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Electrolyte/Electrode Interfaces in All-Solid-State Lithium Batteries: A Review

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Abstract

All-solid-state lithium batteries are promising next-generation energy storage devices that have gained increasing attention in the past decades due to their huge potential towards higher energy density and safety. As a key component, solid electrolytes have also attracted significant attention and have experienced major breakthroughs, especially in terms of Li-ion conductivity. However, the poor electrode compatibility of solid electrolytes can lead to the degradation of electrolyte/electrode interfaces, which is the major cause for failure in all-solid-state lithium batteries. To address this, this review will summarize the in-depth understanding of physical and chemical interactions between electrolytes and electrodes with a focus on the contact, charge transfer and Li dendrite formation occurring at electrolyte/electrode interfaces. Based on mechanistic analyses, this review will also briefly present corresponding strategies to enhance electrolyte/electrode interfaces through compositional modifications and structural designs. Overall, the comprehensive insights into electrolyte/electrode interfaces provided by this review can guide the future investigation of all-solid-state lithium batteries.

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Fig. 1
Fig. 2

Copyright © 2017, American Chemical Society. b Improved wettability of Ga-doped LLZO to Li through Li-deficient compound protection. Reprinted with permission from Ref. [26]. Copyright © 2019, American Chemical Society. c Pressure-dependent Nyquist plots of Li|LLZO|Li cells. Reprinted with permission from Ref. [28]. Copyright © 2019, American Chemical Society. d Relationship between the logarithm of interfacial resistance and surface adhesion strength of Li|LLZO|Li cells. Reprinted with permission from Ref. [29]. Copyright © 2018, Elsevier

Fig. 3

Copyright © 2006, Elsevier. b 3D reconstructed rendering image of a cathode showing the connectivity of each component. Reprinted with permission from Ref. [18]. Copyright © 2018, American Chemical Society. c Visualizations of models with different active material (grey) and electrolyte (yellow) contents and sizes. The top is a 30 wt% 3 µm electrolyte and a 70 wt% 5 µm active material; the bottom is a 20 wt% 8 µm electrolyte and an 80 wt% 5 µm active material. Reprinted with permission from Ref. [38]. Copyright © 2019, John Wiley & Sons. d Exemplary active material microstructures at a 55 vol% fraction with (5, 10, 15) μm particle diameters and respective electron connected particles (yellow) and electron unconnected particles (red). Reprinted with permission from Ref. [39]. Copyright © 2019, American Chemical Society

Fig. 4

Copyright © 2017, American Chemical Society. b 2D slices of LAGPO pellets after cycling for (1) 0, (2) 24, (3) 32, (4) 44 and (5) 52 h. Dark lines represent cracks (top). Increases in crack volume and amounts of charge transfer are shown by using blue arrows and green arrows, respectively (bottom). Reprinted with permission from Ref. [42]. Copyright © 2019, American Chemical Society. c Li distribution and hydrostatic stress in a cathode at different stages of charge. Cracks, marked by black lines, propagate from corner to corner and cut off Li-ion diffusion pathways. Reprinted with permission from Ref. [46]. Copyright © 2017, Royal Society of Chemistry

Fig. 5

Copyright © 2017, American Chemical Society. b Electrochemical stability windows and potential profiles in ASSLBs. Reprinted with permission from Ref. [53]. Copyright © 2015, American Chemical Society. c Reaction and formation of an electron insulator SEI layer (left); reaction and formation of a degradation layer with high electron conductivity (right); Li potentials between Li metal and electrolytes in different interphase types (bottom). Reprinted with permission from Ref. [21]. Copyright © 2018, American Association for the Advancement of Science

Fig. 6

Copyright © 2010, American Chemical Society. b EELS O K-edge spectra across the LLZO/Li interface showing the formation of an ultra-thin tetragonal LLZO interphase. Reprinted with permission from Ref. [73]. Copyright © 2016, American Chemical Society. c O K-edge X-ray absorption spectroscopy data across the LLZO/LCO interface showing the formation of La2Zr2O7, Li2CO3 and LaCoO3 blocking interphases [79]. d XPS spectra across the LAGPO/Li interface showing the partial reduction of Ti4+ to Ti3+ in LAGPO. Reprinted with permission from Ref. [85]. Copyright © 2013, American Chemical Society

Fig. 7

Copyright © 2014, American Chemical Society. b Space charge layer effects on an LAGPO/Li2V2O5 interface. The space charge layer led to higher barriers for Li-ion diffusion and smaller exchange current density. Reprinted with permission from Ref. [98]. Copyright © 2020, Elsevier. c Li and electron distributions near an LATPO/LCO interface in the charged state (top) and typical distribution of measured potential (bottom). Reprinted with permission from Ref. [99]. Copyright © 2010, John Wiley & Sons

