Manipulating charge-transfer kinetics and a flow-domain LiF-rich interphase to enable high-performance microsized silicon-silver-carbon composite anodes for solid-state batteries

Han, Xiang1; Gu, Lanhui1; Sun, Zhefei2; Chen, Minfeng1; Zhang, Yinggan2; Luo, Linshan3; Xu, Min1; Chen, Songyan3; Liu, Haodong6; Wan, Jiayu7; He, Yan-Bing4,5; Chen, Jizhang1; Zhang, Qiaobao2,8

2023-09-01

10.1039/d3ee01696

ENERGY & ENVIRONMENTAL SCIENCE   Impact Factor & Quartile

1754-5692

1754-5706

["A silicon (Si) anode with a high theoretical specific capacity (3579 mA h g-1) offers great promise for realizing high-energy solid-state batteries (SSBs). However, given Si's huge volume variations during cycling, sluggish kinetics and unfavorable interface stability with a solid-state electrolyte (SSE), its practical potential in SSBs has not been fully exploited. Herein, we propose a design of highly dense Ag nanoparticles decorated with porous microsized Si, which is coated by thin-layer carbon (PS-Ag-C) working as a high-performance anode for boosting SSB performance. Specifically, the mechanical stress at the interface, originating from a large volume change of Si, can be alleviated by the highly porous architecture. Meanwhile, continuous charge transfer within Si can be achieved by the introduction of Ag nanoparticles, a thin carbon layer and the as-formed Ag-Li alloys, which contribute to high-rate capability and stable cycling performance. Furthermore, coupled with a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/Li1.3Al0.3Ti1.7(PO4)3 (LATP) SSE with low mobility, a flow-domain LiF-rich solid-electrolyte-interphase (SEI) is formed, ensuring desirable interfacial and mechanical stability. Accordingly, the as-fabricated PS-Ag-C anode achieves high reversible capacities of 3030.3 mA h g-1 at 0.2 A g-1 with an initial Coulombic efficiency of 90% and 1600 mA h g-1 over 500 cycles at 1 A g-1, respectively. In particular, we observed that the highest areal capacity reaches 4.0 mA h cm-2 over 100 cycles at 0.5 A g-1 in Si-based SSBs with organic-inorganic composite SSEs. Moreover, a solid-state full cell assembled with the as-obtained PS-Ag-C anode and LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode demonstrates high capacity and desirable cycling stability. This work provides new insights into developing a high-capacity and durable Si anode for high-performance SSBs.","A high-capacity and durable PS-Ag-C composite anode in combination with a PVDF-HEP/LATP solid-state electrolyte has been successfully designed and fabricated, demonstrating boosted electrochemical performance for solid-state batteries."]

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This research was financially supported by the National Natural Science Foundation of China (22209075, 52072323, 51902165, and 52122211), the Natural Science Foundation of Jiangsu Province (BK20200800), the Frontier Exploration Projects of Longmen Laborato["22209075","52072323","51902165","52122211"] ; National Natural Science Foundation of China["BK20200800","LMQYTSKT008"] ; Natural Science Foundation of Jiangsu Province[JCYJ20220818101003008]

Chemistry ; Energy & Fuels ; Engineering ; Environmental Sciences & Ecology

Chemistry, Multidisciplinary ; Energy & Fuels ; Engineering, Chemical ; Environmental Sciences

WOS:001083059100001

ROYAL SOC CHEMISTRY

Web of Science

1.Nanjing Forestry Univ, Coll Mat Sci & Engn, Coinnovat Ctr Efficient Proc & Utilizat Forest Res, Nanjing 210037, Jiangsu, Peoples R China
2.Xiamen Univ, Coll Mat, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
3.Xiamen Univ, Dept Phys, Xiamen 361005, Fujian, Peoples R China
4.Tsinghua Univ, Inst Mat Res IMR, Shenzhen All Solid State Lithium Battery Electroly, Tsinghua Shenzhen Int Grad Sch, Shenzhen, Peoples R China
5.Tsinghua Univ, Inst Mat Res IMR, Shenzhen Geim Graphene Ctr, Tsinghua Shenzhen Int Grad Sch, Shenzhen, Peoples R China
6.Univ Calif San Diego, Chem Engn, La Jolla, CA 92093 USA
7.Southern Univ Sci & Technol, Dept Mech & Energy Engn, Shenzhen, Peoples R China
8.Xiamen Univ, Shenzhen Res Inst, Shenzhen 518000, Peoples R China

Han, Xiang,Gu, Lanhui,Sun, Zhefei,et al. Manipulating charge-transfer kinetics and a flow-domain LiF-rich interphase to enable high-performance microsized silicon-silver-carbon composite anodes for solid-state batteries[J]. ENERGY & ENVIRONMENTAL SCIENCE,2023.

Han, Xiang.,Gu, Lanhui.,Sun, Zhefei.,Chen, Minfeng.,Zhang, Yinggan.,...&Zhang, Qiaobao.(2023).Manipulating charge-transfer kinetics and a flow-domain LiF-rich interphase to enable high-performance microsized silicon-silver-carbon composite anodes for solid-state batteries.ENERGY & ENVIRONMENTAL SCIENCE.

Han, Xiang,et al."Manipulating charge-transfer kinetics and a flow-domain LiF-rich interphase to enable high-performance microsized silicon-silver-carbon composite anodes for solid-state batteries".ENERGY & ENVIRONMENTAL SCIENCE (2023).