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Small · 2024 ·Vol. 20 ·期 34 ·2312059 · IF 13

Construction of Hierarchical Conductive Networks for LiNi0.8Mn0.1Co0.1O2 Cathode toward Stable Cycling at High Areal Mass Loadings

Lu Wei,Hongyuan Wu,Songtao Liu,Yuyu Zhou,Xin Guo

Realizing high-performance thick electrodes is considered as a practical strategy to promote the energy density of lithium-ion batteries. However, establishing effective transport pathways for both lithium-ions and electrons in a thick electrode is very challenging. This study develops a hierarchical conductive network structure for constructing high-performance NMC811 (LiNi 0.8 Mn 0.1 Co 0.1 O 2 ) cathode toward stable cycling at high areal mass loadings. The hierarchical conductive networks are composed of a Li + /e − mixed conducting interface (lithium polyacrylate/hydroxyl-functionalized multiwalled carbon nanotubes) on NMC811 particles, and a segregated network of single-walled carbon nanotubes in the electrode, without any additional binders or carbon black. Such strategy endows the NMC811 cathode (up to 250 µm and 50 mg cm −2 ) with low porosity/tortuosity, ultrahigh Li + /e - conductivities and excellent mechanical property at low carbon nanotube content (1.8 wt%). It significantly improves the electrochemical reaction homogeneity along the electrode depth, meanwhile effectively inhibits the side reactions at the electrode/electrolyte interface and cracks in the NMC particles during cycling. This work emphasizes the crucial role of the electronic/ionic cooperative transportation in the performance deterioration of thick cathodes, and provide guidance for architecture optimization and performance improvement of thick electrodes toward practical applications, not just for the NMC811 cathode.

研究领域: 材料科学 · 电化学
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Small · 2025 · IF 12.1

A Comprehensive Strategy Enables High-Loading BiOBr@BiOIO3 Cathodes for Quasi Ah-Level Aqueous Zn-Ion Batteries

Jiajun Wan,Qian Zhang,Xu Jia,Pengfei Zhang,Yuanze Yu,Jiyang Tian,Jie Liu

Aqueous Zn-ion batteries (AZIBs) recently have attracted broad attention. To achieve high energy density of AZIBs, constructing high-loading cathodes is the prerequisite. However, the cycling stability of high-loading cathodes still faces great challenges. Herein, a comprehensive strategy is proposed to improve the structural stability of the cathode material and mechanical stability of the high-loading cathode. The BiOBr@BiOIO 3 heterostructure are successfully constructed via sharing the interfacial oxygen atoms, in which the interfacial effect can effectively enhance the reaction dynamics and structural stability. Meanwhile, a biomimetic binder is skillfully designed via in situ dual cross-linking between guar gum and cation ions to achieve the application of water-based and sustainable polymer binder in AZIBs. Density functional theory calculations demonstrate the guar gum possesses strong affinity toward BiOBr@BiOIO 3 to firmly adhere the active materials. Quantitative nanomechanic technology visually demonstrates the robust mechanical properties of the as-obtained BiOBr@BiOIO 3 cathode. As a result, when the active material loading increases to as high as 100.71 mg cm −2 , an ultrahigh areal capacity of 20.02 mAh cm −2 can be achieved. Specially, a quasi-Ah-level (0.244 Ah) pouch-type cell with a loading of 1.17 g can be constructed, showing the practical application potential.

