Journal of the American Chemical Society
DOI: 10.1021/jacs.3c04734
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12 Jul 12:33
[ASAP] 3D Covalent Organic Framework as a Metastable Intermediate in the Formation of a Double-Stranded Helical Covalent Polymer
by Lacey J. Wayment, Xubo Wang, Shaofeng Huang, Matthew S. McCoy, Hongxuan Chen, Yiming Hu, Yinghua Jin, Sandeep Sharma, and Wei Zhang
07 Jun 02:24
Engineering the Structural Uniformity of Gel Polymer Electrolytes via Pattern‐Guided Alignment for Durable, Safe Solid‐State Lithium Metal Batteries
by Qi Kang,
Zechao Zhuang,
Yijie Liu,
Zhenhui Liu,
Yong Li,
Bin Sun,
Fei Pei,
Han Zhu,
Hongfei Li,
Pengli Li,
Ying Lin,
Kunming Shi,
Yingke Zhu,
Jie Chen,
Chaoqun Shi,
Yan Zhao,
Pingkai Jiang,
Yongyao Xia,
Dingsheng Wang,
Xingyi Huang
An ultrathin gel polymer electrolyte (P-PPL) with patterned structure and superior mechanical toughness (≈613%) for durable and safe solid-state lithium metal battery is developed. The special patterned structure enables rapid ionic transfer kinetics and uniform Li+ flux. The solid-state LiFePO4||P-PPL||Li batteries exhibit excellent cycling stability, high rate capacity as well as high safety.
Abstract
Ultrathin and super-toughness gel polymer electrolytes (GPEs) are the key enabling technology for durable, safe, and high-energy density solid-state lithium metal batteries (SSLMBs) but extremely challenging. However, GPEs with limited uniformity and continuity exhibit an uneven Li+ flux distribution, leading to nonuniform deposition. Herein, a fiber patterning strategy for developing and engineering ultrathin (16 µm) fibrous GPEs with high ionic conductivity (≈0.4 mS cm−1) and superior mechanical toughness (≈613%) for durable and safe SSLMBs is proposed. The special patterned structure provides fast Li+ transport channels and tailoring solvation structure of traditional LiPF6-based carbonate electrolyte, enabling rapid ionic transfer kinetics and uniform Li+ flux, and boosting stability against Li anodes, thus realizing ultralong Li plating/stripping in the symmetrical cell over 3000 h at 1.0 mA cm−2, 1.0 mAh cm−2. Moreover, the SSLMBs with high LiFePO4 loading of 10.58 mg cm−2 deliver ultralong stable cycling life over 1570 cycles at 1.0 C with 92.5% capacity retention and excellent rate capacity of 129.8 mAh g−1 at 5.0 C with a cut-off voltage of 4.2 V (100% depth-of-discharge). Patterned GPEs systems are powerful strategies for producing durable and safe SSLMBs.
27 Feb 07:25
Electrode–Electrolyte Interfacial Chemistry Modulation for Ultra‐High Rate Sodium‐Ion Batteries
by Zheng Tang,
Hong Wang,
Peng-Fei Wu,
Si-Yu Zhou,
Yuan-Cheng Huang,
Rui Zhang,
Dan Sun,
You-Gen Tang,
Haiyan Wang
In a THF-based electrolyte with a weak solvation structure, Na+ desolvation is fast and a uniform solid electrolyte interphase (SEI) with abundant NaF and organic compounds is generated on the commercial hard carbon anode. This greatly enhances the interface stability and enables the rapid migration of Na+ in the SEI, thus realizing the high rate capability, long-term stability and good low-temperature performance for the hard carbon anode.
Abstract
Sodium-ion batteries capable of operating at rate and temperature extremes are highly desirable, but elusive due to the dynamics and thermodynamics limitations. Herein, a strategy of electrode–electrolyte interfacial chemistry modulation is proposed. The commercial hard carbon demonstrates superior rate performance with 212 mAh g−1 at an ultra-high current density of 5 A g−1 in the electrolyte with weak ion solvation/desolvation, which is much higher than those in common electrolytes (nearly no capacity in carbonate-based electrolytes). Even at −20 °C, a high capacity of 175 mAh g−1 (74 % of its room-temperature capacity) can be maintained at 2 A g−1. Such an electrode retains 90 % of its initial capacity after 1000 cycles. As proven, weak ion solvation/desolvation of tetrahydrofuran greatly facilitates fast-ion diffusion at the SEI/electrolyte interface and homogeneous SEI with well-distributed NaF and organic components ensures fast Na+ diffusion through the SEI layer and a stable interface.
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