Highly elastic polyrotaxane binders for mechanically stable lithium hosts in lithium‐metal batteries

  

 Figure S1. Cycling performance of LiCu asymmetric cells with Li metal anodes containing

CNT network with a mass loading of 0.33 gcnt cm௅2 _{and 0.99 gcnt cm}௅2 _{when tested with 1} mAh cm௅2 _{at 3 mA cm}௅2_{. These comparative data show the importance of CNT content in} sustaining its network during repeated Li uptakerelease cycles. 

 



Figure S2. FTIR spectra of hydroxylpropylated polyrotaxane (HPR), PAA and PRPAA. The

peak of PRPAA at 1730 cm௅1 _{indicates ester linkage between PAA and HPR.} 

 



Figure S3. Synthetic scheme of PRPAA.

 

 



Figure S5. (a) Topview SEM image of fCNT network and (b) its magnified view. (c) XPS

spectrum of the fCNT network in O 1s branch. (d) Peeling test result of the fCNT network without any binder.



 

Figure S6. Photographs of fCNTbinder network (a) before and (b) after peeling test.



 

Figure S7. (a) SEM image of Li plated bare CNT network at 1 mA cm௅2 _{(plating capacity = 1} mAh cm௅2_{) and (b) its magnified view. }

 

 Figure S8. Crosssectional SEM images of (a) fCNTPVA network and (b) fCNTPRPAA

network after Li stripping. Current density = 1 mA cm௅2_{. Areal capacity = 1 mAh cm}௅2_.

 

 Figure S9. Topview SEM images: (a) Li plated and (b) stripped fCNTPVA network; (c) Li

plated and (d) stripped fCNTPRPAA network.

 

 Figure S10. Strain recovery of PVA and PRPAA films over repeated stretchrecovery cycles.

The recovery was estimated based on the formula: ሺሺࡸ െ ࡸ૙ሻȀࡸ૙ሻ ൈ ૚૙૙ (L: Length of film after cycling, L0: Length of pristine film). 

 



Figure S11. Top view SEM images of (a) fCNTPVA and (b) fCNTPRPAA networks when

the CNT composite films were stretched until crack was generated.

 

 Figure S12. Coulombic efficiencies of LiCu asymmetric cells with Li metal anodes

containing bare CNT, fCNTPVA, and fCNTPRPAA networks when tested at 6 mA cm௅2 _with 1 mAh cm௅2_{. }

 

 

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 Figure S15. (a) Capacity retentions of bare CNT, fCNTPVA, and fCNTPRPAA networks

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