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Title: Efficient diffusion of superdense lithium via atomic channels for dendrite-free lithium–metal batteries

Journal Article · · Energy & Environmental Science
DOI:https://doi.org/10.1039/d1ee02205a· OSTI ID:1869925
ORCiD logo [1];  [1]; ORCiD logo [2];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [3];  [2]; ORCiD logo [5]; ORCiD logo [1]
  1. Xiamen University (China)
  2. Beijing University of Chemical Technology (China)
  3. Xiamen University (China); Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen (China)
  4. Argonne National Lab. (ANL), Lemont, IL (United States)
  5. Argonne National Lab. (ANL), Lemont, IL (United States); Stanford Univ., CA (United States); Imam AbduIrahman Bin Faisal Univ. (IAU), Dammam (Saudi Arabia)

The non-uniform aggregation of fast-diffused Li on an anode surface would aggravate its tip-effect-induced nucleation/growth, leading to the notorious dendrite growth in Li metal batteries (LMBs). Tuning the Li diffusion on the anode surface has been regarded previously as a mainstream method to induce its uniform deposition, while the diffusion of Li in the anode bulk is usually ignored. In this study, conceptually different from the classic surface modification, we propose a molecular tunnelling strategy to construct atomic channels in graphite bulk, which enables the fast diffusion of superdense Li. Density functional theory calculations and ab initio molecular dynamics simulations prove that the bulk diffusion through atomic channels could become a new and dominating path. Its reversible and efficient diffusion has been further visualized by in situ transmission electron microscopy. As a result, when coupled with high-loading LiFePO4 cathodes (20 mg cm–2), a high areal capacity and 100% capacity retention are achieved over 370 cycles. Through this work a new strategy is developed based on the bulk-diffusion of superdense Li for dendrite-free LMBs, which can be pervasive in other high-performance energy storage systems.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; National Natural Science Foundation of China (NSFC); National Key Research and Development Program of China; US-China Clean Energy Research Centre (CERC-CVC2); USDOE
Grant/Contract Number:
AC02-06CH11357; 91934303; 21673198; 21673194; 21621091; 21620102007; 2016YFB0100202
OSTI ID:
1869925
Alternate ID(s):
OSTI ID: 1832923
Journal Information:
Energy & Environmental Science, Vol. 15, Issue 1; ISSN 1754-5692
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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