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1 tom-thik Interlyer Mde of VD-Grown Grphene Film on Seprtor for dvned thium-sulfur tteries Zhenzhen Du 1, hengkun Guo 2, njun Wng 3, jun Hu 1, Song Jin 1, Timing Zhng 1, Honghng Jin 1, Zhiki Qi 1, Sen Xin 2, Xinghu Kong 2 *, Yu-Guo Guo 4, Hengxing Ji 1 *, nd -Jun Wn 1,4 * 1 Deprtment of Mterils Siene nd Engineering, S Key Lortory of Mterils for Energy onversion, ihem (ollortive Innovtion enter of hemistry for Energy Mterils), University of Siene nd Tehnology of hin, Hefei 2326, hin; 2 Deprtment of hemistry nd hemil Engineering, Hefei University of Tehnology, Hefei 239, hin; 3 Hefei Ntionl Lortory for Physil Sienes t the Mirosle nd enter for Miro- nd Nnosle Reserh nd Frition, University of Siene nd Tehnology of hin, Hefei 2326, hin; 4 Key Lortory of Moleulr Nnostruture nd Nnotehnology, Institute of hemistry, hinese demy of Sienes nd eijing Ntionl Lortory for Moleulr Sienes, eijing 119, hin. *orresponding uthor: kongxh@hfut.edu.n, jihengx@ust.edu.n, wnlijun@is..n. S-1

2 Figure S1. Photogrphs of VD grphene film overed on () opper foil nd () trnsferred on polyethylene terephthlte (PET) sustrte. () Optil trnspreny of 1-lyer nd 2-lyer grphene film on PET. The trnspreny vlues mrked y the rrows re otined t 55 nm. 1s spetr of grphene (d) grown on u foil nd (e) trnsferred onto SiO 2 /Si sustrte y TRT. The XPS of 1s spetr of grphene on oth u nd SiO 2 /Si hve intensive pek entered t ev tht n e ssigned to - onds. 1 The full width t hlf mximum (FWHM) of this pek, whih stnds for the rtio etween sp 3 -hyridized ron nd sp 2 -hyridized ron, re.9 nd 1.1 ev, respetively, inditing similr sp 3 -/sp 2 - rtio for the grphene efore nd fter trnsfer. Moreover, the stellite peks t inding energies of > ev n e ssigned to -O funtionl groups. These funtionl groups showing in the XPS of grphene on u my ome from dsorents t the grphene surfe when exposure to ir or euse of prtil oxidtion of grphene on u. However, the reltive intensity of these stellite peks re lmost identil for the grphene on u nd SiO 2 /Si. Therefore, the residue indued y TRT n e ignored. S-2

3 Figure S2. () Shemti of stking single lyers of VD-grphene to otin grphene film with different numer of lyers nd trnsferring the film to PP seprtor. Photogrphs of () re-pp, (), (d), nd (e). SEM imges of (f), (g) nd (h). Tle S1. Sheet resistnes of VD-grphene overed PP seprtors with different numer of stked lyers. Type of the seprtor Sheet resistne (Ω/ ) rek-iruit S-3

4 4 3 Roughness (Rq): 12.5 nm 2 Y (nm) µm -3 d Y (nm) X (µm) 3 Roughness (Rq): 9.6 nm µm X (µm) Figure S3. FM imges nd the mesured surfe roughness for (,) re-pp nd (,d). S-4

5 Tle S2. Eletrohemil performne of the -S tteries ssemled with different seprtors. oting lyer Grphene oxide Mss loding (mg m -2 ) Intil speifi pity (m h g -1 ) yle numers (n) pity dey rte (per yle) urrent density %.1 17 Ref. ) Grphene %.89 2 MWNT % 1 21 MNT@PEG %.5 22 MOF/GO %.5 23 oo ron fier % 1 24 Super P %.1 25 Super P %.5 26 Mesporous ron Miroporous ron nnofier Mesporous ron % % %.5 29 TiO 2 /grphene %.5 3 Super P %.5 31 Miroporous ron/peg Polymer oted ron nnotue MWNT-PNI /TiO 2 /PNI MWNT/SiO 2 /MWNT seprtor ) These referenes re listed in the min text % % % % %.5 This work S-5