Fig. 8

Copyright © 2018, American Association for the Advancement of Science. b Schematic of an LPSCl/Li interface cycled at an overall current density above critical current density for striping. Reprinted with permission from Ref. [104]. Copyright © 2019, Springer Nature. c X-ray tomographic reconstructions of void phases in the interior of LLZO sintered at 1050, 1100 and 1150 °C. Reprinted with permission from Ref. [106]. Copyright © 2018, American Chemical Society. d SEM micrographs of the web structure in cycled LLZO. Reprinted with permission from Ref. [107]. Copyright © 2017, Elsevier. e Transverse view showing the leaf-like morphology of Li filaments that have penetrated into or completely through single-crystal LLZO. Reprinted with permission from Ref. [112]. Copyright © 2018, The Electrochemical Society

Fig. 9

Copyright © 2017, American Chemical Society. b Time-resolved Li concentration profiles for LCO|LiPON|Cu, Li|LLZO|Cu and Li|LPS|Pt cells. c Correlations between cumulative charge (the orange line) and cumulative neutron depth profiling counts (green dots) in the total region (surface and bulk) of Li|LLZO|Cu and Li|LPS|Pt cells at 100 °C. d Li concentration profiles in LLZO and LPS at different times during Li plating. Reprinted with permission from Ref. [24]. Copyright © 2019, Springer Nature. e Distribution of excess electrons (the yellow region) in LLZO (left) and phase-field simulation results showing isolated dendrite nucleation (right). Reprinted with permission from Ref. [119]. Copyright © 2019, American Chemical Society

Fig. 10

Copyright © 2016, Springer Nature. b Pretreatment processes for the formation of a LiF-rich SEI layer between LPS and Li. Reprinted with permission from Ref. [21]. Copyright © 2018, American Association for the Advancement of Science. c Li deposition behaviors by using LLZO electrolytes and LLZO-2 wt% Li3OCl composite electrolytes, formation of an interlayer between LLZO-2 wt%, Li3OCl and Li through the in situ decomposition of Li3OCl. Reprinted with permission from Ref. [133]. Copyright © 2018, Elsevier. d Li dendrite formation in pristine LiBH4 and Li dendrite suppression in LiF modified LiBH4. Reprinted with permission from Ref. [138]. Copyright © 2019, John Wiley & Sons

Fig. 11

Copyright © 2015, The Electrochemical Society. b Structure and characterization of hierarchical Li3PO4@NCM811 (top); impedance plots of ASSLBs using NCM811 with and without coating after 100 cycles. Reprinted with permission from Ref. [150]. Copyright © 2020, Elsevier. c Specific recommendations of coating materials obtained by high-throughput screening and detailed case studies. Reprinted with permission from Ref. [151]. Copyright © 2019, Elsevier

Fig. 12

Copyright © 2018, Elsevier. b The working principle of an all-in-one solid-state Li||S battery based on the tri-layer garnet electrolyte. Reprinted with permission from Ref. [162]. Copyright © 2018, Elsevier. c Intimate contact between LLZO and Li as enabled by the hyper-elastic substrate PDMS. Reprinted with permission from Ref. [167]. Copyright © 2020, American Chemical Society

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Acknowledgements

The authors gratefully acknowledge the support of the National Natural Science Foundation of China (51671135, 51971146, 51971147), the Major Program for the Scientific Research Innovation Plan of Shanghai Education Commission (2019-01-07-00-07-E00015), the Program of Shanghai Subject Chief Scientist (17XD1403000), the Shanghai Outstanding Academic Leaders Plan, the Shanghai Rising-Star Program (20QA1407100) and the General Program of Natural Science Foundation of Shanghai (20ZR1438400).

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Authors and Affiliations

  1. School of Materials Science and Engineering, University of Shanghai for Science and Technology, Shanghai, 200093, China

    Yuepeng Pang, Jinyu Pan, Junhe Yang & Shiyou Zheng

  2. Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD, 20742, USA

    Chunsheng Wang

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  1. Yuepeng Pang
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  2. Jinyu Pan
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  3. Junhe Yang
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  4. Shiyou Zheng
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Contributions

SZ and CW proposed the idea for this review. YP and JP performed the literature search and data analysis, YP wrote the first draft of this review, and JY, SZ and CW revised this review.

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Correspondence to Shiyou Zheng or Chunsheng Wang.

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Pang, Y., Pan, J., Yang, J. et al. Electrolyte/Electrode Interfaces in All-Solid-State Lithium Batteries: A Review. Electrochem. Energ. Rev. 4, 169–193 (2021). https://doi.org/10.1007/s41918-020-00092-1

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