tracking formation is also important in diagnosing failure. Online electrochemical mass spectrometry (OEMS) powerful situ technique study gas high‐voltage charge. However, differences OEMS experimental setups between different groups make it challenging compare results groups. In this perspective, various factors influence based on collected group presented. The focus conditions release, with particular emphasis reactive oxygen subsequent chemical reactions electrolyte. Promising strategies, electrolytes, compositional tuning, surface coatings effective suppressing highlighted. Critical insights into mitigating degradation provided guide development safer, high‐energy batteries.

Язык: Английский

Процитировано

30

Unraveling 3d Transition Metal (Ni, Co, Mn, Fe, Cr, V) Ions Migration in Layered Oxide Cathodes: A Pathway to Superior Li‐Ion and Na‐Ion Battery Cathodes DOI Open Access
Shengnan He, Rui Zhang,

Xi Han

и другие.

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 13, 2025

Abstract Li‐ion and Na‐ion batteries are promising systems for powering electric vehicles grid storage. Layered 3d transition metal oxides A x TMO 2 (A = Li, Na; TM metals; 0 < ≤ 2) have drawn extensive attention as cathode materials due to their exceptional energy densities. However, they suffer from several technical challenges caused by crystal structure degradation associated with ions migration, such poor cycling stability, inferior rate capability, significant voltage hysteresis, serious decay. Aiming tackle these challenges, this review provides an in‐depth discussion comprehensive understanding of the migration behaviors in . First, key thermodynamics kinetics that impact discussed, covering ionic radius, electronic configuration, arrangement, barrier. In particular, details provided regarding universal specific characteristics Ni, Co, Mn, Fe, Cr, V layered materials. Subsequently, impacts migrations on electrochemical performance emphasized terms fundamental science behind issues, strategies modulate advanced development summarized. Besides, characterization techniques probing present, like neutron diffraction (ND), scanning transmission electron microscopy (STEM), nuclear magnetic resonance (NMR), others. Finally, future directions regard comprehensively concluded. This offers valuable insights into basic design oxide batteries.

Язык: Английский

Процитировано

3

Understanding the Insight Mechanism of Chemical‐Mechanical Degradation of Layered Co‐Free Ni‐Rich Cathode Materials: A Review DOI
Hang Li, Li Wang,

Youzhi Song

и другие.

Small, Год журнала: 2023, Номер 19(32)

Опубликована: Май 8, 2023

Abstract Layered Cobalt (Co)‐free Nickel (Ni)‐rich cathode materials have attracted much attention due to their high energy density and low cost. Still, further development is hampered by material instability caused the chemical/mechanical degradation of material. Although there are numerous doping modification approaches improve stability layered materials, these still in laboratory stage require research before commercial application. To fully exploit potential a more comprehensive theoretical understanding underlying issues necessary, along with active exploration previously unrevealed mechanisms. This paper presents phase transition mechanism Co‐free Ni‐rich existing problems, state‐of‐the‐art characterization tools employed study transition. The causes crystal structure degradation, interfacial instability, mechanical elaborated, from material's its atomic orbital splitting. By organizing summarizing mechanisms, this aims establish connections among common problems identify future priorities, thereby facilitating rapid materials.

Язык: Английский

Процитировано

37

Localized High‐Concentration Electrolytes with Low‐Cost Diluents Compatible with Both Cobalt‐Free LiNiO2 Cathode and Lithium‐Metal Anode DOI Open Access
Zezhou Guo, Zehao Cui,

Richard Sim

и другие.

Small, Год журнала: 2023, Номер 19(49)

Опубликована: Авг. 11, 2023

Abstract High‐nickel layered oxide cathodes and lithium‐metal anode are promising candidates for next‐generation battery systems due to their high energy density. Nevertheless, the instability of electrode–electrolyte interphase is hindering practical application. Localized high‐concentration electrolytes (LHCEs) present a solution achieving uniform lithium deposition stable cathode–electrolyte interphase. However, limited choice diluents cost restricting implementation. Four novel cost‐effective performance with highly reactive LiNiO 2 cathode Li‐metal reported here. The results show that all LHCE cells exhibit Coulombic efficiency >99.38% in Li | Cu capacity retention >85% after 250 cycles. Advanced characterizations unveil cell operation well‐tuned interphases morphology. In addition, online electrochemical mass spectroscopy differential scanning calorimetry reveal gas generation heat‐release greatly reduced LHCEs presented. Overall, study provides new insights into role offers valuable guidance further optimization density batteries.