研究领域: 材料科学 · 电化学 · 储能技术
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Journal of Physical Chemistry C · 2023 · IF 3.7

Flame-Retardant Gel Electrolyte toward High-Safety Lithium Metal Batteries with High-Mass-Loading Cathodes

Geng Tang,Shao-Peng Shen,Hong-Ji Li,Liang Zhang,Jin-Chi Zheng,Yuan Luo,Jun-Pei Yue,Yongzheng Shi,Zhe Chen

Gel electrolytes are an important transitional state in developing lithium-ion conductors from the liquid state to the solid state. However, very few gel electrolytes have been realized to enable the long-term operation of high-safety lithium metal batteries (LMBs) with high-mass-loading cathodes. Here, we propose a dual-salt gel electrolyte with a flame-retardant plasticizer (denoted as PVC/TEP electrolyte) for LMBs. Flame-retardant molecules were encapsulated into the PVC matrix via in situ polymerization of a vinylene carbonate monomer. The resultant PVC/TEP electrolyte possesses a high ionic conductivity of ∼3.1 × 10–3 S cm–1 at 30 °C, a wide electrochemical window of ∼4.85 V, and low self-extinguishing times of less than 0.3 s g–1 due to the homogeneous distribution of flame-retardant and fluorine-rich dual salts. Consequently, gel electrolyte-based LMBs with high-mass-loading cathodes (8.49 mg cm–2) achieve comparable rate performance to liquid electrolyte-based LMBs and long cycle life well beyond them.

研究领域: 材料科学 · 电化学 · 能源存储
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ELECTROCHIMICA ACTA · 2021 · IF 6.901

3-Thiopheneboronic acid: an effective additive for regulation on electrode/electrolyte interphase of lithium metal battery with high-loading cathode

Wenhao Ren,Yun Huang,Saisai Li,Junyuan Gan,Jun Yang,Xing Li,Mingshan Wang,Haijun Cao

Lithium metal has been considered as a potential replacement for the commercialized graphite anode to further boost the energy density of Li-ion batteries. However, Li dendrite growth during Li plating/stripping causes safety concern and poor lifespan of Li metal batteries (LMBs). In addition, the deploy of Ni-rich high-loading LiNi x Co y Mn 1-x-y O 2 (NCM, 0.6 ≤  x  ≤ 0.95) is also an efficient way for boosting energy density. However, the dissolution of transition metal ion and structure evolution during cell operation can leave an adverse effect on cell performances. Herein, dual-functional 3-thiopheneboronic acid (TB) additive is used to form a lithium borate-rich solid electrolyte interphase (SEI) on Li anode and an improved cathode electrolyte interphase (CEI) on Ni-rich cathode. The TB-induced SEI layer is conductive and stable, and thus beneficial to improving kinetic limitation of Li nucleation and obtain a uniform morphology of Li deposition. When the TB-protected Li metal anode matches the high-loading LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NMC622) cathode (13.65 mg cm −2 ), high initial capacities of 163.78 mAh g −1 (2.23 mAh cm −2 ) at 0.2 C and 164.82 mAh g −1 (2.25 mAh cm −2 ) at 0.5 C after activation are obtained, attributing to the effective SEI and stable CEI induced by TB. This strategy of introducing additives into LMB system with Ni-rich high-loading NMC cathode affords an emerging energy storage system to demonstrates the material engineering of batteries with very high energy density.

CAS / MDL: 6165-69-1
研究领域: 材料科学 · 能源存储技术
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Novel Aliphatic polycarbonate binders for Solvent‑free manufacturing High‑loading cathodes of high-performance lithium-ion batteries

Guan Xi,Zhe Zhang,Lei Zhong,Shuanjin Wang,Min Xiao,Dongmei Han,Sheng Huang,Yuezhong Meng

To achieve high energy density lithium-ion battery depends on high area load of the active material in the cathode. However, it is challenging to attain high loading of active material by traditional wet coating method due to large amount of organic solvent used. A solvent-free manufacturing cathode that take advantages of viscous flow polymer binder under shearing force of ball-milling to bind the active materials and the conductive carbon uniformly on the current collector is an environment-friendly alternative and has attracted increasing attention. Herein, a solvent free manufacturing LiFeO 4 cathode with thermoplastic polymer poly(lactide-co-propylene carbonate) as functional binder has high area loading up to 57 mg/cm 2 of active material, and the battery assembled with such a LiFeO 4 cathode and lithium metal anode can release a specific capacity of 135.5 mAh/g at 0.2C. In addition, the cathode using poly(propylene carbonate) or polycaprolactone functional binder can also be loaded with 40 mg/cm 2 of active material, which expands the variety of binders for solvent free manufacturing electrodes. Solvent free manufacturing electrodes with such functional binders are expected to break through the technical bottleneck of lithium-ion battery with high energy density.