6 15 Speifi pity (m h g -1 ) Speifi pity (m h g -1 ) 1 group 1:pure S 1mg m -2 2 wt.% NO yle numer (n).1 group 4: S/RGO 1mg m -2 without NO yle numer (n) oulomi effiieny (%) oulomi effiieny (%) 15 Speifi pity (m h g -1 ) 1 group 2: S/MEGO 1mg m -2 2 wt.% NO d 16 Speifi pity (m h g -1 ) 12 8 yle numer (n) group 5: S/rGO 3.2mg m -2 2 wt.% NO yle numer (n) oulomi effiieny (%) oulomi effiieny (%) e 16 1 Speifi pity (m h g -1 ) 12 8 group 6: S/rGO 3.2mg m -2 without NO yle numer (n) oulomi effiieny (%) Figure S4. yling performne of -S ells ssemled with () pure S, () S/MEGO nd () S/rGO thode with S mss loding of 1 mg m -2, nd (d,e) S/rGO thode with S mss loding of 3.2 mg m -2. The ells in (), () nd (d) were ssemled with eletrolyte onting 2 wt.% NO 3, while the ells in () nd (e) were ssemle without NO 3 dditive. The speifi pities inrese nd the pity dey rtes derese when the -S ells were ssemled with ompring to those with re-pp. S-6

7 urrent () urrent ( ) e urrent ( ) g urrent () mv s -1.1 mv s -1.2 mv s -1.3 mv s Potentil (V vs. + /).5 mv s -1.1 mv s -1.2 mv s -1.3 mv s Potentil (V vs. + /).5 mv s -1.1 mv s -1.2 mv s -1.3 mv s Potentil (V vs. + /) mv s -1.1 mv s -1.2 mv s -1.3 mv s Potentil (V vs. + /) Ip () d f Ip () Ip () h Ip ().4.2. D + ()=4.37 x1-8 m 2 S -1 D + ()=.55 x1-8 m 2 S -1 D + ()=.44 x1-8 m 2 S v.5 (V.5 s -.5 ) D + ()=4.11 x1-8 m 2 S -1 D + ()=.66 x1-8 m 2 S -1 D + ()=.9 x1-8 m 2 S v.5 (V.5 s -.5 ) D + ()=6.65 x1-8 m 2 S -1 D + ()=.73 x1-8 m 2 S -1 D + ()=1.1 x1-8 m 2 S v.5 (V.5 s -.5 ) D + ()=4.51 x1-8 m 2 S -1 D + ()=.71 x1-8 m 2 S -1 D + ()=.62 x1-8 m 2 S v.5 (V.5 s -.5 ) Figure S5. yli voltmmogrms t different voltge sn rtes nd the liner fits of the pek urrents of -S tteries with (,) re-pp, (,d), (e,f), nd (g,h). S-7

8 2G-PET fresh yled Figure S6. Resistnes of () 2-lyer VD-grphene film on PET sustrte nd () efore nd () fter yling. The tiny resistne hnge onfirms good mehnil strength nd exellent dhesion of VD-grphene lyers on PP seprtor. S-8

9 urrent density (m mg -1 ) urrent density (m mg -1 ) e urrent density (m mg -1 ) rd Potentil (V vs. + /) Potentil (V vs. + /) rd 3th Potentil (V vs. + /) urrent density (m mg -1 ) d urrent density (m mg -1 ) f urrent density (m mg -1 ) rd rd Potentil (V vs. + /) Potentil (V vs. + /) rd Potentil (V vs. + /) Figure S7. V profiles of the -S ells ssemled with () re-pp, (), (), nd (d) in potentil window of V vs. + /. V profiles of the -S ells ssemled with in potentil window of (e) V nd (f) V vs. + /. S-9

10 -Zim (ohms) Fresh tteries -Zim (ohms) fter 5 hrge/dishrge yles Zre (ohms) Zre (ohms) Figure S8. Nyquist plots of -S ells () efore yling nd () fter 5 hrge/dishrge yles. Speifi pity (m h g -1 ) yle numer (n) oulomi effiieny (%) Figure S9. yle performne of the -S ells ssemled with re-pp,,, nd. Potentil (V vs. + /) Speifi pity (m h g -1 ) Figure S1. Glvnostti hrge/dishrge profiles of the -S ells mesured t.1. S-1

11 4 S S Intensity (.u.) 3 S -1 T Intensity (.u.) 4 3 S -1 T inding energy (ev) inding energy (ev) S d 4 S S -1 Intensity (.u.) 4 3 S -1 T Intensity (.u.) 3 T inding energy (ev) inding energy (ev) Figure S11. XPS showing the S 2p signls quired t the surfe () re-pp, (), (), nd (d) whih were fed to the thode side fter 5 hrge/dishrge yles. Referenes 1. Henriette, E.-S. XPS Photoemission in roneous Mterils: Defet Pek eside the Grphiti symmetri Pek. ron, 24, 42, S-11