Язык: Английский

Процитировано

36

Impact of Dopants on Suppressing Gas Evolution from High-Nickel Layered Oxide Cathodes DOI

Richard Sim,

Zehao Cui, Arumugam Manthiram

и другие.

ACS Energy Letters, Год журнала: 2023, Номер 8(12), С. 5143 - 5148

Опубликована: Ноя. 17, 2023

Gas release from high-Ni layered oxide cathodes (LiNixMn1-x-y-zCoyAlzO2; x > 0.8) can jeopardize the overall performance and safety characteristics of cell. A comprehensive assessment rational cathode design with common dopants, such as Ni, Co, Al, Mn, to suppress gas evolution is crucial for battery safety, yet it remains be conducted. Here, we present an in situ analysis nine materials online electrochemical mass spectrometry (OEMS). We show that, regardless dopant, reactive oxygen lattice a critical process evolution. series comparisons reveals that intensity onset point are strongly dependent on composition. Notably, Al Mn most effective dopants at 4.4 V. further highlight stability limits, across these compositions, between 85% 93% state-of-charge.

Язык: Английский

Процитировано

30

Understanding the Effects of Al and Mn Doping on the H2–H3 Phase Transition in High-Nickel Layered Oxide Cathodes DOI

J. Brandon Adamo,

Arumugam Manthiram

Chemistry of Materials, Год журнала: 2024, Номер 36(12), С. 6226 - 6236

Опубликована: Июнь 4, 2024

High-nickel layered oxide cathodes make up a promising family of materials for next-generation lithium-ion batteries (LIBs). Deleterious phase transitions and surface instabilities, however, have hindered their mass adoption. Al doping Mn both been shown to improve cyclability at the expense initial capacity. However, effects these dopants on performance high-voltage H2–H3 transition remain unexplored. Herein, we examine in Li[Ni0.95Al0.05]O2 Li[Ni0.95Mn0.05]O2 comparison that undoped LiNiO2 (LNO). We find 5% suppress delay higher voltage but appear affect its reversibility only minimally. further reduce increase impedance with when passing through do so Cyclic step chronoamperometry shows rate compared LNO. This is attributed widened lithium diffusion channels high states charge enabled by dopants, which verified X-ray diffraction. work provides insights into transition, necessary optimized cycling protocols LIBs, improves our general understanding crucial energy materials.

Язык: Английский

Процитировано

15

Enabling the Strengthened Structural and Interfacial Stability of High‐Nickel LiNi0.9Co0.05Mn0.05O2 Cathode by a Coating‐Doping‐Microstructure Regulation Three‐In‐One Strategy DOI

Yue Zou,

Yonglin Tang, Qizheng Zheng

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Июль 10, 2024

Abstract High‐nickel layered cathodes exhibit great promise in advancing high‐energy‐density batteries owing to their significant advantages high energy capacity and low cost, but they suffer severe structural interfacial deterioration during cycling, resulting safety risk reduced cycle life. Herein, drawing inspiration from the melting point infusion capability of Sb 2 Se 3 , a three‐pronged strategy aimed at simultaneously achieving coating on primary secondary particles surface, doping elongated slimed particle morphology is proposed developed fortify stability high‐nickel LiNi 0.9 Co 0.05 Mn O (NCM90) cathode. The “melted infused” plays beneficial role defensive effect particle's surfaces, mitigating deterioration. In addition, enhanced achieved by both 5+ regulated morphology, contributing alleviated breakage ultimately reinforced cycling stability. Consequently, ‐NCM90 electrodes significantly improve performance, which maintain higher retentions 96.6% 4.3 V after 100 cycles 80.2% 1C/5C 500 cycles. coating‐doping‐microstructure regulation three‐in‐one for improving NCM offers innovative ideas design advancement lithium‐ion batteries.

Язык: Английский

Процитировано

14