研究领域: 电化学 · 材料科学 · 能源存储 · 高分子化学 · 电池技术 · 绿色制造
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ADVANCED MATERIALS · 2020 ·Vol. 33 ·期 1 ·2002325 · IF 27.398

All-Solid-State Batteries with a Limited Lithium Metal Anode at Room Temperature using a Garnet-Based Electrolyte

Shaojie Chen,Jingxuan Zhang,Lu Nie,Xiangchen Hu,Yuanqi Huang,Yi Yu,Wei Liu

Metallic lithium (Li), considered as the ultimate anode, is expected to promise high-energy rechargeable batteries. However, owing to the continuous Li consumption during the repeated Li plating/stripping cycling, excess amount of the Li metal anode is commonly utilized in lithium-metal batteries (LMBs), leading to reduced energy density and increased cost. Here, an all-solid-state lithium-metal battery (ASSLMB) based on a garnet-oxide solid electrolyte with an ultralow negative/positive electrode capacity ratio (N/P ratio) is reported. Compared with the counterpart using a liquid electrolyte at the same low N/P ratios, ASSLMBs show longer cycling life, which is attributed to the higher Coulombic efficiency maintained during cycling. The effect of the species of the interface layer on the cycling performance of ASSLMBs with low N/P ratio is also studied. Importantly, it is demonstrated that the ASSLMB using a limited Li metal anode paired with a LiFePO 4 cathode (5.9 N/P ratio) delivers a stable long-term cycling performance at room temperature. Furthermore, it is revealed that enhanced specific energies for ASSLMBs with low N/P ratios can be further achieved by the use of a high-voltage or high mass-loading cathode. This study sheds light on the practical high-energy all-solid-state batteries under the constrained condition of a limited Li metal anode.

CAS / MDL: 1310-66-3 1314-23-4
研究领域: 材料科学 · 电化学 · 能量存储 · 电池技术
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JOURNAL OF POWER SOURCES · 2022 · IF 9.794

Enhanced performance of flexible quasi-solid-state lithium batteries with high-loading cathode enabled by laser drilling

Shaoping Wu,Hongpeng Zheng,Nan Zhang,Weizheng Cheng,Hezhou Liu,Huanan Duan

Gel electrolyte composite with high areal capacity cathode effectively improves battery energy density and safety. Still, the insufficient interface contact between electrolyte and electrode limits the capacity release inside the thick cathode. Here, we rationally design a self-supporting cathode and use the in-situ polymerization method to integrate the gel electrolyte with the cathode. This cathode can effectively reduce the content of inactive electrode components. Meanwhile, the design of the regularly-arranged pore structure of the cathode introduced by laser texturing facilitates the penetration of the prepolymer solution and enables outstanding lithium-ion transport. Notably, the quasi-solid LiFePO 4 /Li half-cell with active material loading of 8 mg cm −2 exhibits good electrochemical performance (118.5 mAh g −1 after 100 cycles at 0.2C at room temperature). Moreover, when the loading of active materials increases to 30 mg cm −2 , the LiFePO 4 /Li 4 Ti 5 O 12 full-cell can still have a relatively high discharge capacity (105.9 mAh g −1 after 400 cycles at 0.2C at room temperature). It is worth noting that the quasi-solid pouch cell prepared by in-situ polymerization has a certain flexibility, indicating that this strategy has application potential in flexible electronic devices.

研究领域: 材料科学 · 电化学 · 电池技术 · 柔性电子
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