All-solid-state lithium-metal batteries (ASSLMBs) are widely considered as the ultimately advanced lithium batteries owing to their improved energy density and enhanced safety features. Among various solid electrolytes, sulfide solid electrolyte (SSE) Li 6 PS 5 Cl has garnered significant attention. However, its application is limited by its poor cyclability and low critical current density (CCD). In this study, we introduce a novel approach to enhance the performance of Li 6 PS 5 Cl by doping it with fluorine, using lithium fluoride nanoparticles (LiFs) as the doping precursor. The F-doped electrolyte Li 6 PS 5 Cl-0.2LiF(nano) shows a doubled CCD, from 0.5 to 1.0 mA/cm 2 without compromising the ionic conductivity; in fact, conductivity is enhanced from 2.82 to 3.30 mS/cm, contrary to the typical performance decline seen in conventionally doped Li 6 PS 5 Cl electrolytes. In symmetric Li|SSE|Li cells, the lifetime of Li 6 PS 5 Cl-0.2LiF(nano) is 4 times longer than that of Li 6 PS 5 Cl, achieving 1500 h vs. 371 h under a charging/discharging current density of 0.2 mA/cm 2 . In Li|SSE|LiNbO 3 @NCM721 full cells, which are tested under a cycling rate of 0.1 C at 30 °C, the lifetime of Li 6 PS 5 Cl-0.2LiF(nano) is four times that of Li 6 PS 5 Cl, reaching 100 cycles vs. 26 cycles. Therefore, the doping of nano-LiF offers a promising approach to developing high-performance Li 6 PS 5 Cl for ASSLMBs. Graphical Abstract
Yan Wenlin,Mu Zhenliang,Wang Zhixuan,Huang Yuli,Wu Dengxu,Lu Pushun,Lu Jiaze,Xu Jieru,Wu Yujing,Ma Tenghuan,Yang Ming,Zhu Xiang,Xia Yu,Shi Shaochen,Chen Liquan,Li Hong,Wu Fan
All-solid-state batteries (ASSBs) with Li metal anodes or Si anodes are promising candidates to achieve high energy density and improved safety, but they suffer from undesirable lithium dendrite growth or huge volume expansion, respectively. Here we synthesize a hard-carbon-stabilized Li–Si alloy anode in which sintering of Si leads to the transformation of micro-metre particles into dense continuum. A 3D ionic-electronic-conductive network composed of plastically deformable Li-rich phases (Li 15 Si 4 and LiC 6 ) that enlarges active area and relieves stress concentration is created in the anode, leading to improved electrode kinetics and mechanical stability. With the hard-carbon-stabilized Li-Si anode, full cells using LiCoO 2 or LiNi 0.8 Co 0.1 Mn 0.1 O 2 cathodes and Li 6 PS 5 Cl electrolyte achieve favourable rate capability and cycle stability. In particular, the ASSB with LiNi 0.8 Co 0.1 Mn 0.1 O 2 at high loading of 5.86 mAh cm −2 delivers 5,000 cycles at 1 C (5.86 mA cm −2 ), demonstrating the potential of using hard-carbon-stabilized Li–Si alloy anodes for practical applications of ASSBs.
Jiaxing Lv,Ying Jiang,Guozhong Lu,Xiaobing Lou,Bingwen Hu
In traditional operations of all-solid-state lithium metal batteries (ASSLMBs), a small thin lithium metal circular disk is employed as a lithium metal anode (LMA). However, ASSLMBs with a circular-disk LMA often fail in <150 cycles with low capacity retention. In this work, we developed a new ring-shaped LMA to improve cyclability. Full cells consisting of a ring-shaped LMA, a LiCoO2 cathode, and a Li6PS5Cl electrolyte maintain good capacity retention of 83.65% at 0.3C after 300 cycles. Moreover, in situ L-band electron paramagnetic resonance imaging (EPRI) showed that fewer Li dendrites are formed on a ring-shaped LMA. This work highlights the importance of the design of the shape of the LMA to mitigate the growth of lithium dendrites and shows that L-band EPRI is a useful technique for ASSLMBs.
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