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Title Page 2

Abstract 5

Contents 7

Ⅰ. Introduction 11

Ⅱ. Experimental 15

2.1. Materials 15

2.2. Fabrication of all-solid-state batteries 15

2.3. Electrochemical characterization 16

Ⅲ. Results and Discussion 17

3.1. Characteristics 17

3.2. Interfacial Diffusion 23

3.3. Minimize the side reaction 26

3.4. Host to reserve lithium metal 28

3.5. Electrochemical performance 33

Ⅳ. Conclusion 40

Ⅴ. Reference 41

List of Figures 8

Figure 1. The characteristic of a porous graphitic carbon framework 14

Figure 2. The configuration of all-solid-state batteries 14

Figure 3. The morphologies of OMGC 17

Figure 4. Mesoporous characteristics of OMGC 18

Figure 5. Full capacity of lithium metal plating in OMGC framework 19

Figure 6. Comparison of electrochemical property of OMGC with other carbons 19

Figure 7. The scheme of lithium storage process along the PGCF 20

Figure 8. The simulation 21

Figure 9. The schematic of lithium deposition process 21

Figure 10. The voltage profile of PGCF half-cell 22

Figure 11. In-situ TEM image 23

Figure 12. The capture image 23

Figure 13. The SEM image of PGCF electrode 24

Figure 14. The optical images 24

Figure 15. The voltage profiles 25

Figure 16. The schematic of PGCF with SE electrode and PGCF without SE electrode 27

Figure 17. The XPS spectrum 27

Figure 18. The initial cycle performance 27

Figure 19. The cross-sectional SEM image 28

Figure 20. The ToF-SIMS data 29

Figure 21. The scheme of half-cell 30

Figure 22. The cross-sectional SEM image 30

Figure 23. The cross-sectional image of Cu half-cell 31

Figure 24. ToF-SIMS data 31

Figure 25. a) Operando differential electrochemical pressiometry after plating along the cycles of PGCF... 32

Figure 26. The impedance plot 33

Figure 27. The in-situ GEIS Nyquist plot 34

Figure 28. The voltage profile of in-situ GEIS of stripping step 34

Figure 29. The long-term cycle performance 35

Figure 30. The voltage profile 36

Figure 31. The schematic explaining the irreversible capacity along the cycles 37

Figure 32. The chronoamperometry (CA) analysis 37

Figure 33. The galvanostatic intermittent titration technique (GITT) analysis 38

Figure 34. The cycle performance of PGCF 38

Figure 35. The cycle performance 39

초록보기

 All-solid-state batteries (ASSBs), equipped with highly ion-conductive sulfide solid electrolyte and utilizing lithium metal plating/stripping as anode electrochemistry, suffers from (1) chemical vulnerability of the solid electrolyte with lithium metal and (2) physical growth of lithium metal to penetrate the electrolyte. Porous electron-conductive structures having lithium metal reservoir is expected to solve the concerns only if lithium is able to move to cover the whole structure without the help of solid electrolyte. By employing a porous graphitic carbon framework (PGCF) between a sulfide solid electrolyte layer and a copper current collector in ASSB, we successfully demonstrated that lithium metal was reversibly plated and stripped during battery operation. The void volume of the framework was fully filled with lithium metal, despite ionic pathways were not provided separately even without additional lithiophiles when an enough amount of lithium metal was allowed to be plated. The successful ASSB operation and the electrolyte-absent PGCF utilization for plating were read by a consecutive mechanism of (1) graphitic skeleton lithiation followed by(2) lithium metal plating on the lithiated carbon surface, and subsequently metal growth via Coble creep of lithium along the lithium-carbon interface toward current collector. The void volume of the framework and the interfacial diffusion are believed to suppress dendritic growth of lithium metal and minimize the electrolyte-metal contact by relieving the stress developed by electrochemically generated lithium metal mass.

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