High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes

Han, Fudong; Westover, Andrew S.; Yue, Jie; Fan, Xiulin; Wang, Fei; Chi, Miaofang; Leonard, Donovan N.; Dudney, Nancy J.; Wang, Howard; Wang, Chunsheng

doi:10.1038/s41560-018-0312-z

High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes

Journal Article · Sun Jan 13 23:00:00 EST 2019 · Nature Energy

DOI:https://doi.org/10.1038/s41560-018-0312-z· OSTI ID:1557527

Han, Fudong ^[1]; ^[2]; Yue, Jie ^[1]; Fan, Xiulin ^[1]; ^[1]; ^[2]; ^[2]; ^[2]; ^[1]; ^[1]

Univ. of Maryland, College Park, MD (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Solid electrolytes (SEs) are widely considered as an ‘enabler’ of lithium anodes for high-energy batteries. However, recent reports demonstrate that the Li dendrite formation in Li₇La₃Zr₂O₁₂ (LLZO) and Li₂S–P₂S₅ is actually much easier than that in liquid electrolytes of lithium batteries, by mechanisms that remain elusive. Here we illustrate the origin of the dendrite formation by monitoring the dynamic evolution of Li concentration profiles in three popular but representative SEs (LiPON, LLZO and amorphous Li₃PS₄) during lithium plating using time-resolved operando neutron depth profiling. Although no apparent changes in the lithium concentration in LiPON can be observed, we visualize the direct deposition of Li inside the bulk LLZO and Li₃PS₄. Furthermore, our findings suggest the high electronic conductivity of LLZO and Li₃PS₄ is mostly responsible for dendrite formation in these SEs. Lowering the electronic conductivity, rather than further increasing the ionic conductivity of SEs, is therefore critical for the success of all-solid-state Li batteries.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Nanostructures for Electrical Energy Storage (NEES); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Advanced Research Projects Agency - Energy (ARPA-E)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1557527

Journal Information:: Nature Energy, Journal Name: Nature Energy Journal Issue: 3 Vol. 4; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Ultrathin, flexible, solid polymer composite electrolyte enabled with aligned nanoporous host for lithium batteries Wan, Jiayu; Xie, Jin; Kong, Xian Nature Nanotechnology, Vol. 14, Issue 7 https://doi.org/10.1038/s41565-019-0465-3	journal	May 2019
Designing solid-state electrolytes for safe, energy-dense batteries Zhao, Qing; Stalin, Sanjuna; Zhao, Chen-Zi Nature Reviews Materials, Vol. 5, Issue 3 https://doi.org/10.1038/s41578-019-0165-5	journal	February 2020
Dendrite nucleation in lithium-conductive ceramics Li, Guanchen; Monroe, Charles W. Physical Chemistry Chemical Physics, Vol. 21, Issue 36 https://doi.org/10.1039/c9cp03884a	journal	January 2019
Experimental and numerical analysis to identify the performance limiting mechanisms in solid-state lithium cells under pulse operating conditions Pang, Mei-Chin; Hao, Yucang; Marinescu, Monica Physical Chemistry Chemical Physics, Vol. 21, Issue 41 https://doi.org/10.1039/c9cp03886h	journal	January 2019
Recent advances in the interface engineering of solid-state Li-ion batteries with artificial buffer layers: challenges, materials, construction, and characterization Du, Mingjie; Liao, Kaiming; Lu, Qian Energy & Environmental Science, Vol. 12, Issue 6 https://doi.org/10.1039/c9ee00515c	journal	January 2019
A bird's-eye view of Li-stuffed garnet-type Li ₇ La ₃ Zr ₂ O ₁₂ ceramic electrolytes for advanced all-solid-state Li batteries Samson, Alfred Junio; Hofstetter, Kyle; Bag, Sourav Energy & Environmental Science, Vol. 12, Issue 10 https://doi.org/10.1039/c9ee01548e	journal	January 2019
Design of a mixed conductive garnet/Li interface for dendrite-free solid lithium metal batteries Huo, Hanyu; Chen, Yue; Li, Ruying Energy & Environmental Science, Vol. 13, Issue 1 https://doi.org/10.1039/c9ee01903k	journal	January 2020
A more stable lithium anode by mechanical constriction for solid state batteries Su, Yibo; Ye, Luhan; Fitzhugh, William Energy & Environmental Science, Vol. 13, Issue 3 https://doi.org/10.1039/c9ee04007b	journal	January 2020
Solid-state electrolyte considerations for electric vehicle batteries Shen, Hao; Yi, Eongyu; Cheng, Lei Sustainable Energy & Fuels, Vol. 3, Issue 7 https://doi.org/10.1039/c9se00119k	journal	January 2019
The effects of mechanical constriction on the operation of sulfide based solid-state batteries Fitzhugh, William; Ye, Luhan; Li, Xin Journal of Materials Chemistry A, Vol. 7, Issue 41 https://doi.org/10.1039/c9ta05248h	journal	January 2019
A high performance all solid state lithium sulfur battery with lithium thiophosphate solid electrolyte Bonnick, Patrick; Niitani, Keita; Nose, Masafumi Journal of Materials Chemistry A, Vol. 7, Issue 42 https://doi.org/10.1039/c9ta06971b	journal	January 2019
Theoretical formulation of Na ₃ AO ₄ X (A = S/Se, X = F/Cl) as high-performance solid electrolytes for all-solid-state sodium batteries Yu, Yuran; Wang, Zhuo; Shao, Guosheng Journal of Materials Chemistry A, Vol. 7, Issue 38 https://doi.org/10.1039/c9ta08584j	journal	January 2019
Sulfuryl chloride as a functional additive towards dendrite-free and long-life Li metal anodes Fu, Xiangxiang; Wang, Gang; Dang, Dai Journal of Materials Chemistry A, Vol. 7, Issue 43 https://doi.org/10.1039/c9ta09068a	journal	January 2019
Probing into the origin of an electronic conductivity surge in a garnet solid-state electrolyte Song, Yongli; Yang, Luyi; Tao, Lei Journal of Materials Chemistry A, Vol. 7, Issue 40 https://doi.org/10.1039/c9ta10269h	journal	January 2019
How Metallic Protection Layers Extend the Lifetime of NASICON-Based Solid-State Lithium Batteries Cortes, Francisco Javier Quintero; Lewis, John A.; Tippens, Jared Journal of The Electrochemical Society, Vol. 167, Issue 5 https://doi.org/10.1149/2.0032005jes	journal	October 2019
Hot Formation for Improved Low Temperature Cycling of Anode-Free Lithium Metal Batteries Genovese, Matthew; Louli, A. J.; Weber, Rochelle Journal of The Electrochemical Society, Vol. 166, Issue 14 https://doi.org/10.1149/2.0661914jes	journal	January 2019
Dense, Melt Cast Sulfide Glass Electrolyte Separators for Li Metal Batteries Yersak, Thomas A.; Salvador, James R.; Pieczonka, Nicholas P. W. Journal of The Electrochemical Society, Vol. 166, Issue 8 https://doi.org/10.1149/2.0841908jes	journal	January 2019

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